Co-reporter:Qianqian Liu, Lu Zhang, Yuanyuan Chai, and Wei-Lin Dai
The Journal of Physical Chemistry C November 22, 2017 Volume 121(Issue 46) pp:25898-25898
Publication Date(Web):October 31, 2017
DOI:10.1021/acs.jpcc.7b08819
Single-crystal sodium niobate with wire- and cube-like structures has been created by a facile and eco-friendly route including a hydrothermal as well as in-site self-assembled process via optimizing thermal treatment temperature. Comparative studies were carried out to evaluate the structure and phase transformation during the fabrication course. A possible growth mechanism of NaNbO3 with controllable morphologies was elucidated based on the time- and temperature-dependent evolution experiments. In addition, special attention was paid to figure out the mutual relationship between the unique structure features and photocatalytic performance toward photocatalytic H2 evolution. The results illustrated that the NaNbO3 nanowires formed at 500 °C calcinations exhibited the highest photocatalytic activity compared with other materials and presented super stability as well. The superior photocatalytic performance could be interpreted in terms of the better crystalline, fewer defects, and perfect 1D nanowire morphology as demonstrated by TEM and SEM images, FT-IR, and Raman spectroscopy analysis. Additionally, a deep insight into the underlying of the photocatalytic reaction mechanism was proposed. These findings shed light on an efficient and facile pathway for the creation and formation mechanisms of photocatalytic materials, which provided new opportunities for solar-energy conversion.
Co-reporter:Xiuying Guo;Anyuan Yin;Kangnian Fan
The Journal of Physical Chemistry C June 25, 2009 Volume 113(Issue 25) pp:11003-11013
Publication Date(Web):2017-2-22
DOI:10.1021/jp902688b
Copper-containing mesoporous HMS catalysts prepared via a one-pot synthesis method based on sol−gel chemistry have been systematically characterized focusing on the effect of copper loading. Structural characterization of a series of different copper loading samples was performed by means of N2 adsorption, X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, temperature programmed reduction, N2O titration, and X-ray photoelectron spectroscopy. It is concluded that the copper loading has a great influence on the pore structure of the catalyst. On the basis of the characterizations, the copper species on calcined CuO/HMS samples and reduced Cu/HMS samples were assigned. The synergetic effect between the Cu0 and Cu+ is considered to be responsible for the enhanced catalytic performance in the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG). The maximum ratio of Cu0/Cu+ obtained via tuning the copper loading can result in the highest DMO hydrogenation activity and EG selectivity.
Co-reporter:Qianqian Liu, Yuanyuan Chai, Lu Zhang, Jia Ren, Wei-Lin Dai
Applied Catalysis B: Environmental 2017 Volume 205(Volume 205) pp:
Publication Date(Web):15 May 2017
DOI:10.1016/j.apcatb.2016.12.065
•Pt nanoparticles (NPs) supported on wire- and cube- like NaNbO3.•A facile hydrothermal route combined with in situ photodeposition method.•Nanowire exhibited 25 times higher H2 production than nanocube.•Super stability up to 15 h in the process of photocatalytic H2 production.•Better distribution of Pt NPs and much stronger interaction of Pt and NaNbO3 nanowire.Pt nanoparticles (NPs) supported on wire- and cube- like NaNbO3 were successfully synthesized by a facile hydrothermal route combined with in situ photodeposition method. Photocatalytic performances towards photocatalytic H2 production and organic-pollutant degradation of NaNbO3 with morphology of nanowire and nanocube, with or without support of Pt NPs were comparatively investigated. In addition, special attention was paid to investigate the influence of the morphologies on the photocatalytic performance of Pt/NaNbO3 systems. It was found that, by incorporation of Pt NPs, Pt/NaNbO3 systems show much higher activity than their counterparts. Moreover, by contrast with Pt/NaNbO3 nanocube, the Pt NPs tend to be better uniformly dispersed on NaNbO3 nanowire while prefer to agglomerate on NaNbO3 nanocube, resulting in more direct contact between Pt NPs and NaNbO3 nanowire. Meanwhile, it was found that the stronger interaction of Pt NPs and NaNbO3 nanowire, confirmed by XRD, Raman spectroscopy and XPS, significantly enhanced the electron transfer between NaNbO3 nanowire and Pt NPs, and hence further increased the separation efficiency of electron-hole pairs. Thus, a remarkably more enhanced photocatalytic activity of Pt/NaNbO3 nanowire than other materials has been realized, and this catalyst presented super stability as well. A deep insight into the underlying of the photocatalytic reaction mechanism was also proposed.Download high-res image (141KB)Download full-size image
Co-reporter:Jia Ren, Xin Liu, Ruihua Gao, Wei-Lin Dai
Journal of Energy Chemistry 2017 Volume 26, Issue 4(Volume 26, Issue 4) pp:
Publication Date(Web):1 July 2017
DOI:10.1016/j.jechem.2017.01.007
The morphology effect of Zr-doped CeO2 was studied in terms of their activities in the selective oxidation of styrene to styrene oxide using tert-butyl hydroperoxide as the oxidant. In the present work, Zr-doped CeO2 nanorods exhibited the highest catalytic performance (yield of styrene oxide and TOF value) followed by nanoparticles and nanocubes. For the Zr-doped CeO2 nanorods, the apparent activation energy is 56.3 kJ/mol, which is much lower than the values of catalysts supported on nanoparticles and nanocubes (73.3 and 93.4 kJ/mol). The high resolution transmission electron microscopy results indicated that (1 0 0) and (1 1 0) crystal planes are predominantly exposed for Zr-doped CeO2 nanorods while (1 0 0) and (1 1 1) for nanocubes, (1 1 1) for nanoparticles. The remarkably increased catalytic activity of the Zr-doped CeO2 nanorods is mainly attributed to the higher percentage of Ce3+ species and more oxygen vacancies, which are associated with their exposed (1 0 0) and (1 1 0) crystal planes. Furthermore, recycling studies proved that the heterogeneous Zr-doped CeO2 nanorods did not lose its initial high catalytic activity after five successive recycles.Download high-res image (120KB)Download full-size imageZr-doped CeO2 catalysts with different morphologies catalyzing styrene oxidation were investigated and Zr-doped CeO2 nanorods exhibited the highest catalytic performance according to the highest Ce3+ content and oxygen vacancies.
Co-reporter:
Chinese Journal of Chemistry 2017 Volume 35(Issue 2) pp:125-125
Publication Date(Web):2017/02/01
DOI:10.1002/cjoc.201770021
The cover picture shows a new one step approach to synthesize g-C3N4 nano-sheets by direct thermal pyrolysis process of urea in NH3 atmosphere. For the first time, the influence of the preparation gas atmosphere on the composition, crystalline and polymerization degree, and the photocatalytic activity of the g-C3N4 synthesized from thermal condensation of urea was investigated. Furthermore, we studied in depth the structure-performance relationship in the system, and it was found that the synergistic effect of the larger surface area, the adjusted band energy structure and the well crystallization may be conductive to the higher separation of the electron- hole pair, thus leading to the wonderful performance for the g-C3N4-NH3. Notably, the method has the merits of low cost, scalable production and environmental friendliness. More details are discussed in the article by Dai et al. on page 173–182.
Co-reporter:
Chinese Journal of Chemistry 2017 Volume 35(Issue 2) pp:173-182
Publication Date(Web):2017/02/01
DOI:10.1002/cjoc.201600608
AbstractWe developed a new one step approach to synthesize g-C3N4 nano-sheets by direct thermal pyrolysis process of urea in NH3 atmosphere. For the first time, the influence of the preparation gas atmosphere on the composition, crystalline and polymerization degree, and the activity of the g-C3N4 synthesized from thermal condensation of urea was investigated. Impressively, the g-C3N4 nano-sheets obtained under NH3 gas atmosphere exhibited much superior photo-catalytic activities to the prepared g-C3N4 in air or N2, and the rate of the g-C3N4-NH3 was about 5 times higher than that on g-C3N4-N2 sample. The detailed characterization analysis revealed that NH3 thermal pyrolysis atmosphere contributed to the polymerization degree and the formation of the layer with a more regular structure due to the efficiently extending of the conjugated π-conjugative system, which was favorable to the transfer of the photo-induced charge carriers. Furthermore, we studied in depth the structure-performance relationship in the system, and it was found that the synergistic effect of the larger surface area, the adjusted band energy structure and the well crystallization may be conductive to the higher separation of the electron–hole pair, thus leading to the wonderful performance for the g-C3N4-NH3. Notably, the method has the merits of low cost, scalable production and environmental friendliness.
Co-reporter:Jing Ding, Lu Zhang, Qianqian Liu, Wei-Lin Dai, Guofeng Guan
Applied Catalysis B: Environmental 2017 Volume 203(Volume 203) pp:
Publication Date(Web):1 April 2017
DOI:10.1016/j.apcatb.2016.10.028
•Close contact and strong interaction between Ag NPs and WO3-110 nanorods.•Efficient charge separation of {001} facets of nanorods and SPR effect of Ag NPs.•Size-dependent effect in the photocatalytic activity of the nanocatalyst.•Greatly enhanced photocatalytic activity than pure WO3-110 nanorod.Novel visible-light-driven plasmonic photocatalyst Ag/WO3-110 nanorods with the dominant {001} exposed facets were prepared via a two-step hydrothermal treatment and in-situ photoreduction reaction. The as-prepared samples were characterized by various analytical techniques, such as X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, UV–vis diffuse reflectance spectroscopy, photoluminescence spectra and electrochemical impedance spectroscopy. The results illustrated that the intrinsic nature of charge separation on the {001} facets of WO3-110 nanorods as well as the surface plasmon resonance (SPR) effect of Ag nanoparticles (Ag NPs) can facilitate the charge transfer between Ag NPs and the {001} facets of WO3-110 nanorods. Moreover, the size of Ag NPs also plays an important role in the SPR effect and the photogenerated carrier separation. Those Ag NPs loaded on {001} facets of WO3 nanorods exhibit size-dependent photocatalytic activity for the MO and RhB degradation. Additionally, the underlying photocatalytic reaction mechanism was further investigated by the photoelectrochemical experiment and the controlled experiments using radical scavengers.Download high-res image (139KB)Download full-size image
Co-reporter:Jia Ren;Xin Liu;Lu Zhang;Qianqian Liu;Ruihua Gao
RSC Advances (2011-Present) 2017 vol. 7(Issue 9) pp:5340-5348
Publication Date(Web):2017/01/17
DOI:10.1039/C6RA26137J
A series of g-C3N4 nanosheets were synthesized by thermal oxidation with long time heating and etching. With an increase in heating time from 1.0 to 3.0 h, the g-C3N4 nanosheet was obtained with a thinner layer thickness, larger BET surface area and higher graphic nitrogen ratio. As a metal-free heterogeneous catalyst, the g-C3N4 NS-3 h nanosheets show a superior catalytic performance for the epoxidation of styrene to styrene oxide than that of the bulk g-C3N4 and other recently reported metal-free materials. The higher activity of the g-C3N4 NS-3 h synthesized by long time thermal oxidative etching might be ascribed to the enlarged specific surface, pore volume and higher graphic nitrogen ratio with the loose and soft laminar morphology. The graphitic nitrogen species play a key role in the catalytic reaction based on a good linear correlation between the content of these species and the activity results. The g-C3N4 nanosheets are very stable and can be reused 5 times without obvious loss of catalytic activity.
Co-reporter:Yuanyuan Cui;Bin Wang;Chao Wen;Xi Chen ;Dr. Wei-Lin Dai
ChemCatChem 2016 Volume 8( Issue 3) pp:527-531
Publication Date(Web):
DOI:10.1002/cctc.201501055
Abstract
Copper-based activated-carbon (AC)-supported catalysts were synthesized by a facile ammonia evaporation–impregnation method. Unlike the conventional Cu/SiO2 catalyst, which showed highly catalytic selectivity towards ethylene glycol (EG) or EtOH, Cu/AC catalysts display unique selectivity to methyl glycolate (MG). The catalytic performance relies on the high content of surface Cu+ species and the relatively large copper particles with moderate hydrogenation activity.
Co-reporter:Jing Ding
The Journal of Physical Chemistry C 2016 Volume 120(Issue 8) pp:4345-4353
Publication Date(Web):February 3, 2016
DOI:10.1021/acs.jpcc.5b10580
WO3 nanorods with a regular hexagonal morphology and different exposed facets were fabricated by hydrothermal treatment, and then Ag nanoparticles (Ag NPs) selectively deposited onto hexagonal WO3 nanorods with different facets were also successfully synthesized through an in situ photoreduction method. The prepared samples were characterized by various analytical techniques, such as X-ray diffraction, X-ray photoelectron spectroscopy, UV–vis diffuse reflectance spectroscopy, photoluminescence spectra, and so on. The results illustrated that the intrinsic nature of charge separation on the {001} facets of WO3-110 nanorods and the surface plasmon resonance (SPR) effect both contribute to the enhancement of visible-light absorption and the decrease of the recombination of the photogenerated electron–hole pairs. For comparison, Ag/WO3-110 catalysts with dominant exposed {001} facets exhibited much better photocatalytic activity than that of Ag/WO3-001 with a high percentage of exposed {100} and {010} facets for the degradation of organic pollutants (including rhodamine B, methyl orange, and so on) under the visible-light irradiation. In addition, the underlying photocatalytic reaction mechanism was further investigated by the controlled experiments using radical scavengers.
Co-reporter:Xi Chen, Yuanyuan Cui, Chao Wen, Bin Wang and Wei-Lin Dai
Chemical Communications 2015 vol. 51(Issue 72) pp:13776-13778
Publication Date(Web):22 Jul 2015
DOI:10.1039/C5CC05030H
Continuous fixed-bed catalytic hydrogenation of ethylene carbonate (EC) to methanol and ethylene glycol (EG), an emerging synthetic process of methanol via indirect conversion of CO2, was successfully performed over Cu/HMS catalysts prepared by the ammonia evaporation (AE) method. The catalysts possessed superb performance with a conversion of 100% and a selectivity to methanol of 74%.
Co-reporter:Li Wang, Yuanyuan Chai, Jia Ren, Jing Ding, Qianqian Liu and Wei-Lin Dai
Dalton Transactions 2015 vol. 44(Issue 33) pp:14625-14634
Publication Date(Web):13 Jul 2015
DOI:10.1039/C5DT01961C
Novel 3D hierarchical Ag3PO4/MoS2 composites were successfully prepared through a facile and reproducible hydrothermal-in situ precipitation method. The 3D flower-like spherical MoS2 nanoarchitectures acted as an excellent supporting matrix for the in situ growth of Ag3PO4 nanoparticles. The photocatalytic performance of the composites and the effect of the amount of MoS2 were investigated. The obtained hierarchical Ag3PO4/MoS2 composites exhibited significantly enhanced performance for photocatalytic oxidation of Rhodamine B (RhB) compared with pure Ag3PO4 under visible light irradiation. Ag3PO4/MoS2 composites with 15 wt% of MoS2 showed the optimal photoactivity for the degradation of RhB, which was approximately 4.8 times as high as that of pure Ag3PO4. What's more, the optimal Ag3PO4/MoS2 composite also showed better photodegradation efficiency for methyl orange (MO) and p-chlorophenol (4-CP) than pure Ag3PO4. More attractively, the stability of Ag3PO4 was improved after the in situ deposition of Ag3PO4 particles on the surface of MoS2 nanoflakes due to the conductivity of MoS2 itself as electron acceptors. The enhanced performance of the hierarchical Ag3PO4/MoS2 composites under visible light was caused by a synergistic effect including the improved separation of photogenerated charge carriers, boosted light harvesting, a relatively high surface area and matching energy band structures between the two components. Interestingly, the heterostructured Ag3PO4/MoS2 composite reduced the use of the noble metal silver, thereby effectively reducing the cost of the Ag3PO4 based photocatalyst. Ultimately, a MoS2 involved photocatalytic mechanism for the hierarchical Ag3PO4/MoS2 composites was also proposed.
Co-reporter:Li Wang, Jing Ding, Yuanyuan Chai, Qianqian Liu, Jia Ren, Xin Liu and Wei-Lin Dai
Dalton Transactions 2015 vol. 44(Issue 24) pp:11223-11234
Publication Date(Web):11 May 2015
DOI:10.1039/C5DT01479D
A novel CeO2 nanorod/g-C3N4/N-rGO ternary composite was synthesized using a simple ultrasonic-heat treatment method for application in the photocatalytic degradation of organic pollutants under the irradiation of visible light. This material shows superior photocatalytic activity compared with pure g-C3N4 and CeO2 nanorods, and the photodegradation rate of RhB is up to 2.1-fold higher than that of the g-C3N4/N-rGO (at the optimum content of 0.25 wt% N-rGO) catalyst when the content of CeO2 nanorods was 2 wt%. The enhancement of photocatalytic activity could be attributed to the synergistic effect among CeO2, g-C3N4 and N-rGO (serves as a conductive network), which was found to lead to more efficient separation of photogenerated electron–hole pairs, resulting in the effective photodegradation of organic pollutants. In addition, superoxide radical anions (˙O2−) and holes (h+) were considered as the main reactive species during the photodegradation process, and the ternary composite also exhibited preferable stability for the decomposition of RhB. This work provides an in-depth perspective for understanding the N-doped graphene-involved photocatalytic mechanism.
Co-reporter:Bin Wang, Chao Wen, Yuanyuan Cui, Xi Chen, Yu Dong and Wei-Lin Dai
RSC Advances 2015 vol. 5(Issue 37) pp:29040-29047
Publication Date(Web):10 Mar 2015
DOI:10.1039/C5RA00053J
A series of Cu-based TiO2-supported catalysts were synthesized via facile ammonia evaporation for the selective hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG). A 100% conversion of DMO, 99% selectivity for EG, and super stability were achieved over the 20% Cu/P25 TiO2 catalyst. The effect of the crystal phase of the titania support and the interaction between Cu and P25 were investigated. The active copper species located at the interface between the anatase and rutile phases play important roles in the selective hydrogenation. The excellent catalytic performance was mainly attributed to better copper dispersion and an appropriate ratio of Cu0/Cu+, which stems from the intimate interaction between Cu and the P25 support.
Co-reporter:Xin-Li Yang, Li-Ming Qiao, Wei-Lin Dai
Microporous and Mesoporous Materials 2015 Volume 211() pp:73-81
Publication Date(Web):15 July 2015
DOI:10.1016/j.micromeso.2015.02.035
•Phosphotungstic acids encapsulated in UiO-66 by the direct synthesis method.•Highly dispersed HPWs into the microporous cages of UiO-66.•Crystal structure and morphology of UiO-66 were well preserved.•Excellent catalytic activity and reusability in the oxidation of CPE to GA.•94.8% CPE conversion and 78.3% GA yield were obtained.A heterogenous Zr-based metal organic framework (UiO-66) encapsulating phosphotungstic acid (HPWs) catalyst (HPWs@UiO-66), was prepared by a simple direct hydrothermal reaction of ZrCl4, terephthalic acid, and HPWs in DMF. The as-prepared novel material was very active as the catalyst for the selective oxidation of cyclopentene (CPE) to glutaraldehyde (GA) with environmentally benign hydrogen peroxide as the oxidant. The crystal structure and morphology of UiO-66 were well preserved after the incorporation of HPWs, as confirmed by X-ray diffraction (XRD), SEM, and TEM. Moreover, the XRD, N2 adsorption, and FT-IR analyses reveal that HPW components could stably exist in the nanocages of UiO-66. FT-IR-CO adsorption experiments indicated that additional Lewis acid sites were present in the HPWs@UiO-66 sample, which were essential to catalyze the selective oxidation of CPE to GA. A proper amount of HPWs and their high dispersion accounted for high catalytic activity. Almost complete conversion of CPE (∼94.8%) and high yield of GA (∼78.3%) were obtained using the 35 wt% HPWs@UiO-66 catalyst. Furthermore, HPW components hardly leached in the reaction solution, enabling the catalyst to be used for three reaction cycles without obvious deactivation.
Co-reporter:Yuanyuan Chai, Li Wang, Jia Ren, Wei-Lin Dai
Applied Surface Science 2015 Volume 324() pp:212-220
Publication Date(Web):1 January 2015
DOI:10.1016/j.apsusc.2014.09.207
Highlights
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Highly efficient visible-light-driven Ag3PO4/SBA-15 nanocomposite.
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Application in the photo-degradation of RhB.
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Synthesis from a facile and simple colloidal method.
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20%-Ag3PO4/SBA-15 shows 8 times faster degradation rate than Ag3PO4.
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Super stability and recycling ability.
Co-reporter:Yuanyuan Cui, Chao Wen, Xi Chen and Wei-Lin Dai
RSC Advances 2014 vol. 4(Issue 59) pp:31162-31165
Publication Date(Web):11 Jul 2014
DOI:10.1039/C4RA05014B
The distribution of 2-methoxyethanol and ethylene glycol can be controlled by regulating the surface acidity of copper based zirconia catalysts for hydrogenation of dimethyl oxalate. The yield of 2-methoxyethanol can reach 68% due to the synergistic effect of the surface acid site and active copper site.
Co-reporter:Luyao Zou;Yuanyuan Cui ;Weilin Dai
Chinese Journal of Chemistry 2014 Volume 32( Issue 3) pp:257-262
Publication Date(Web):
DOI:10.1002/cjoc.201300875
Abstract
Au/TiO2 catalyst is firstly reported to be efficient in the hydrogenation of nitrobenzene to produce p-aminophenol with a high PAP selectivity of 81% and overall yield more than 63%. The catalyst is also quite stable and can be reused for at least 4 times with only slight decrease in activity.
Co-reporter:Chao Wen, Yuanyuan Cui, Wei-Lin Dai, Songhai Xie and Kangnian Fan
Chemical Communications 2013 vol. 49(Issue 45) pp:5195-5197
Publication Date(Web):17 Apr 2013
DOI:10.1039/C3CC40570B
The variation of the supports on the Cu/SiO2 catalyst plays an important role in the catalytic performance for hydrogenation of dimethyl oxalate. The loss of silica in the form of tetramethoxysilane from the support under the reaction conditions is responsible for the deactivation of the Cu/SiO2 catalyst.
Co-reporter:Yuanyuan Cui, Ying Wang, Kangnian Fan, Wei-Lin Dai
Applied Surface Science 2013 Volume 279() pp:391-399
Publication Date(Web):15 August 2013
DOI:10.1016/j.apsusc.2013.04.125
Highlights
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Highly active AuAg/TiO2 bimetallic catalysts were prepared.
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The reaction was carried out under solvent-free conditions.
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Different calcinations temperature leads to different activities.
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The best yield of benzyl alcohol to sodium benzoate reached 85%.
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The catalyst can be reused for 6 times without obvious deactivation.
Co-reporter:Quanjing Zhu, Xiaofeng Chu, Zhaoyan Zhang, Wei-Lin Dai and Kangnian Fan
RSC Advances 2013 vol. 3(Issue 6) pp:1744-1747
Publication Date(Web):04 Dec 2012
DOI:10.1039/C2RA22194B
A novel and green route is reported for the selective oxidation of cyclopentene oxide to glutaraldehyde by using aqueous H2O2 as the oxidant and WS2@hexagonal mesoporous silica (WS2@HMS) material as the catalyst, which shows a very large surface area, high efficiency, excellent selectivity and outstanding reusability.
Co-reporter:Chao Wen;Yuanyuan Cui;Dr. Anyuan Yin; Kangnian Fan ;Dr. Wei-Lin Dai
ChemCatChem 2013 Volume 5( Issue 1) pp:
Publication Date(Web):
DOI:10.1002/cctc.201290050
Co-reporter:Chao Wen;Yuanyuan Cui;Dr. Anyuan Yin; Kangnian Fan ;Dr. Wei-Lin Dai
ChemCatChem 2013 Volume 5( Issue 1) pp:138-141
Publication Date(Web):
DOI:10.1002/cctc.201200444
Co-reporter:Xiaofeng Chu, Quanjing Zhu, Wei-Lin Dai and Kangnian Fan
RSC Advances 2012 vol. 2(Issue 18) pp:7135-7139
Publication Date(Web):13 Jun 2012
DOI:10.1039/C2RA21068A
Graphite oxide (GO) was synthesized from natural graphite powder using Hummers' method. A large number of oxygen-containing functional groups (C–O and CO) on the surface of graphite oxide were obtained, as identified by Fourier-transform infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS). The GO material shows outstanding catalytic performance and stability in the selective oxidation of glutaraldehyde to glutaric acid with aqueous H2O2. The catalytic activity has a slight increase when the GO is treated with 50% aqueous H2O2 solution and decreases evidently when the GO is treated with KBH4, which could be attributed to the increase in the amount of C–O and CO moieties after oxidation treatment or the decrease in the amount after reduction treatment. The oxygen-containing functional groups on the graphite oxide surface may play an important role in the catalytic process.
Co-reporter:Ruihua Gao, Quanjing Zhu, Wei-Lin Dai and Kangnian Fan
RSC Advances 2012 vol. 2(Issue 14) pp:6087-6093
Publication Date(Web):06 Jun 2012
DOI:10.1039/C2RA20779F
Dicyclopentadiene dioxide (2) was synthesized using an economic and green reaction by the direct oxidation of dicyclopentadiene (DCPD) with aqueous H2O2 over tungstic acid and aminopropyl-immobilized phosphotungstic acid on SBA-15, which was successfully obtained by the immobilization of the supported heteropolyacid (HPW) on the surface of the ordered mesoporous silica, SBA-15, by means of chemical bonding to aminosilane groups. The as-obtained materials were characterized by N2 sorption, transmission electron microscopy (TEM), X-ray diffraction (XRD), 31P-magic angle spinning (MAS) NMR and Raman spectroscopy. The 16% HPW-NH2-SBA-15 is highly efficient in the reaction with a DCPD conversion of 100% and (2) selectivity up to 97%. It is interesting that this material could be reused six times without any significant loss of activity and selectivity. The good stability can be attributed to the strong interaction between the amino groups on the surface of SBA-15 and HPW anions.
Co-reporter:Jiamin Zheng, Jie Huang, Xian Li, Wei-Lin Dai and Kangnian Fan
RSC Advances 2012 vol. 2(Issue 9) pp:3801-3809
Publication Date(Web):06 Feb 2012
DOI:10.1039/C2RA20196H
Nano-sized gold catalysts have attracted much interest during recent years. Here, we report a new material to improve the catalytic activity and recyclability of gold catalysts. Multi-component Fe–Al–O oxides prepared by impregnation (γ-Fe2O3/γ-Al2O3 and Al2O3/α-Fe2O3) and encapsulation (Fe2O3@Al2O3) methods were employed as carriers for gold catalysts. The Au/Fe–Al–O composites exhibited efficient catalytic activity and selectivity for the lactonization of 1,4-butanediol to γ-butyrolactone. They could also be easily recovered due to their super-paramagnetic property. XRD, TEM, XPS and H2-TPR were used to characterize the composites. The influence of surface Fe/Al ratio on Au/(Fe2O3@Al2O3) composites was also studied by adjusting the Fe/Al molar ratio for comparison and the optimal Fe/Al ratio was found to be 1:4. The results confirmed that higher conversion and selectivity were obtained due to the bifunctional effect of Fe2O3 and Al2O3.
Co-reporter:Ying Wang, Jia-Min Zheng, Kangnian Fan and Wei-Lin Dai
Green Chemistry 2011 vol. 13(Issue 7) pp:1644-1647
Publication Date(Web):18 May 2011
DOI:10.1039/C1GC15311K
A novel green route to synthesize sodium benzoate from the one-pot oxidation of benzyl alcohol using air as the oxidant and AuAg/TiO2 as the catalyst under solvent-free conditions is presented. This process proceeds with advantages from the viewpoint of green chemistry due to non-toxic reagents, no waste emission and high recyclability of catalysts, which can retain high catalytic activity (yield > 75%) even after 6 runs.
Co-reporter:Ruihua Gao, Quanjing Zhu, Wei-Lin Dai and Kangnian Fan
Green Chemistry 2011 vol. 13(Issue 3) pp:702-708
Publication Date(Web):03 Feb 2011
DOI:10.1039/C0GC00691B
The heteropoly phosphotungstic acid, H3PW12O40 (HPW), was successfully immobilized on the surface of MCF, SBA-15 and MCM-41 by means of chemical bonding to aminosilane groups. The as-obtained materials were characterized by N2 sorption, TEM, XRD, FT-IR, 13C-, 29Si-, 31P-MAS NMR and XPS. Characterization results suggest that the surface area decreased after grafting amino groups to silica. The as-prepared HPW-NH2-MCF is highly efficient in the O-heterocyclization of cycloocta-1,5-diene (COD) to 2,6-dihydroxy-9-oxabicyclo[3.3.1] nonane (1) and 2-hydroxy-9-oxabicyclo [3.3.1] nonane-6-one (2) with a COD conversion of 100% and (1 + 2) selectivity up to 98%. It is worth mentioning that this material could be reused six times without any significant loss of activity and selectivity. The good stability can be attributed to the strong interaction between the amino groups on the surface of MCF and HPW anions.
Co-reporter:Anyuan Yin, Chao Wen, Wei-Lin Dai and Kangnian Fan
Journal of Materials Chemistry A 2011 vol. 21(Issue 25) pp:8997-8999
Publication Date(Web):31 May 2011
DOI:10.1039/C1JM10646E
CuAu/HMS alloy nanoparticles constructed viaammonia-evaporation–deposition–precipitation were prepared and exhibited excellent performance in methyl glycolate synthesis.
Co-reporter:Xiaofeng Chu, Ying-Yi Le, Quanjing Zhu, Kangnian Fan, Wei-Lin Dai
Applied Surface Science 2011 Volume 257(Issue 20) pp:8605-8609
Publication Date(Web):1 August 2011
DOI:10.1016/j.apsusc.2011.05.030
Abstract
The organoamino-functionalized mesoporous silicas with different distribution patterns—site-isolation or site-aggregation are prepared using post-grafting method. We have investigated the effects of the solvents and the catalytic reactivity of these catalysts. It is found that, using the polar ethanol as solvent, the catalytic center is site-isolated. Contrarily, the catalytic center is site-aggregated with the non-polar toluene. Characterization techniques, including transmission electron microscopy, nitrogen sorption experiments, thermogravimetric analysis, and ultraviolet–visible absorbance spectroscopy, demonstrate the most important dependencies of the distribution pattern on the polarity of solvent.
Co-reporter:Anyuan Yin, Chao Wen, Wei-Lin Dai, Kangnian Fan
Applied Surface Science 2011 Volume 257(Issue 13) pp:5844-5849
Publication Date(Web):15 April 2011
DOI:10.1016/j.apsusc.2011.01.117
Abstract
Cu/SiO2 catalysts with different bimodal pore structures adjusted by the ratio of HMS and silica sol were prepared via modified impregnation method. Structure evolutions of the catalyst were systematically characterized by N2-physisorption, X-ray diffraction, H2 temperature-programmed reduction, N2O titration and X-ray photoelectron spectroscopy. The results show that the composite silica supported copper catalysts showed remarkably enhanced catalytic performance in the selective hydrogenation of dimethyl oxalate to ethylene glycol compared to the individual silica supported ones obtained by the same method. The dimethyl oxalate conversion and the ethylene glycol selectivity can reach 100% and 98% at 473 K with 2.5 MPa H2 pressure and 1.5 h−1 liquid hour space velocity of dimethyl oxalate over the optimized Cu/SiO2 catalyst. The remarkably enhanced catalytic performance of Cu/SiO2 catalysts might be attributed to the homogeneous dispersion and uniformity of the active copper species and to the larger copper surface areas attained on the HMS supports with large pore diameters and surface areas.
Co-reporter:Bowen Ma;Jianfeng Guo;Luyao Zou;Weilin Dai;Kangnian Fan
Chinese Journal of Chemistry 2011 Volume 29( Issue 4) pp:857-859
Publication Date(Web):
DOI:10.1002/cjoc.201190170
Abstract
Ag/AgCl@cotton-fabric plasmonic photocatalyst has been synthesized by a facile method, which exhibits excellent stability for the decomposition of RhB and conveniency in the separation and recovery of the catalyst from the solution.
Co-reporter:Xiaoyang Guo;Anyuan Yin;Xiaodong Guo;Xiuying Guo;Weilin Dai;Kangnian Fan
Chinese Journal of Chemistry 2011 Volume 29( Issue 8) pp:1563-15662
Publication Date(Web):
DOI:10.1002/cjoc.201180281
Abstract
CoAl alloy catalyst is found, for the first time, to be highly active, selective and reusable for the synthesis of diols via the hydrogenolysis of glycerol under mild conditions. The products and the catalyst could be self-separated from the reaction system through a simple reactor.
Co-reporter:Quan-Jing Zhu, Wei-Lin Dai and Kang-Nian Fan
Green Chemistry 2010 vol. 12(Issue 2) pp:205-208
Publication Date(Web):07 Dec 2009
DOI:10.1039/B921334A
A new economic and green route to synthesize phthalide from 1,2-benzenedimethanol using aqueous hydrogen peroxide as the oxidant and tungstic acid as the catalyst under organic solvent-free conditions is presented. This process proceeds with advantages from the viewpoint of green chemistry, in which the only by-product of H2O2 is water and the catalyst can also be easily recovered. The desired product with high purity and good yield can be conveniently obtained when cooled after reaction.
Co-reporter:Anyuan Yin, Xiaoyang Guo, Weilin Dai and Kangnian Fan
Chemical Communications 2010 vol. 46(Issue 24) pp:4348-4350
Publication Date(Web):12 May 2010
DOI:10.1039/C0CC00581A
Ag/SiO2 prepared by a sol–gel process is highly effective for selective gas-phase hydrogenation of dimethyl oxalate to corresponding alcohols. The catalysts are of great potential as industrially viable and novel catalysts for the production of methyl glycolate and ethylene glycol.
Co-reporter:Jianfeng Guo;Jingxia Li;Anyuan Yin;Kangnian Fan ; Dr. Weilin Dai
Chinese Journal of Chemistry 2010 Volume 28( Issue 11) pp:2144-2150
Publication Date(Web):
DOI:10.1002/cjoc.201090355
Abstract
Sulfur doped ZnO/TiO2 nanocomposite photocatalysts were synthesized by a facile sol-gel method. The structure and properties of catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), UV-vis diffusive reflectance spectroscopy (DRS) and N2 desorption-adsorption isotherm. The XRD study showed that TiO2 was anatase phase and there was no obvious difference in crystal composition of various S-ZnO/TiO2. The XPS study showed that the Zn element exists as ZnO and S atoms form SO2−4. The prepared samples had mesoporosity revealed by N2 desorption-adsorption isotherm result. The degradation of Rhodamine B dye under visible light irradiation was chosen as probe reaction to evaluate the photocatalytic activity of the ZnO/TiO2 nanocomposite. The commercial TiO2 photocatalyst (Degussa P25) was taken as standard photocatalyst to contrast the prepared different photocatalyst in current work. The improvement of the photocatalytic activity of S-ZnO/TiO2 composite photocatalyst can be attributed to the suitable energetic positions between ZnO and TiO2, the acidity site caused by sulfur doping and the enlargement of the specific area. S-3.0ZnO/TiO2 exhibited the highest photocatalytic activity under visible light irradiation after Zn amount was optimized, which was 2.6 times higher than P25.
Co-reporter:Anyuan Yin, Xiaoyang Guo, Wei-Lin Dai and Kangnian Fan
The Journal of Physical Chemistry C 2010 Volume 114(Issue 18) pp:8523-8532
Publication Date(Web):April 20, 2010
DOI:10.1021/jp101636e
Copper-containing mesoporous Al-HMS catalysts prepared via the deposition−precipitation method have been found to be highly efficient in the catalytic hydrogenation of dimethyl oxalate (DMO) to ethylene glycohol (EG). Besides the Al chemical environment, the Si/Al ratios of the mesoporous support show remarkable effect on the catalytic performance. The DMO hydrogenation activity increased with the increasing of Al content in the support, and the highest catalytic activity was obtained when the Si/Al ratio of the support reached 25. A series of catalysts with different Si/Al ratios were characterized by N2 adsorption−desorption, X-ray diffraction, temperature-programmed reduction, N2O titration, NMR, and X-ray photoelectron spectroscopy. 27Al NMR shows that the tetrahedral coordination Al species that exists in the framework of the support could enhance the catalytic performance while the extraframework Al species would decrease the catalytic properties. The structural defects produced in the Al-containing mesoporous support play an important role in improving the dispersion of active copper species and enhancing the interaction between the copper species and support. On the basis of the characterizations, the copper species on calcined CuO/Al-HMS samples and reduced Cu/Al-HMS samples were assigned. The improvement of the catalytic performance with proper Si/Al ratio may be ascribed to the increasing defect sites associated with Al cations and the electronic promotion.
Co-reporter:Anyuan Yin;Xiuying Guo;Kangnian Fan
ChemCatChem 2010 Volume 2( Issue 2) pp:206-213
Publication Date(Web):
DOI:10.1002/cctc.200900244
Abstract
A series of Cu/HMS (HMS=hexagonal mesoporous silica) catalysts, synthesized by ion exchange at temperatures from 303 to 363 K, are extensively investigated as catalysts for the hydrogenation of dimethyl oxalate to ethylene glycol. The physicochemical properties and catalytic activity are compared with those of a catalyst prepared by the conventional impregnation method. Characterization of the Cu/HMS catalysts shows that the surface and textural structure of the HMS support as well as the dispersion and nature of copper species depend strongly on the ion-exchange temperature. Temperature-programmed reduction patterns reveal the presence of three types of copper species. N2O titration experiments show that the catalyst prepared by ion-exchange treatment at 333 K has the highest metallic copper surface area. A 98 % ethylene glycol yield is attained over the catalyst ion-exchanged at 333 K, illustrating that an optimum ion-exchange temperature is beneficial for the generation of copper catalysts with enhanced activity.
Co-reporter:An-Yuan Yin, Xiu-Ying Guo, Wei-Lin Dai and Kang-Nian Fan
Green Chemistry 2009 vol. 11(Issue 10) pp:1514-1516
Publication Date(Web):14 Aug 2009
DOI:10.1039/B913395J
A new energy-efficient and atom-economical catalytic route for the direct catalytic synthesis of propylene glycol and ethylene glycol from glycerol under milder reaction conditions is presented. The one-pot aqueous-phase process is based on Raney Ni as a versatile catalyst.
Co-reporter:Xiuying Guo;Anyuan Yin;Kangnian Fan
Catalysis Letters 2009 Volume 132( Issue 1-2) pp:22-27
Publication Date(Web):2009 September
DOI:10.1007/s10562-009-0043-7
High copper contented mesoporous Cu/SBA-15 catalysts with high copper dispersion were successfully synthesized via the simple ammonia-driving deposition-precipitation method. The physicochemical properties of these Cu/SBA-15 catalysts have been studied through various characterization methods such as BET, XRD, SEM, TEM and TPR. The catalytic activities of these catalysts were determined on the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG) under gas-phase fixed-bed conditions at high space-time yield. The results revealed that the high copper contented Cu/SBA-15 catalyst still has high specific area, proper pore volume and mesoporous structure, and the catalysts showed much high activities compared to the one prepared by impregnation method. This finding opens a new avenue for the selection of better catalyst for the hydrogenation of DMO to EG.
Co-reporter:Jingxia Li, Jianhua Xu, Wei-Lin Dai and Kangnian Fan
The Journal of Physical Chemistry C 2009 Volume 113(Issue 19) pp:8343-8349
Publication Date(Web):2017-2-22
DOI:10.1021/jp8114012
The 1% silver clusters containing twistlike helix titania nanoparticles have been synthesized and tested in photocatalytic applications. The special twistlike helix structures were obtained by controlling the hydrolysis of titanium tetrachloride, while variety of routes were investigated to deposit the silver nanoparticles, where impregnation, chemical deposition, and photodeposition methods are adopted to fabricate the Ag/TiO2 samples. The influence of the photocatalytic activity of the mesoporous helix materials and the preparation methods on the final structure of the samples was investigated, including the surface area, pore size, silver crystallite size, silver distribution, and silver surface content. The dispersion and particle size of Ag clusters or nanoparticles on Ag/TiO2 nanocatalysts were investigated by TEM analysis. The surface Ag nanoparticles contents were determined by XPS results. Diffuse reflectance and photoluminescence analysis were used to investigate the visible light adsorption ability and the active sites amount including photoinduced electrons and holes. The experimental results show that the chemical deposition method is an efficient method to synthesize Ag/TiO2 catalysts with highly dispersed nanoparticles of metallic Ag. The Ag/TiO2 sample prepared through the chemical deposition method shows the best photocatalytic activity, and its photocatalytic activity is superior to that of P25 and pure TiO2 sample. The superior activity of Ag/TiO2 photocatalysts can be rationalized in terms of well dispersion and suitable surface content of Ag nanoparticles that will effectively decrease the recombination rate of photoinduced electrons and holes and then increase the photooxidation efficiency of the catalysts.
Co-reporter:Jing-Xia LI;Li-Ping REN;Yong CAO ;Kang-Nian FAN
Chinese Journal of Chemistry 2008 Volume 26( Issue 6) pp:1045-1051
Publication Date(Web):
DOI:10.1002/cjoc.200890186
Abstract
Catalytic direct dehydrogenation of methanol to formaldehyde was carried out over Ag-SiO2-MgO-Al2O3 catalysts prepared by sol-gel method. The optimal preparation mass fractions were determined as 8.3% MgO, 16.5% Al2O3 and 20% silver loading. Using this optimum catalyst, excellent activity and selectivity were obtained. The conversion of methanol and the selectivity to formaldehyde both reached 100%, which were much higher than other previously reported silver supported catalysts. Based on combined characterizations, such as X-ray diffraction (XRD), scanning electronic microscopy (SEM), diffuse reflectance ultraviolet-visible spectroscopy (UV-Vis, DRS), nitrogen adsorption at low temperature, temperature programmed desorption of ammonia (NH3-TPD), desorption of CO2 (CO2-TPD), etc., the correlation of the catalytic performance to the structural properties of the Ag-SiO2- MgO-Al2O3 catalyst was discussed in detail. This perfect catalytic performance in the direct dehydrogenation of methanol to formaldehyde without any side-products is attributed to its unique flower-like structure with a surface area less than 1 m2/g, and the strong interactions between neutralized support and the nano-sized Ag particles as active centers.
Co-reporter:Jie Huang, Wei-Lin Dai and Kangnian Fan
The Journal of Physical Chemistry C 2008 Volume 112(Issue 41) pp:16110-16117
Publication Date(Web):2017-2-22
DOI:10.1021/jp8043913
FeOx of different crystal phases were synthesized by altering the calcination temperature of the precursors obtained by a hydrothermal method. Crystal transformation from maghemite to hematite begins at calcination temperature of 573 K. Gold was deposited on the support uniformly with average size of approximately 5 nm. It is found that the as-prepared catalysts show superior activity and selectivity to the commercial Fe2O3 supported gold catalysts in the oxidation of 1,4-butanediol and 1,5-pentanediol to the corresponding lactones. Support shows dramatic influence on the intrinsic properties of gold particles including particle size and electronic nature. Strong interaction between gold and the nanosized ferric oxide support was studied by XPS and TEM.
Co-reporter:Jingxia Li, Wei-Lin Dai and Kangnian Fan
The Journal of Physical Chemistry C 2008 Volume 112(Issue 45) pp:17657-17663
Publication Date(Web):2017-2-22
DOI:10.1021/jp806703n
Highly ordered mesoporous MgO catalysts with tunable pore size distribution and fairly good alkaline property were successfully obtained by a double replication procedure. Small-angle XRD, TEM, and nitrogen adsorption and desorption results show that these mesoporous MgO materials possess a highly ordered 2D hexagonal mesostructure with tunable pore diameter that is obtained using different hydrothermal temperature derived SBA-15 and CNK-3 carbon as templates. The alkaline density was determined for all samples from the technique of temperature-programmed desorption of CO2 and FT-IR, and the mesoporous MgO with large pore diameter shows more basic sites than the reference bulk one. Such mesoporous MgO materials have been successfully used as base catalysts in the Baeyer−Villiger oxidation of cyclic ketones to the corresponding lactones. 100% adamantanone conversion and >99% lactone selectivity were obtained over mesoporous MgO-373. The pore diameter has slight influence on the conversion of ketones, since the average pore diameters of mesoporous MgO are large enough to allow the reactants free access to the active sites. In terms of the proposed mechanism, the enhanced medium alkaline properties will be more favorable for the attack by hydrogen peroxide to form a hydroperoxide and percarbonic oxide, and in turn enhancing the catalytic activity. In addition, the higher surface area and large pore volume are attributed to the higher activity of mesoporous MgO-373 than the others, signifying the promising potential applications of these mesoporous MgO materials in alkaline catalysis.
Co-reporter:Ruihua Gao, Wei-Lin Dai, Yingyi Le, Xinli Yang, Yong Cao, Hexing Li and Kangnian Fan
Green Chemistry 2007 vol. 9(Issue 8) pp:878-881
Publication Date(Web):23 Mar 2007
DOI:10.1039/B618297F
The hydroxy- and carbonyl-derivatives of 9-oxabicyclo[3.3.1]nonane have been synthesized through an economic and green catalytic reaction between cycloocta-1,5-diene (COD) and aqueous H2O2 with tungstic acid as the catalyst. This process has advantages from the viewpoint of green chemistry, in that the aqueous H2O2 is used as the green oxygen donor, the only by-product of H2O2 is water and the tungstic acid catalyst can also be easily recovered. The excellent yields of the object products (1 and 2) (see Scheme 1) are reached easily under mild reaction conditions.
Co-reporter:Li-Ping Ren, Wei-Lin Dai, Yong Cao, Hexing Li and Kangnian Fan
Chemical Communications 2003 (Issue 24) pp:3030-3031
Publication Date(Web):11 Nov 2003
DOI:10.1039/B310316A
Novel Ag–SiO2–MgO–Al2O3 catalyst prepared by sol–gel method showed extremely high activity and selectivity (both equal to 100%) in the direct dehydrogenation of methanol to anhydrous formaldehyde.
Co-reporter:Wei-Lin Dai, Hao Chen, Yong Cao, Hexing Li, Songhai Xie and Kangnian Fan
Chemical Communications 2003 (Issue 7) pp:892-893
Publication Date(Web):05 Mar 2003
DOI:10.1039/B211666A
A highly active and perfectly structured W-MCM41 catalyst for the oxidative cleavage of cyclopentene to glutaraldehyde was synthesized through a novel economic and green synthetic method by using Na2SiO3 as the Si source and CH3COOC2H5 as the hydrolyzer.
Co-reporter:Qianqian Liu, Jing Ding, Yuanyuan Chai, Junqi Zhao, Shibiao Cheng, Baoning Zong, Wei-Lin Dai
Journal of Environmental Chemical Engineering (June 2015) Volume 3(Issue 2) pp:1072-1080
Publication Date(Web):1 June 2015
DOI:10.1016/j.jece.2015.02.016
•H2WO4 coupling g-C3N4 are successfully prepared for the first time.•Simple synthesis method was adopted.•10% H2WO4/g-C3N4 catalyst shows 50 times higher activity than the pure one.•Superior stability even after nine successive runs.•Synergistic interaction plays very important role in the degradation of RhB.The modified graphitic carbon nitride (g-C3N4) nanosheets by coupling with H2WO4 are fabricated via an easy, mild and environmental-friendly impregnation method for the first time. Compared with bare g-C3N4 and H2WO4, the H2WO4/g-C3N4 composite shows significant enhancement in the visible-light-driven photoactivity toward the degradation of Rhodamine B (RhB). It is found that 10 wt.% H2WO4/g-C3N4 exhibits the best photocatalytic performance, with around 20 times higher activity than that of pure g-C3N4 nanosheets. The remarkably increased performance is mainly attributed to the existing synergistic interaction between H2WO4 and g-C3N4. The strong interaction could reduce the photoinduced electron–hole recombination and further improve the photocatalytic activity. Additionally, O2− is the dominating reactive species for the degradation of RhB, which has been confirmed by the radical scavengers tests. The synthesized photocatalysts present super stability even after nine successive runs. Considering the low-cost, easy preparation process and ultra-high activity, the H2WO4/g-C3N4 photocatalyst can be served as a promising candidate for environment cleaning and waste water treatment.Download high-res image (334KB)Download full-size image
Co-reporter:Anyuan Yin, Xiuying Guo, Wei-Lin Dai, Hexing Li, Kangnian Fan
Applied Catalysis A: General (31 October 2008) Volume 349(Issues 1–2) pp:91-99
Publication Date(Web):31 October 2008
DOI:10.1016/j.apcata.2008.07.020
Co-reporter:Xin-Li Yang, Wei-Lin Dai, Ruihua Gao, Kangnian Fan
Journal of Catalysis (25 July 2007) Volume 249(Issue 2) pp:278-288
Publication Date(Web):25 July 2007
DOI:10.1016/j.jcat.2007.05.002
Tungsten-doped ordered SBA-15 prepared by the in situ synthesis method was systematically characterized by UV-Raman, UV–vis DRS, FT-IR, XPS, and H2-TPR. It was found that the dispersion and nature of the tungsten species depend strongly on the tungsten oxide content. The tungsten species are located mainly in isolated tetrahedral or low-condensed oligomeric environments, and there are strong interaction between tungsten species and the silica-based matrix at tungsten oxide content <20 wt%. Higher tungsten oxide content leads to the formation of bulk tungsten species. It was also found that the ordered hexagonal mesoporous structure of SBA-15 is retained, and strong Brønsted and Lewis acid sites are formed on tungsten incorporation. The superior catalytic performance in the selective oxidation of cyclopentene has been attributed to its proper content of tungsten species, high dispersion, and strong surface acidity.
Co-reporter:Zhaoyan Zhang, Quanjing Zhu, Jing Ding, Xin Liu, Wei-Lin Dai
Applied Catalysis A: General (22 July 2014) Volume 482() pp:171-178
Publication Date(Web):22 July 2014
DOI:10.1016/j.apcata.2014.05.030
Co-reporter:Jian-Hua Xu, Jingxia Li, Wei-Lin Dai, Yong Cao, Hexing Li, Kangnian Fan
Applied Catalysis B: Environmental (21 February 2008) Volume 79(Issue 1) pp:72-80
Publication Date(Web):21 February 2008
DOI:10.1016/j.apcatb.2007.10.008
Co-reporter:Anyuan Yin, Chao Wen, Xiaoyang Guo, Wei-Lin Dai, Kangnian Fan
Journal of Catalysis (16 May 2011) Volume 280(Issue 1) pp:77-88
Publication Date(Web):16 May 2011
DOI:10.1016/j.jcat.2011.03.006
A novel family of heterogeneous Cu–Ni/SiO2 catalysts with appropriate metal ratios displayed outstanding selectivity to methyl glycolate (96%) and to ethylene glycol (98%) in the chemoselective gas-phase hydrogenation of dimethyloxalate. The chemical states of nickel species were found to have a strong influence on the structural evolution of the catalysts and correspondent catalytic behaviors. The selectivity to the two products could be tuned by modulating the chemical states of nickel species. It is shown that oxidative nickel species are helpful in improving the dispersion of copper species because of the enrichment of copper on the surface of the nickel species, thus enhancing the catalytic activity and selectivity to ethylene glycol. The selectivity to methyl glycolate could be greatly improved by the Cu–Ni bimetallic catalyst. An 83% yield of methyl glycolate and a 98% yield of ethylene glycol could be obtained over the bimetallic Cu–Ni catalyst and the NiO-modified catalyst, respectively.Graphical abstractCu–Ni/HMS catalyst exhibited excellent catalytic performance in chemoselective hydrogenation of dimethyloxalate. Methyl glycolate (MG) and ethylene glycol (EG) could be effectively obtained via tuning the surface chemical states of nickel species.Download high-res image (60KB)Download full-size imageHighlights► 86% yield of methyl glycolate and 98% yield of ethylene glycol could be achieved. ► Chemical states of Ni were found to have great effect on the catalytic behaviors. ► Improved catalytic performance were due to the enhanced dispersion of Cu species. ► Methyl glycolate could be obtained over the bimetallic CuNi supported catalyst. ► Enhanced selectivity originated from the synergetic effect of bimetallic Cu and Ni.
Co-reporter:Jie Huang, Wei-Lin Dai, Hexing Li, Kangnian Fan
Journal of Catalysis (15 November 2007) Volume 252(Issue 1) pp:69-76
Publication Date(Web):15 November 2007
DOI:10.1016/j.jcat.2007.09.011
Au/TiO2 catalysts prepared by the deposition–precipitation method showed excellent activity and selectivity in the oxidative cyclization of 1,4-butanediol to γ-butyrolactone, with high yields (>99%) under mild conditions (413 K, 1.25 MPa air). Catalysts with 3–8% gold loading and calcined at 573–673 K were all highly active for the formation of γ-butyrolactone, as demonstrated by XRD, TEM, XPS, ICP and UV–vis DRS results. It is concluded that highly dispersed small (2–10 nm) gold particles are formed with the surface enrichment of gold. The ratio of cationic gold to metallic gold depends on the treatment temperature. These findings, combined with those of the activity tests, lead to the conclusion that the surface metallic nanosized gold particles are active sites. The catalyst can be reused with no drop in activity or selectivity.
Co-reporter:Ruihua Gao, Hui Chen, Yingyi Le, Wei-Lin Dai, Kangnian Fan
Applied Catalysis A: General (15 January 2009) Volume 352(Issues 1–2) pp:61-65
Publication Date(Web):15 January 2009
DOI:10.1016/j.apcata.2008.09.031
Co-reporter:Jie Huang, Wei-Lin Dai, Kangnian Fan
Journal of Catalysis (10 September 2009) Volume 266(Issue 2) pp:228-235
Publication Date(Web):10 September 2009
DOI:10.1016/j.jcat.2009.06.011
Iron oxides in different crystal forms with identical particle size and morphology are employed as supports for gold catalysts. By using the oxidative dehydrogenation of 1,4-butanediol to γ-butyrolactone as the probe reaction, combined with some characterizations such as XRD, TEM, XPS, and H2–TPR, support effect of Au/FeOx catalysts is established in this study. Turnover frequency value follows the order Au/Fe3O4 > Au/α-Fe2O3 > Au/γ-Fe2O3. Size effect of Au/Fe3O4 catalysts with different gold particle size distributions obtained by treating under different atmospheres is also studied for comparison, and the results imply the slight effect of gold particle size. Variation in catalytic behavior of gold catalysts on different iron-oxide supports originates from the discrepancy in gold geometry, gold oxidation state, and gold-support contact interface structures which are caused by difference in support intrinsic properties such as microcrystalline structure and oxidation state.Gold supported on different iron oxides shows different catalytic behavior in the oxidation of 1,4-butanediol to γ-butyrolactone. The support effect is more significant than the gold particle size effect.Download high-res image (58KB)Download full-size image
Co-reporter:Hui Chen, Wei-Lin Dai, Ruihua Gao, Yong Cao, Hexing Li, Kangnian Fan
Applied Catalysis A: General (10 September 2007) Volume 328(Issue 2) pp:
Publication Date(Web):10 September 2007
DOI:10.1016/j.apcata.2007.06.021
Selective oxidation of cyclopentane-1,2-diol to glutaric acid (GAC) over different kinds of materials has been carried out with aqueous hydrogen peroxide. The homogenous tungstic acid catalyst was tried first, which showed a yield of GAC as high as 91.2%. However, the separation, recovering and reusing of the homogeneous catalyst are very difficult, thus restricting its further application in industry. Then tungsten-containing mesoporous silica (W-MCM-41) was next tried as a heterogeneous catalyst. Although the activity was about 20% lower than that of the homogeneous one, it was much more easily to be separated, recovered and reused. It is interesting to find that the phase-transfer material shows the best performance in the reaction, during which the yields of GAC on [π-C5H5NC16H33]2{W2O3[O2]4} (CW) and [π-C5H5NC16H33]3{PO4[WO3]4} (CPW) were 91.3 and 94.3%, respectively. These two materials demonstrated the characteristic features of “reaction-controlled phase-transfer”; the samples dissolved during the reaction and precipitated after the reaction. Therefore, these materials show the advantages of both homogeneous and heterogeneous catalysis and can easily be recovered and reused. The fresh samples and the recovered ones were all characterized by FT-IR, Raman, 31P NMR and XPS spectroscopy. The structures of these two materials all changed after the reaction, polymerizing by forming W–Oc–W (edge-sharing) bonds. XPS results revealed that the recovered samples of CW and CPW are all more stable than the corresponding fresh ones due to the changes of the coordination circumstances.Selective oxidation of cyclopentane-1,2-diol to glutaric acid with aqueous hydrogen peroxide was carried out over different kinds of materials: the homogeneous H2WO4, the heterogeneous W-MCM-41 and the phase-transfer catalysts. The homogeneous and phase-transfer catalysts showed very high activity that the GAC yields were higher than 90% while the heterogeneous and phase-transfer catalysts were convenient to be recovered and reused.
Co-reporter:Ruihua Gao, Xinli Yang, Wei-Lin Dai, Yingyi Le, Hexing Li, Kangnian Fan
Journal of Catalysis (10 June 2008) Volume 256(Issue 2) pp:259-267
Publication Date(Web):10 June 2008
DOI:10.1016/j.jcat.2008.03.017
For the first time, the high-activity, single-site mesoporous WO3-MCF materials were synthesized and characterized by N2 sorption, TEM, UV–vis DRS, UV-Raman, and XPS. It was found that the dispersion and nature of the tungsten species depend strongly on the tungsten oxide content and the support characteristic. The novel catalyst remains a highly ordered mesostructure of the silica support. The catalytic performance of the materials in the epoxidation of cycloocta-1,5-diene with aqueous H2O2 was investigated. The excellent catalytic performance of WO3-MCF in the selective oxidation of cycloocta-1,5-diene was attributed to the presence of isolated tetrahedral {WO4} species and the unique pore structure. The novel catalyst can be easily recycled after reaction and reused many times with no significant loss of activity. The good stability can be attributed to the presence of isolated tungsten species anchored on the support through WOSi covalent bonds.
Co-reporter:Ruihua Gao, Wei-Lin Dai, Xinli Yang, Hexing Li, Kangnian Fan
Applied Catalysis A: General (1 November 2007) Volume 332(Issue 1) pp:138-145
Publication Date(Web):1 November 2007
DOI:10.1016/j.apcata.2007.08.012
Co-reporter:Jia Ren, Yuanyuan Chai, Qianqian Liu, Lu Zhang, Wei-Lin Dai
Applied Surface Science (1 May 2017) Volume 403() pp:
Publication Date(Web):1 May 2017
DOI:10.1016/j.apsusc.2017.01.172
•Ag3PO4 nanoparticles decorated with graphite-like carbon nitride material (g-C3N4).•Synthesized by a template-free in situ precipitation method.•Excellent (7 times higher) photooxidation ability.•Much more stable than pure Ag3PO4 in the photodegradation process.•Formation of heterojunction between Ag3PO4 and g-C3N4 contributed to the separation efficiency.The method of decorating Ag3PO4 nanoparticles with carbon nitride material (g-C3N4) is demonstrated as an efficient pathway to remarkably improve the stability and photocatalytic performance of Ag3PO4 nanoparticles which have been widely used in photocatalysis, but limited by the instability. The improved material herein results in the largely enhanced photocatalytic performance for water purification under visible light irradiation, which was nearly 7 times as high as that of pure Ag3PO4. Meanwhile, the as-obtained materials show the unique stable property, mainly contributed by the protection effect of decorated g-C3N4 sheet. Additionally, the radical trapping experiments revealed that the introduction of g-C3N4 transformed the photocatalytic mechanism to some degree, where O2− played a more important role. The tremendous enhancement in catalytic performance may be attributed to the larger surface area, controllable particle size and the synergistic effect between Ag3PO4 and g-C3N4, promoting the separation efficiency of the photogenerated electron-hole pairs. The decorating system can in principle be broadly put into use for unstable photocatalysts.
Co-reporter:Yuanyuan Cui and Wei-Lin Dai
Catalysis Science & Technology (2011-Present) 2016 - vol. 6(Issue 21) pp:NaN7762-7762
Publication Date(Web):2016/09/16
DOI:10.1039/C6CY01575A
The present work determined the morphology and crystal plane effects of nanoceria on the activity of Cu/CeO2 catalysts in the gas/solid-phase hydrogenation of CO2-derived diethyl carbonate (DEC) to methanol. The effect of the terminating crystalline planes of CeO2 ({100}, {110}, and {111}) on the behaviour of copper species dispersed over CeO2 nanocubes, nanorods and nanoparticles was examined in detail using a variety of characterization techniques. HRTEM studies revealed that CeO2 nanorods were mainly enclosed by {100} and {110} planes, nanoparticles exhibited only {111} surfaces, and nanocubes predominantly displayed {100} planes. Cu/CeO2 nanorods (Cu/Ce-NR) possessed higher Cu+/Cu0 ratios and more oxygen vacancies than Cu/CeO2 nanoparticles (Cu/Ce-NP) and Cu/CeO2 nanocubes (Cu/Ce-NC), which indicated that there was a stronger interaction between Cu and CeO2 nanorods. A test of activity in the hydrogenation of DEC showed that Cu/Ce-NR was more active than Cu/Ce-NP and Cu/Ce-NC, which could be attributed to the higher value of SCu0, surface oxygen mobility and Cu+/Cu0 ratio. These results confirm that the activity of Cu/CeO2 catalysts for the hydrogenation of DEC is greatly affected by the shape/crystal planes of CeO2.
Co-reporter:Anyuan Yin, Xiaoyang Guo, Weilin Dai and Kangnian Fan
Chemical Communications 2010 - vol. 46(Issue 24) pp:NaN4350-4350
Publication Date(Web):2010/05/12
DOI:10.1039/C0CC00581A
Ag/SiO2 prepared by a sol–gel process is highly effective for selective gas-phase hydrogenation of dimethyl oxalate to corresponding alcohols. The catalysts are of great potential as industrially viable and novel catalysts for the production of methyl glycolate and ethylene glycol.
Co-reporter:Anyuan Yin, Chao Wen, Wei-Lin Dai and Kangnian Fan
Journal of Materials Chemistry A 2011 - vol. 21(Issue 25) pp:NaN8999-8999
Publication Date(Web):2011/05/31
DOI:10.1039/C1JM10646E
CuAu/HMS alloy nanoparticles constructed viaammonia-evaporation–deposition–precipitation were prepared and exhibited excellent performance in methyl glycolate synthesis.
Co-reporter:Li Wang, Yuanyuan Chai, Jia Ren, Jing Ding, Qianqian Liu and Wei-Lin Dai
Dalton Transactions 2015 - vol. 44(Issue 33) pp:NaN14634-14634
Publication Date(Web):2015/07/13
DOI:10.1039/C5DT01961C
Novel 3D hierarchical Ag3PO4/MoS2 composites were successfully prepared through a facile and reproducible hydrothermal-in situ precipitation method. The 3D flower-like spherical MoS2 nanoarchitectures acted as an excellent supporting matrix for the in situ growth of Ag3PO4 nanoparticles. The photocatalytic performance of the composites and the effect of the amount of MoS2 were investigated. The obtained hierarchical Ag3PO4/MoS2 composites exhibited significantly enhanced performance for photocatalytic oxidation of Rhodamine B (RhB) compared with pure Ag3PO4 under visible light irradiation. Ag3PO4/MoS2 composites with 15 wt% of MoS2 showed the optimal photoactivity for the degradation of RhB, which was approximately 4.8 times as high as that of pure Ag3PO4. What's more, the optimal Ag3PO4/MoS2 composite also showed better photodegradation efficiency for methyl orange (MO) and p-chlorophenol (4-CP) than pure Ag3PO4. More attractively, the stability of Ag3PO4 was improved after the in situ deposition of Ag3PO4 particles on the surface of MoS2 nanoflakes due to the conductivity of MoS2 itself as electron acceptors. The enhanced performance of the hierarchical Ag3PO4/MoS2 composites under visible light was caused by a synergistic effect including the improved separation of photogenerated charge carriers, boosted light harvesting, a relatively high surface area and matching energy band structures between the two components. Interestingly, the heterostructured Ag3PO4/MoS2 composite reduced the use of the noble metal silver, thereby effectively reducing the cost of the Ag3PO4 based photocatalyst. Ultimately, a MoS2 involved photocatalytic mechanism for the hierarchical Ag3PO4/MoS2 composites was also proposed.
Co-reporter:Li Wang, Jing Ding, Yuanyuan Chai, Qianqian Liu, Jia Ren, Xin Liu and Wei-Lin Dai
Dalton Transactions 2015 - vol. 44(Issue 24) pp:NaN11234-11234
Publication Date(Web):2015/05/11
DOI:10.1039/C5DT01479D
A novel CeO2 nanorod/g-C3N4/N-rGO ternary composite was synthesized using a simple ultrasonic-heat treatment method for application in the photocatalytic degradation of organic pollutants under the irradiation of visible light. This material shows superior photocatalytic activity compared with pure g-C3N4 and CeO2 nanorods, and the photodegradation rate of RhB is up to 2.1-fold higher than that of the g-C3N4/N-rGO (at the optimum content of 0.25 wt% N-rGO) catalyst when the content of CeO2 nanorods was 2 wt%. The enhancement of photocatalytic activity could be attributed to the synergistic effect among CeO2, g-C3N4 and N-rGO (serves as a conductive network), which was found to lead to more efficient separation of photogenerated electron–hole pairs, resulting in the effective photodegradation of organic pollutants. In addition, superoxide radical anions (˙O2−) and holes (h+) were considered as the main reactive species during the photodegradation process, and the ternary composite also exhibited preferable stability for the decomposition of RhB. This work provides an in-depth perspective for understanding the N-doped graphene-involved photocatalytic mechanism.
Co-reporter:Chao Wen, Yuanyuan Cui, Wei-Lin Dai, Songhai Xie and Kangnian Fan
Chemical Communications 2013 - vol. 49(Issue 45) pp:NaN5197-5197
Publication Date(Web):2013/04/17
DOI:10.1039/C3CC40570B
The variation of the supports on the Cu/SiO2 catalyst plays an important role in the catalytic performance for hydrogenation of dimethyl oxalate. The loss of silica in the form of tetramethoxysilane from the support under the reaction conditions is responsible for the deactivation of the Cu/SiO2 catalyst.
Co-reporter:Xi Chen, Yuanyuan Cui, Chao Wen, Bin Wang and Wei-Lin Dai
Chemical Communications 2015 - vol. 51(Issue 72) pp:NaN13778-13778
Publication Date(Web):2015/07/22
DOI:10.1039/C5CC05030H
Continuous fixed-bed catalytic hydrogenation of ethylene carbonate (EC) to methanol and ethylene glycol (EG), an emerging synthetic process of methanol via indirect conversion of CO2, was successfully performed over Cu/HMS catalysts prepared by the ammonia evaporation (AE) method. The catalysts possessed superb performance with a conversion of 100% and a selectivity to methanol of 74%.