Co-reporter:Shuo Cui, Shixiang Lu, Wenguo Xu, Bei Wu
Journal of Solid State Chemistry 2017 Volume 254(Volume 254) pp:
Publication Date(Web):1 October 2017
DOI:10.1016/j.jssc.2017.06.017
•Superhydrophobic Pt3Fe/Fe composed was fabricated on iron sheet.•The growth process is without using any seed and organic solvent.•Superhydrophobic Pt3Fe/Fe composed show superior oil/water separation capacity.•Superhydrophobic Pt3Fe/Fe composed show high photocatalytic activity.Well-defined Pt3Fe/Fe superhydrophobic materials on iron sheet with special properties, such as corrosion resistance, superhydrophobicity and superoleophilicity, was fabricated. The fabrication process involved etching in hydrochloric acid aqueous solution and simple replacement deposition process without using any seed and organic solvent, and then annealing. The electrochemical measurements show that the resultant surface in 3.5% sodium chloride solution displays good corrosion resistance. Also, it is proved that the obtained surface has better mechanical abrasion resistance via scratch test. The superoleophilicity and low water adhesion force of the obtained surface endow it high oil/water separation capacity. The as-prepared nanocomposites display enhanced catalytic activity and kinetics toward degradation of methyl orange. In particular, it possesses the most efficient degradation capacity (95%) towards methyl orange at a high concentration (17.5 mg/L) in 80 min. The improved stability and excellent catalytic activity of the Pt3Fe/Fe nanocomposites promise new opportunities for the development of waste water treatment.The illustration of application of superhydrophobic Pt3Fe/Fe surfaceDownload high-res image (160KB)Download full-size image
Co-reporter:Bei Wu, Shixiang Lu, Wenguo Xu, Shuo Cui, Jingyan Li, PengFei Han
Surface and Coatings Technology 2017 Volume 330(Volume 330) pp:
Publication Date(Web):1 December 2017
DOI:10.1016/j.surfcoat.2017.09.060
•A composite Co-Al alloy superhydrophobic surface was prepared.•The as-prepared surfaces exhibited excellent superhydrophobicity.•The superhydrophobic surface exhibited good corrosion resistance.•The superhydrophobic surface exhibited good catalytic activity.A textured flower-like cobalt superhydrophobic surface (SHS) with a water contact angle of 160° and a sliding angle of less than 1° was fabricated on aluminum substrate by immersing the processed aluminum sheets perpendicularly into cobalt (II) nitrate aqueous solution and followed by annealing treatment. The morphology and chemical composition of the SHS were characterized using scanning electron microscopy (SEM), atomic force microscopy (AFM), X-ray diffraction pattern (XRD), Energy-dispersive spectroscopy (EDS) and X-ray photoelectron spectroscopy (XPS). The corrosion resistance of the samples was characterized via polarization, Nyquist and bode modulus plots. The photocatalysis of samples was also studied by catalytic degradation of methyl orange under a UV lamp (λ = 365 nm) with a light intensity of 8 W. The cobalt superhydrophobic sample not only exhibited excellent catalytic properties, but also substantially improved the corrosion resistance of aluminum substrate.Download high-res image (84KB)Download full-size image
Co-reporter:Yuanyuan Cheng, Shixiang Lu, Wenguo Xu, Rabah Boukherroub, Sabine Szunerits, Wei Liang
Journal of Alloys and Compounds 2017 Volume 723(Volume 723) pp:
Publication Date(Web):5 November 2017
DOI:10.1016/j.jallcom.2017.06.241
•NiO/ZnO SHS have been fabricated on zinc substrate via deposition and anneal.•Anneal treatment is important for the combination between substrate and coatings.•Surface wettability is controlled and influenced by various conditions.•SHS exhibit exquisite roll-down, anti-corrosion and anti-abrasion properties.The paper reports on the preparation of NiO/ZnO superhydrophobic surfaces (SHS) on zinc via chemical substitution/deposition and thermal annealing. The resulting surfaces display superhydrophobic behavior with a water contact angle (WCA) of 153° and a sliding angle (SA) of ∼5° without the use of any additional organic coating. Using the Cassie-Baxter equation, it is found that about 91.6% serves as the contact area of the water droplet and air, leading to the roll down property of the water droplet on the surface. The surface superhydrophobicity is controlled and influenced by various preparation conditions: the thermal treatment, which causes the generation of NiO and ZnO layers, and the formation of polygonal honeycomb structures and disappearance of silk flower-like clusters. The resulting NiO/ZnO SHS exhibit roll down, anti-corrosion and anti-abrasion properties. The corrosion current density of the NiO/ZnO SHS (5.7 × 10−4 A cm−2) is decreased by more than 1 order of magnitude when compared to the untreated Zn surface (1.4 × 10−3 A cm−2). EIS results also indicate that the SHS possesses higher anti-corrosion performance. The superhydrophobic sample, after annealing treatment, can sustain a collapsing force of about 7.8 N, which is better than the superhydrophilic sample without annealing treatment (∼5.2 N). This controlled fabrication process may offer new avenues for designing superhydrophobic surfaces with corrosion resistance for more practical applications.Download high-res image (266KB)Download full-size image
Co-reporter:Yuanyuan Cheng;Shixiang Lu;Hong Tao
New Journal of Chemistry (1998-Present) 2017 vol. 41(Issue 12) pp:5205-5214
Publication Date(Web):2017/06/12
DOI:10.1039/C7NJ00658F
Herein, Cu–CuO–Fe2O3/Fe superhydrophobic surfaces (SHSs) were successfully fabricated on an iron substrate via chemical substitution deposition and subsequent annealing treatment. The resulting surfaces exhibit remarkable superhydrophobicity with a water CA of 165 ± 2° and an SA of approximately 0° without any organic modification. The surface morphology and chemical compositions were investigated using field emission scanning electron microscopy (FESEM), energy dispersive spectroscopy (EDS), X-ray powder diffraction (XRD), and X-ray photoelectron spectroscopy (XPS); moreover, the surface roughness was analyzed via atomic force microscopy (AFM). The thermal treatment, which caused generation of a new chemical substance and formation of micro-/nano-binary architectures, was important for superhydrophobicity and also enhanced the affinity of the iron substrate for the coatings. The annealing temperature and time were further investigated to explain the significance of the surface morphology and chemical composition in the fabrication of the optimal SH samples under appropriate conditions. The resulting SHSs exhibit roll-down, anti-abrasion, and anti-corrosion properties, which may have significant potential value for more applications.
Co-reporter:Yuanyuan Cheng, Shixiang Lu, Wenguo Xu, Huidong Wen and Juan Wang
Journal of Materials Chemistry A 2015 vol. 3(Issue 32) pp:16774-16784
Publication Date(Web):10 Jul 2015
DOI:10.1039/C5TA03979G
Superhydrophobic Au–Zn alloy surfaces have been fabricated successfully on a zinc substrate via chemical substitution deposition and subsequent annealing treatment. The resulting surfaces exhibited remarkable superhydrophobicity with a WCA of 170 ± 2° and a WSA smaller than 1° without any organic modification. The surface morphologies and chemical compositions were investigated using field emission scanning electron microscopy (FESEM), energy-dispersive spectroscopy (EDS), X-ray powder diffraction (XRD) and X-ray photoelectron spectroscopy (XPS), and the surface roughness was analyzed by atomic force microscopy (AFM). The theoretical mechanism for superhydrophobicity and wettability were also analyzed. The surface wettability changed from superhydrophilicity to superhydrophobicity with a stable Cassie–Baxter state via thermal treatment, which caused the generation of Au–Zn alloys (including AuZn3 and AuZn) and ZnO, and the formation of micro-/nano-binary architectures. The resulting superhydrophobic Au–Zn alloy surfaces exhibited exquisite roll-down, self-cleaning, and excellent anti-corrosion properties, and also had a firm mechanical property about 10 N, and this might have important values for more potential applications. The corrosion current density was reduced by more than 2 orders of magnitude for the resulting superhydrophobic surface in comparison with the untreated zinc surface and this should be ascribed to the contribution of Au–Zn alloys on the surface.
Co-reporter:Yuanyuan Cheng, Shixiang Lu, Wenguo Xu and Huidong Wen
RSC Advances 2015 vol. 5(Issue 20) pp:15387-15394
Publication Date(Web):27 Jan 2015
DOI:10.1039/C4RA12909A
Superhydrophobic Au–AlAu4–Al2O3 surfaces have been successfully fabricated on aluminum substrate via immersion in chloroauric acid (HAuCl4) aqueous solution and subsequent annealing treatment. The morphologies of the surfaces exhibit dendritic structures. The surface with remarkable superhydrophobic properties has a water contact angle of 171 ± 2° and a sliding angle of approximately 0°. The effects of the immersion time, immersion concentration, annealing time and annealing temperature on surface wettability were investigated in detail. The corrosion resistance of the untreated aluminum surface and the resulting Au–AlAu4–Al2O3 surface were also investigated via the Tafel extrapolation method. The corrosion current densities are reduced by more than 1 order of magnitude for the resulting surface in comparison with the untreated aluminum surface. The anticorrosion properties of the surfaces get better over the immersion time and this may be due to the generation of corrosion products, which can prevent the corrosion process and protect the substrates. Moreover, the low current density of the resulting superhydrophobic surface demonstrates its excellent corrosion resistance.
Co-reporter:Yuanyuan Cheng, Shixiang Lu and Wenguo Xu
New Journal of Chemistry 2015 vol. 39(Issue 8) pp:6602-6610
Publication Date(Web):23 Jun 2015
DOI:10.1039/C5NJ00651A
A superhydrophilic surface with a static water contact angle of 4° ± 2° via two-step immersion process and a superhydrophobic surface with a static water contact angle of 169° ± 2° and a sliding angle of almost 0° via successive thermal treatment have been successfully fabricated on aluminum substrates. Surface morphologies and chemical compositions were investigated using field emission scanning electron microscopy, X-ray powder diffraction and X-ray photoelectron spectroscopy, and the formation mechanism was also analyzed. The thermal treatment, which causes the generation of oxides and the appearance of nano-sized particles, is very important for the surface characteristic transformation from superhydrophilicity to superhydrophobicity. The effects of various experimental parameters on wettability, corrosion resistance, anti-icing and deicing properties, stability and large-area preparation were also studied. The corrosion rate of the as-prepared superhydrophobic surface decreases by about 57.6 times compared with that of the untreated aluminum surface and about 34.8 times compared with that of the pure copper surface. These excellent properties of the superhydrophobic surface may be favorable for its potential applications and industrialization.
Co-reporter:Haifeng Zhang, Shixiang Lu, Wenguo Xu, Feng Yuan
Surface Science 2014 Volume 625() pp:30-36
Publication Date(Web):July 2014
DOI:10.1016/j.susc.2014.03.003
•H3-22 is the most stable structure in all the considered Si/ZnO (0001) system.•For H3-33 and T4-33, Si3 clusters are formed. It changes to Si4 cluster for T4-44.•The absorbed Si atoms decrease the band gaps of the Si/ZnO (0001) system.•H3-11 has the most significant utilization of sunlight, and then is H3-22.Si atoms adsorbed on ZnO (0001) surface have been investigated by first principles calculations. In the considered Si/ZnO (0001) system, H3-22 is the most stable structure and then is T4-11. The adsorbed Si atoms show many interesting behaviors. For H3-22, the adsorbed Si atoms migrate from two fixed H3 sites to one T4 site and one H3 site. For T4-33 and H3-33, the adsorbed three Si atoms form triangles. For T4-44, one more adsorbed Si atom leads the triangles to change to quadrangle. The triangular or quadrilateral Si structures just belong to S3 and S4 clusters. The electronic properties indicate that the absorbed Si atoms decrease the band gaps of the Si/ZnO (0001) system. The width and position of the band gaps are influenced by the adsorption models. From the optical properties analysis of T4-11 and H3-11, it indicates that H3 sites play a critical role in the red shift of absorption edge and T4 sites almost have little contribution. For H3-33, H3-44 and T4-44, the result indicates that the formed Si clusters lead to a slightly blue shift phenomenon and prevent the absorption of sunlight in the lower energy range.
Co-reporter:Feng Yuan, Haifeng Zhang, Shixiang Lu, Wenguo Xu
Surface Science 2014 Volume 628() pp:126-131
Publication Date(Web):October 2014
DOI:10.1016/j.susc.2014.06.003
•H adsorption and O vacancy on the TiO2(011) surface have been investigated.•Only the O vacancy at the side O site gives rise to a Ti-3d like band gap state.•H adsorption or O vacancy enhances the optical absorptions in the areas of infrared.The hydroxylated and reduced rutile TiO2(011)-2 × 1 surfaces have been investigated by means of first-principles density functional theory calculations. For the H adsorption and O vacancy on the rutile TiO2(011)-2 × 1 surface, we investigated three different surface O sites. Based on the adsorption and formation energy calculations, we find that the top O is an energetically preferential site for the adsorption of H atom or the formation of O vacancy. The calculated electronic structures indicate that the energetically preferential O site cannot create a band gap state; only the O vacancy at the side O site gives rise to a Ti-3d like defect level at the edge of the conduction band. It is worth mentioning that all considered configurations of the H adsorption and O vacancy on the rutile TiO2(011)-2 × 1 surface obviously enhance the optical absorptions in the areas of infrared, not just the rutile TiO2(011)-2 × 1 surface only has a good absorption edge in the visible light region.
Co-reporter:Feng Yuan, Shixiang Lu, Wenguo Xu, Haifeng Zhang
Surface Science 2014 Volume 621() pp:88-93
Publication Date(Web):March 2014
DOI:10.1016/j.susc.2013.11.003
•A theoretical simulation for the surface reconstruction was carried out.•The calculated band gap of 2.08 eV reproduces the experimental value ~ 2.10 eV.•The calculated optical absorption edge shifts to the visible light range.This work investigates surface reconstruction, electronic structure, and optical properties of the rutile TiO2(011)-2 × 1 surface using means of density functional theory calculations. For the surface reconstruction of the rutile TiO2(011) surface, a theoretical simulation with forming from bulk truncation to the 2 × 1 reconstruction was carried out. The calculated band structure shows a direct band gap at Г point, and the band gap of 2.08 eV reproduces the experimental measurement value ~ 2.10 eV very well. Analysis of the density of states reveals that no surface state was introduced into the forbidden gap. Not coincidentally, the calculated optical absorption edge at about 2.01 eV further clarifies the band gap narrowing and such an intrinsic band gap nature effectively pushes the optical absorption edge into the visible light. Hence, our theoretical calculations provide evidence that the rutile TiO2(011)-2 × 1 surface possesses high photocatalytic activity.
Co-reporter:Xiaofeng Shi, Shixiang Lu, Wenguo Xu
Materials Chemistry and Physics 2012 Volume 134(2–3) pp:657-663
Publication Date(Web):15 June 2012
DOI:10.1016/j.matchemphys.2012.03.046
Superhydrophobic surfaces were prepared via immersing the clean perpendicular zinc substrates into aqueous copper chloride (CuCl2) solution and followed by annealing in dry air. Two Superhydrophobic models were obtained by controlling the concentration of CuCl2 aqueous solution. One had a high water contact angle (CA) of 162 ± 2° with a small sliding angle SA of less than 2 ± 1°, which was identified with Cassie–Baxter model, the other had a high CA of larger than 150° with a high adhesion, which was identified with Gecko model. CuZn5–ZnO–CuO micro–nano binary structure leads to superhydrophobicity of the surface. Wettability and durability of surfaces were investigated and a theoretical explanation on superhydrophobic surfaces is presented. Durability test was carried out to study properties of the surface. Formation mechanism of the surface was also explained.Graphical abstractThe zinc substrate was modified by chemical displacement at a perpendicular position and annealed to form the micro–nano binary structure with CuZn5–ZnO–CuO/zinc of Cassie–Baxter model and Gecko model, controlled by CuCl2 aqueous solution concentrations.Highlights► Micro–nano binary structure of Cassie–Baxter model and Gecko model are obtained. ► CuZn5–ZnO–CuO/zinc micro–nano binary structure leads to superhydrophobicity. ► The annealing plays an important role in superhydrophobicity of metallic materials. ► The superhydrophobic surface with Cassie–Baxter model shows a good durability.
Co-reporter:Haifeng Zhang, Zhuo Tao, Wenguo Xu, Shixiang Lu, Feng Yuan
Computational Materials Science 2012 Volume 58() pp:119-124
Publication Date(Web):June 2012
DOI:10.1016/j.commatsci.2012.01.016
Electronic structure, optical properties and photocatalytic activity of S-doped ZnO are investigated by density functional theory (DFT). The configurations with the substitution of O by one and two S atoms in different positions (SO, far-2SO and near-2SO) are considered, and zinc and oxygen vacancies introduced by SO doping (SO–VZn and SO–VO) are also considered. For SO-doped ZnO, S3p states locate above the top of the valence band and mix with O2p states, leading to band gap narrowing, but the influence is slight with the increase of doping concentration. The imaginary parts of dielectric functions and absorption coefficients display that S atoms doping is not the critical factor for improving the photocatalytic activity. The absorption coefficient of introduced native defect (VO and VZn) shows different features in low energy range. The existence of VO in SO-doped ZnO leads to a strong absorption in UV-light range and VZn plays a critical role in visible-light absorption, which may improve the photocatalytic activity of ZnO in the UV-visible light range, corporately.Graphical abstractThe first absorption peak of SO–VZn doped ZnO is located at 2.73 eV, indicating the VZn enhances the utilization rate of sunlight. The existence of VO leads to a strong absorption in UV-light range. Zn and O vacancy introduced by S dopants play a critical role in the photocatalytic application of ZnO..Highlights► S3p states localizing above the top of the valence band lead to band gap narrowing. ► S3p states hybridization with O2p states also lead to band gap narrowing. ► S dopants have a little contribution to photocatalytic activity. ► Defects (VO and VZn) realize photocatalytic application in UV-visible light range.
Co-reporter:Tao Ning, Wenguo Xu, Shixiang Lu
Applied Surface Science 2011 Volume 258(Issue 4) pp:1359-1365
Publication Date(Web):1 December 2011
DOI:10.1016/j.apsusc.2011.09.064
Abstract
Stable superhydrophobic surfaces have been effectively fabricated on the zinc substrates through one-step platinum replacement deposition process without the further modification or any other post processing procedures. The effect of reaction temperatures on the surface morphology and wettability was studied by using SEM and water contact angle (CA) analysis. Under room temperature, the composite structure formed on the zinc substrate was consisted of microscale hexagonal cavities, densely packed nanoparticles layer and micro/nanoscale structures like the flowers. The structure has exhibited great surface roughness and porosity contributing to the superhydrophobicity where the contact angle could reach an ultra high value of around 170°. Under reaction temperature of 80 °C, the composite structure, on the other hand, was hierarchical structure containing lots of nanoscale flowers and some large bushes and showed certain surface roughness (maximum CA value of about 150°). In addition, an optimal superhydrophobic platinum surface was able to provide an effective anticorrosive coating to the zinc substrate when it was immersed into an aqueous solution of sodium chloride (3% NaCl) for up to 20 days. The corrosion process was monitored through electrochemical means and the results are compared with those of unprotected zinc plates.
Co-reporter:Wenguo Xu, Tao Ning, Xiaochan Yang, Shixiang Lu
Applied Surface Science 2011 Volume 257(Issue 11) pp:4801-4806
Publication Date(Web):15 March 2011
DOI:10.1016/j.apsusc.2010.12.059
Abstract
Stable superhydrophobic surfaces were fabricated on the zinc substrates through simple silver replacement deposition process with the modification of octadecyl mercaptan. The effects of reaction conditions on the surface morphology and wettability of the prepared surfaces were carefully studied. The results show that the fabrication of a best superhydrophobic surface depends largely on the moderate reactant concentration. When the concentration of AgNO3 solution was 2 mmol/L, the zinc substrate was covered by a dendritic outline structure. Aggregated silver nanoparticles were formed on the substrate in accordance with some certain laws, exhibiting great surface roughness. The typical hierarchical micro-nanostructures, flower-like structures and porous structures also could be found from the SEM images. The maximal water contact angle (CA) value of about 161 ± 2°, and the minimal sliding angle (SA) of about 2° were obtained under the same reaction condition.
Co-reporter:Wenguo Xu, Xiaofeng Shi, Shixiang Lu
Materials Chemistry and Physics 2011 Volume 129(Issue 3) pp:1042-1046
Publication Date(Web):3 October 2011
DOI:10.1016/j.matchemphys.2011.05.053
Superhydrophobic surface was prepared via immersing the clean perpendicular zinc substrate into aqueous copper (II) chloride (CuCl2) solution and followed by anneal under the humid condition. The prepared samples were characterized by powder X-ray diffraction analysis, X-ray photoelectron spectroscopy, energy-dispersive X-ray spectroscopy (XPS), and scanning electron microscopy (SEM), and energy-dispersive X-ray spectrometry analysis (EDX). SEM images of the films showed that the resulted surfaces exhibit micro–nano binary structures. The resulting surfaces had a high water contact angle (CA) of larger than 150° as well as a small sliding angle (SA) of less than 6°. Cu–Zn alloy formed by chemical displacement. Crystal CuZn5 formed via crystal transition via anneal treatment. Crystal ZnO formed in air or under the humid condition. The CuZn5–ZnO micro–nano binary structures leads to the surface superhydrophobicity.Graphical abstractThe nano-grains on the micro-pillars are formed at the most thermodynamically active sites for saturation, precipitation of the zinc atoms and the surface effect of the micro structure in the process of heat treatment. The micro sized pillars and the nano sized grain composed a micro–nano binary structure, which is analogous to that of the lotus leaf.Highlights► Cu–Zn alloy formed via chemical displacement at a perpendicular way. ► Crystal CuZn5 and ZnO formed via anneal treatment in humidity. ► Micro-pillars and nano-grain composed a micro–nano binary structure. ► Micro–nano surfaces prepared exhibited good superhydrophobicity.
Co-reporter:Shixiang Lu, Yiling Chen, Wenguo Xu, Wei Liu
Applied Surface Science 2010 Volume 256(Issue 20) pp:6072-6075
Publication Date(Web):1 August 2010
DOI:10.1016/j.apsusc.2010.03.122
Abstract
Superhydrophobic surface was prepared by sol–gel method on aluminum substrate via immersing the clean pure aluminum substrate into the solution of zinc nitrate hexahydrate (Zn(NO3)2·6H2O) and hexamethylenetetraamine (C6H12N4) at different molar ratios and unchanged 0.04 mol/L total concentration, then heated at 95 °C in water bath for 1.5 h, subsequently modified with 18 alkanethiols or stearic acid. When the molar ratios of Zn(NO3)2·6H2O and C6H12N4 were changed from 10:1 to 1:1 the contact angle was higher than 150°. The best prepared surface had a high water contact angle of about 154.8°, as well as low angle hysteresis of about 3°. The surface of prepared films using Zn(NO3)2·6H2O and C6H12N4 composed of ZnO and Zn–Al LDH, and Al. SEM images of the film showed that the resulting surface exhibits different flower-shaped wurtzite zinc oxide microstructure and porous Zn–Al LDH. The special flowerlike and porous architecture, along with the low surface energy leads to the surface superhydrophobicity.
Co-reporter:WenGuo Xu, SuZhen Cheng, ShiXiang Lu
Journal of Molecular Structure: THEOCHEM 2009 900(1–3) pp: 77-83
Publication Date(Web):30 April 2009
DOI:10.1016/j.theochem.2008.12.027
Co-reporter:S.N. Dang, S.X. Lu, W.G. Xu, J. Sa
Journal of Non-Crystalline Solids 2008 Volume 354(45–46) pp:5018-5021
Publication Date(Web):15 November 2008
DOI:10.1016/j.jnoncrysol.2008.07.027
The precursor of Fe2O3 was prepared by chemical precipitation method with sodium hydroxide (NaOH) and iron chloride hexahydrate (FeCl3 · 6H2O). The samples annealed at different temperature were characterized by means of X-ray diffraction (XRD) and infrared absorption spectroscopy (IR). Degradation of reactive dye in aqueous solution was used to evaluate the catalytic performance of the Fe2O3. The experiments of degradation had been done in dark place. The experimental results indicated that the catalytic property of the precursor of α-Fe2O3 was excellent. The mechanism of the degradation of reactive dye in aqueous solution was investigated by comparing the data in the absence and presence of oxygen. The precursor of α-Fe2O3 annealed at 300 °C was the best. The degradation rate of reactive brilliant blue X-BR could exceed 95% in 8 min at 25 °C when the concentration of the precursor of α-Fe2O3 was 0.1 g/L. The mechanism of the catalytic oxidation reaction was investigated by comparing the X-BR catalytic oxidation data in the absence and presence of oxygen.
Co-reporter:Wen-Guo Xu, Xiao-Fang Liu, Shi-Xiang Lu
Journal of Molecular Structure: THEOCHEM 2008 Volume 864(1–3) pp:80-84
Publication Date(Web):15 September 2008
DOI:10.1016/j.theochem.2008.06.005
A series of polyazidoprismanes, C6H6−n(N3)n (n = 1–6), has been designed computationally. We have calculated the heats of formation (HOFs) of the title compounds by using density functional theory (DFT) with the 6-31G∗∗ basis set. We chose [3]prismane C6H6-D3h as a reference compound in the process of designing isodesmic reactions. The relationship between the HOFs and the molecular structures is discussed. The results have shown that the HOFs of the title compounds gradually increase with increasing number of azido groups. On average, the contribution of one azido group to the heat of formation is about 348.8 and 349.3 kJ/mol at the B3LYP and B3P86 levels, respectively. The relative stabilities of the title compounds are discussed in terms of the calculated HOFs, and the energy gaps between the frontier orbitals. The interactions of the azido groups in these polyazidoprismanes are also discussed. The results have not only shown that these compounds may be used as high-energy–density materials, but also provide some useful information for further investigation.
Co-reporter:Wenguo Xu, Suzhen Cheng, Shixiang Lu
Journal of Molecular Structure: THEOCHEM 2008 Volume 863(1–3) pp:28-32
Publication Date(Web):30 August 2008
DOI:10.1016/j.theochem.2008.05.010
Optimized molecular structures, electron affinities, and IR-active vibrational frequencies have been predicted using five different hybrid Hartree–Fock/density functional theory (DFT) methods for a series of mono-, di-substituted SF6 compounds. The basis set used in this work is of double-ζ plus polarization quality with additional diffuse s- and p-type functions, denoted DZP++. These methods have been carefully calibrated [J.C. Rienstra-Kiracofe, G.S. Tschumper, H.F. Schaefer, S. Nandi, G.B. Ellison, Chem. Rev. 102 (2002) 231]. The equilibrium configurations of the anions CF3SF4CH3- and CF3SF4CF3- are found to be a zigzag geometry with 2A electronic state. Three different types of the neutral-anion energy separation reported in this work are the adiabatic electron affinity (EAad), the vertical electron affinity (EAvert), and the vertical detachment energy (VDE). The most reliable adiabatic electron affinities of the mono-, di-substituted SF6 compounds obtained at the KMLYP function are 1.48 eV (SF6), 3.20 eV (SF5Cl), 3.49 eV (SF5Br), 1.59 eV (SF5CF3), 3.21 eV (CF3SF4Cl), 3.59 eV (CF3SF4Br), 1.36 eV (CF3SF4CH3), 2.32 eV (CF3SF4CF3), respectively.
Co-reporter:Wen Guo Xu, Rui Chun Zhang, Shi Xiang Lu, Yuan Chun Zhang
Journal of Molecular Structure: THEOCHEM 2008 Volume 864(1–3) pp:1-5
Publication Date(Web):15 September 2008
DOI:10.1016/j.theochem.2008.05.029
The equilibrium geometries, total energies and harmonic vibrational frequencies of planar low-lying states for Si2BX (X = Li, K, O, S) species are investigated at B3LYP/6-311+G∗ and B3PW91/6-311+G∗ levels. The research results show that for Si2BLi, Si2BK and Si2BS species, the C2v isomer is the most stable planar structure, and for Si2BO species, the Cs isomer is the most stable planar structure. Negative nucleus independent chemical shift (NICS) values indicate the existence of aromaticity in planar structures for these species. A detailed molecular orbital (MO) analysis further reveals that a delocalized π MO for two isomers of Si2BX (X = Li, K, O, S) strengthens the structural stability and make these species show strongly aromatic character.
Co-reporter:Wen Guo Xu, Rui Chun Zhang, Shi Xiang Lu, Yuan Chun Zhang
Journal of Molecular Structure: THEOCHEM 2008 Volume 859(1–3) pp:18-21
Publication Date(Web):30 June 2008
DOI:10.1016/j.theochem.2008.02.032
Clusters XSi2Y (X = Al, Ga and Y = P, As) are theoretically investigated using density functional theory (DFT) methods at the B3LYP/6-311+G* and B3PW91/6-311+G* levels of theory. The calculated results showed that for AlSi2P AlSi2As and PSi2Ga species, the C2v isomer is the ground state, respectively, whereas for GaSi2As species, the Cs isomer is the ground state. The wiberg bond index (WBI) suggested the existence of delocalization. Negative nucleus-independent chemical shift (NICS) values indicated that a strong ring current exists in two isomers of those species. A detailed molecular orbital (MO) analysis further revealed that two isomers of these species have π aromaticity, and the two delocalized π electrons does agree well with the (4n + 2) Huckel rule, which is closely connected with the concept of the aromaticity.
Co-reporter:Wenguo Xu, Wangjun Bai
Journal of Molecular Structure: THEOCHEM 2008 Volume 863(1–3) pp:1-8
Publication Date(Web):30 August 2008
DOI:10.1016/j.theochem.2008.03.035
The molecular structures and electron affinities of the SeOn /SeOn- (n = 1–5) species were examined using hybrid Hartree–Fock/density functional theory(DFT). The basis set used in this work was of double-ζ plus polarization quality with additional diffuse s-and p-type functions, denoted DZP++. Seven different density functionals (B3LYP, BLYP, BHLYP, BP86, B3P86, BPW91, and B3PW91) were used in this work. The ground state structures of the SeOn (n = 1–5) was explored in this work. The SeO have a 3Σg− ground state, the SeO2 have an open C2V (ozone-like) structure. For the SeO3, D3h structure is turn to be ground state. The SeO4 has C2V (ozone-like) structure, and The SeO5 has C2 structure. The most reliable adiabatic electron affinities, obtained at the DZP++ BLYP and DZP++ BPW91 level of theory, are be1.38 or 1.40 eV (SeO), 1.87 or 1.89 eV (SeO2), 3.28 or 3.23 eV (SeO3), 4.98 or 4.79 eV (SeO4), 6.15–6.12 eV (SeO5). The BHLYP bond length of the SeO atom, SeO2 molecules predicted by this work are in reasonable agreement with the experimental results. The dissociation energies predicted by the B3P86 method are the most reliable. For the vibrational frequencies of Selenium Oxygen, the B3LYP methods produce good predictions compared with the limited experiments.
Co-reporter:Wenguo Xu, Wangjun Bai
Journal of Molecular Structure: THEOCHEM 2008 Volume 854(1–3) pp:89-105
Publication Date(Web):15 April 2008
DOI:10.1016/j.theochem.2007.12.040
The molecular structures and electron affinities of the Sen/Sen-(n=1–5) species were examined using hybrid Hartree–Fock/density functional theory (DFT). The basis set used in this work was of double-ζ plus polarization quality with additional diffuse s- and p-type functions, denoted DZP++. Seven different density functionals (B3LYP, BLYP, BHLYP, BP86, B3P86, BPW91 and B3PW91) were used in this work. The ground state structures of the Sen (n = 2–5) was explored in this work. The Se2 have a 3Σg- ground state, the Se3 have an open C2V(ozone-like) structure with B3LYP, BLYP, BP86, BPW91 methods and a cyclic D3h structure with BHLYP, B3P86, B3PW91. For the Se4, BHLYP method predict a triplet C2h structure and B3LYP, BLYP, B3P86, BP86, B3PW91 and BPW91 methods turn to be the structure with C2v symmetry. The Se5 have an envelope-shaped structure. The most reliable adiabatic electron affinities, obtained at the DZP++ BHLYP level of theory, are 1.99 eV (Se), 1.88 eV (Se2), 2.75 eV (Se3), 2.72 eV (Se4), 2.10 eV (Se5). The BHLYP adiabatic electron affinities of the Se atom, Se2 molecules predicted by this work are in reasonable agreement with the experimental results. The first dissociation energies for the neutral aluminum clusters predicted by the DFT methods are 3.05–3.99 eV (Se2), 1.44–2.29 eV (Se3), 2.28–3.94 eV (Se4), 2.44–2.98 eV (Se5). The dissociation energies predicted by the BHLYP method are the most reliable. For the vibrational frequencies of Selenium, the B3LYP and BHLYP methods produce good predictions compared with the limited experiments.
Co-reporter:Wenguo Xu, Hongqin Liu, Shixiang Lu, Jinming Xi and Yanbin Wang
Langmuir 2008 Volume 24(Issue 19) pp:10895-10900
Publication Date(Web):September 6, 2008
DOI:10.1021/la800613d
Superhydrophobic surfaces were obtained on copper and galvanized iron substrates by means of a simple solution-immersion process: immersing the clean metal substrates into a methanol solution of hydrolyzed 1H,1H,2H,2H-perfluorooctyltrichlorosilane (CF3(CF2)5(CH2)2SiCl3, FOTMS) for 3−4 days at room temperature and then heated at 130 °C in air for 1 h. Both of the resulting surfaces have a high water contact angle (CA) of larger than 150.0° as well as a small sliding angle (SA) of less than 5°. The formation and structure of the superhydrophobic surfaces were characterized by means of scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and energy-dispersive X-ray spectrometry (EDX). SEM images showed that both of the resulting surfaces exhibited special hierarchical structure. The special hierarchical structure along with the low surface energy leads to the high surface superhydrophobicity.
Co-reporter:Yuanyuan Cheng, Shixiang Lu, Wenguo Xu, Huidong Wen and Juan Wang
Journal of Materials Chemistry A 2015 - vol. 3(Issue 32) pp:NaN16784-16784
Publication Date(Web):2015/07/10
DOI:10.1039/C5TA03979G
Superhydrophobic Au–Zn alloy surfaces have been fabricated successfully on a zinc substrate via chemical substitution deposition and subsequent annealing treatment. The resulting surfaces exhibited remarkable superhydrophobicity with a WCA of 170 ± 2° and a WSA smaller than 1° without any organic modification. The surface morphologies and chemical compositions were investigated using field emission scanning electron microscopy (FESEM), energy-dispersive spectroscopy (EDS), X-ray powder diffraction (XRD) and X-ray photoelectron spectroscopy (XPS), and the surface roughness was analyzed by atomic force microscopy (AFM). The theoretical mechanism for superhydrophobicity and wettability were also analyzed. The surface wettability changed from superhydrophilicity to superhydrophobicity with a stable Cassie–Baxter state via thermal treatment, which caused the generation of Au–Zn alloys (including AuZn3 and AuZn) and ZnO, and the formation of micro-/nano-binary architectures. The resulting superhydrophobic Au–Zn alloy surfaces exhibited exquisite roll-down, self-cleaning, and excellent anti-corrosion properties, and also had a firm mechanical property about 10 N, and this might have important values for more potential applications. The corrosion current density was reduced by more than 2 orders of magnitude for the resulting superhydrophobic surface in comparison with the untreated zinc surface and this should be ascribed to the contribution of Au–Zn alloys on the surface.