Zhi-Hong Liu

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Name: 刘志洪; ZhiHong Liu
Organization: Wuhan University , China
Department: College of Chemistry and Molecular Sciences
Title: Professor(PhD)

TOPICS

Co-reporter:Yu Li;Lingyu Zeng;Cheng Zhong;Xiaohu Dong;Zhiqiang Mao;Zhihong Liu;Songwei Lv;Zhengguo Zhang;Jingui Qin
Advanced Optical Materials 2017 Volume 5(Issue 2) pp:
Publication Date(Web):2017/01/01
DOI:10.1002/adom.201600696
The designed two-photon dye with a β-diketone moiety can undergo a keto-enol equilibrium and thus impart ultrahigh polarity sensitivity. The enol form, as the main component in aprotic environments with a long conjugated chain, displays much stronger two-photon fluorescence, while the keto form in protic environments with negligible fluorescence shows good water-solubility and cell membrane permeability.
Co-reporter:Zhiqiang Mao;Hong Jiang;Zhen Li;Cheng Zhong;Wei Zhang;Zhihong Liu
Chemical Science (2010-Present) 2017 vol. 8(Issue 6) pp:4533-4538
Publication Date(Web):2017/05/30
DOI:10.1039/C7SC00416H
In situ fluorescence imaging of nitric oxide (NO) is a powerful tool for studying the critical roles of NO in biological events. However, the selective imaging of NO is still a challenge because most currently available fluorescent probes rely on the o-phenylenediamine (OPD) recognition site, which reacts with both NO and some abundant reactive carbonyl species (RCS) (such as dehydroascorbic acid and methylglyoxal) and some reactive oxygen/nitrogen species (ROS/RNS). To address this problem, a new fluorescent probe, NCNO, based on the N-nitrosation of aromatic secondary amine was designed to bypass the RCS, ROS, and RNS interference. As was expected, the probe NCNO could recognize NO with pronounced selectivity and sensitivity among ROS, RNS, and RCS. The probe was validated by detecting NO in live cells and deep tissues owing to its two-photon excitation and red-light emission. It was, hence, applied to monitor NO in ischemia reperfusion injury (IRI) in mice kidneys by two-photon microscopy for the first time, and the results vividly revealed the profile of NO generation in situ during the renal IRI process.
Co-reporter:Wenqi Feng, Zhiqiang Mao, Lingzhi Liu, Zhihong Liu
Talanta 2017 Volume 167() pp:134-142
Publication Date(Web):15 May 2017
DOI:10.1016/j.talanta.2017.02.012
•A novel two-photon fluorescent probe for hydrogen sulfide was developed for cell imaging.•The probe can offer ratiometric fluorescence signal under one-photon or two-photon excitation.•Morpholine group was employed to provide lysosome targeting ability.•The probe could detect endogenous and exogenous H2S in lysosomes of living cells with high sensitivity and selectivity.Hydrogen sulfide (H2S) is a kind of gaseous signalling molecule that plays pivotal role in various biological processes. So far, it is still a challenge to develop convenient and reliable methods for H2S detection in lysosomes. Herein, we developed a novel ratiometric two-photon fluorescent probe LR-H2S for imaging H2S in lysosomes. Upon the addition of H2S (using Na2S as a donor) to LR-H2S in buffer solution, the azide group is reduced to amino group and subsequently the carbamate ester is cleaved by 1,6-elimination, resulting in a fluorescence emission increase at 541 nm and a concomitant emission decrease at 475 nm. Under two-photon excitation of 840 nm, an 80-fold fluorescence ratio (F541/F475) enhancement was observed with a wide linear range of 25–2500 μM. The detection limit was calculated to be 0.70 μM based on 3σ/k method, indicating that the probe can detect H2S with a high sensitivity. The probe also shows excellent selectivity toward H2S among other biological interference species and features with low cytotoxicity and favorable two-photon properties. Furthermore, LR-H2S can easily localize in lysosomes and vividly illuminate endogenous/exogenous H2S level and distribution in lysosomes of living SGC-7901 cells.A ratiometric fluorescent probe was constructed for imaging hydrogen sulfide in lysosomes by two-photon microscopy.
Co-reporter:Run-Qing Li, Zhi-Qiang Mao, Lei Rong, Nian Wu, Qi Lei, Jing-Yi Zhu, Lin Zhuang, Xian-Zheng Zhang, Zhi-Hong Liu
Biosensors and Bioelectronics 2017 Volume 87() pp:73-80
Publication Date(Web):15 January 2017
DOI:10.1016/j.bios.2016.08.008
•A simple and efficient two-photon excited fluorescent probe for the real-time detection and imaging of O2•− in living organisms.•Using probe to visualize endogenously generated superoxide anion in inflamed lung.•A potent and practical tool to study superoxide anion in various biological and pathological processes.Herein, we report a novel quinoline derivative-based two-photon fluorescent probe 6-(dimethylamino)quinoline-2-benzothiazoline (HQ), which is capable of tracking superoxide anion in organisms with specific “turn-on” fluorescence response based on extension of π-conjugations and moderate ICT process. The probe exhibited favorable photophysical properties, a broad linear range and high photostability. It can specifically detect superoxide anion with a significant fluorescence enhancement and great linearity from 0 to 500 μM in PBS buffer. Furthermore, HQ shows low cytotoxicity and excellent photostability toward living cells and organisms, which was able to monitor endogenous superoxide anion fluxes in living cells and in vivo. For the first time, endogenous superoxide anion in lung inflammation was visualized successfully by using HQ through two-photon microscopy, and the probe HQ shows great potential for fast in-situ detecting of inflammatory response in live organisms.
Co-reporter:Ping Jiang, Mengyuan He, Lin Shen, Anni Shi, Zhihong Liu
Sensors and Actuators B: Chemical 2017 Volume 239() pp:319-324
Publication Date(Web):February 2017
DOI:10.1016/j.snb.2016.08.005
•A novel paper-supported aptasensor based on luminescence resonance energy transfer from upconversion nanoparticles to carbon nanoparticles was developed.•Carbon nanoparticles were used as energy acceptor for paper-based LRET assays for the first time.•The method was applicable in serum samples for total IgE detection.•The results were well correlated to those obtained from chemiluminescence-based clinical assay.A paper-supported aptasensor was constructed for total IgE using a luminescence resonance energy transfer (LRET) protocol with upconversion nanoparticles (UCNPs) as energy donors and carbon nanoparticles (CNPs) as energy acceptors. This is the first time that zero-dimensional carbon nanoparticles were used as energy acceptors for paper-based LRET assays. The π-π stacking interaction between the aptamer and CNPs brought the energy donor (UCNPs) and energy acceptor (CNPs) in close proximity, induced the LRET process on the surface of paper and thus led to the luminescence quenching of UCNPs. The introduction of IgE inhibited the energy transfer and hence recovered the luminescence of UCNPs in a concentration-dependent manner, as a result of the recognition between IgE and aptamer. This aptasensor can be used to detect IgE concentration in the range of 0.5–80 ng/mL in both buffer solution and human serum samples. The IgE concentrations measured by our method were well correlated to those obtained from chemiluminescence-based clinical assay. Owing to its simplicity and accuracy, the proposed sensor thus showed the potential of clinical applications.
Co-reporter:Baoping Zhai;Wei Hu;Jinyu Sun;Siyu Chi;Yidi Lei;Fang Zhang;Cheng Zhong;Zhihong Liu
Analyst (1876-Present) 2017 vol. 142(Issue 9) pp:1545-1553
Publication Date(Web):2017/05/02
DOI:10.1039/C7AN00058H
A two-photon fluorescent probe FNTR for nitroreductase was synthesized by using 9,9-dimethyl-2-acetyl-fluoren-7-methylamino (1) as a two-photon fluorophore and a p-nitrobenzyl carbamate group as a recognition domain for nitroreductase (NTR). The probe and the fluorophore were tested under one- and two-photon modes respectively. After reacting with nitroreductase, FNTR had a 130-fold fluorescence enhancement at 563 nm in 10 min and the maximal two-photon action cross-section value was detected as 66 GM at 750 nm. The probe showed a high sensitivity with a detection limit as low as 23.67 ng ml−1, high selectivity, low cytotoxicity and good photostability. In the presence of reduced nicotinamide adenine dinucleotide (NADH), endogenous NTR was detected in living cells, tissues and zebrafish. Cobalt chloride was used to induce chemical hypoxia to produce NTR, which generated enhanced fluorescence in cells and tumor tissues. Finally, two-photon fluorescence imaging of NTR was achieved in zebrafish at a penetration depth of up to 200 μm.
Co-reporter:Zhiqiang Mao, Wenqi Feng, Zhen Li, Lingyu Zeng, Weijie Lv and Zhihong Liu  
Chemical Science 2016 vol. 7(Issue 8) pp:5230-5235
Publication Date(Web):26 Apr 2016
DOI:10.1039/C6SC01313A
As a pivotal signalling molecule involved in various physiological and pathological processes, nitric oxide (NO) has motivated increasing interest in the last few decades. Although a considerable number of fluorescent probes have been developed for NO imaging, the in situ tracking of this gas molecule in biological events remains a big challenge, mainly because of the relatively short excitation and/or emission wavelengths, which are subject to background interference and lowered collection efficiency in deep-tissue imaging. Herein, we report a far-red emissive (650 nm) two-photon (TP) excitable NRNO probe, using Nile Red as the TP fluorophore, for NO detection and imaging both in vitro and in vivo. The NRNO probe shows a fast (within 180 s) and specific fluorescence response toward NO with a limit of detection (LOD) as low as 46 nM. The excellent properties of NRNO enable it to sensitively detect both exogenously and endogenously generated NO in living cells. The “NIR in” and “far-red out” lights lead to improved penetrating ability, thus endowing the probe with high resolution for the illumination of deep tissues. It is therefore able to visualize the NO generation in a lipopolysaccharide (LPS)-mediated inflammation process for the first time. Our results demonstrate that NRNO could be a practical tool for studying the NO-related biological events. Moreover, this study also suggests the possibility of using Nile Red and its derivatives to develop far-red emissive TP probes, which is an important, yet undeveloped area.
Co-reporter:Xuefeng Li, Hao Ren, Zhijuan Zou, Jiaojiao Sun, Jingyu Wang and Zhihong Liu  
Chemical Communications 2016 vol. 52(Issue 3) pp:453-456
Publication Date(Web):06 Oct 2015
DOI:10.1039/C5CC07372C
Molecularly grafted carbon nitride (CN) nanosheets, matching well with the emission energy of upconversion phosphors (UCPs), were acquired for the first time. As a result of energy gap engineering, the assembled composites successfully realized the full use of visible-NIR light and afforded much higher activity than any CN- or UCP-based photocatalyst ever reported.
Co-reporter:Mengyuan He, Zhen Li, Yiying Ge, and Zhihong Liu
Analytical Chemistry 2016 Volume 88(Issue 3) pp:1530
Publication Date(Web):January 20, 2016
DOI:10.1021/acs.analchem.5b04863
We report the first portable upconversion nanoparticles (UCNPs)-based paper device for road-side field testing of cocaine. Upon the recognition of cocaine by two pieces of rationally designed aptamer fragments, the luminescence of UCNPs immobilized on the paper is quenched by Au nanoparticles (AuNPs), which indicates the cocaine concentration. This device can give quantitative results in a short time with high sensitivity using only a smartphone as the apparatus. Moreover, this device is applicable in human saliva samples, and it also can be used to monitor the cocaine content change in blood samples. The results of this work demonstrate the prospect of developing UCNPs-based paper devices for field testing of drug abuse.
Co-reporter:Tao Liang, Zhen Li, Dan Song, Lin Shen, Qinggeng Zhuang, and Zhihong Liu
Analytical Chemistry 2016 Volume 88(Issue 20) pp:9989
Publication Date(Web):September 15, 2016
DOI:10.1021/acs.analchem.6b01963
Upconversion nanoparticles (UCNPs) are attracting increasing attention in biosensing and imaging. The design of UCNP-based probes currently relies exclusively on the luminescence resonance energy transfer (LRET) principle. The prerequisite spectral overlap in LRET leads to limited flexibility in probe design, thus hindering the construction and application of upconversion (UC) probes. To change this situation, we herein present a new approach to construct UC probes by use of heavy metal ion-induced quenching. We reveal that heavy metal ions can quench the upconversion luminescence (UCL) to >95% without the occurrence of spectral overlap. A proof-of-concept UC probe for biothiols by manipulating Cu2+ as the switch of luminescence exhibits satisfying performance both in vitro and in bioimaging. This is the first report of a UC probe utilizing heavy metal ions to govern the read-out signal. The strategy is much simpler than the LRET principle and highly efficient, which provides a new way to design and apply UCNP-based probes.
Co-reporter:Zhen Li; Songwei Lv; Yali Wang; Shiyu Chen;Zhihong Liu
Journal of the American Chemical Society 2015 Volume 137(Issue 9) pp:3421-3427
Publication Date(Web):February 24, 2015
DOI:10.1021/jacs.5b01504
Upconversion nanoparticles (UCNPs) are promising energy donors for luminescence resonance energy transfer (LRET) and have widely been used to construct nanoprobes. To improve the LRET efficiency, which is currently a limiting factor for UCNPs-based bioassay, we herein propose a strategy to construct LRET-based nanoprobe using UCNPs with confined emitters and bared surface as the luminophore, with Ca2+ as the proof-of-concept target. The sandwich-structure upconversion nanoparticles (SWUCNPs) are designed with a core-inner shell-outer shell architecture, in which the emitting ions (Ln3+) are precisely located in the inner shell near the particle surface, which is close enough to external energy acceptors. The target receptor (Fluo-4) is directly tagged on bared surface of SWUCNPs, which further reduces the donor-to-acceptor distance. Our strategy contributes to significantly improved LRET efficiency and hence affords an ultrahigh sensitivity for Ca2+ detection. The as-constructed nanoprobe is structurally stable and exhibits good biocompatibility, which ensures uptake and reliable observation in living cells. The nanoprobe can be used for monitoring the different levels of cytosol [Ca2+] in living cells. Furthermore, it is applicable in Ca2+ imaging in mice liver tissues.
Co-reporter:Zhen Li; Tao Liang; Songwei Lv; Qinggeng Zhuang;Zhihong Liu
Journal of the American Chemical Society 2015 Volume 137(Issue 34) pp:11179-11185
Publication Date(Web):August 19, 2015
DOI:10.1021/jacs.5b06972
The detection of •OH in live organisms is crucial to the understanding of its physiological and pathological roles; while this is too challenging because of the extremely low concentration and high reactivity of the species in the body. Herein, we report the rational design and fabrication of an NIR-light excited luminescence resonance energy transfer-based nanoprobe, which for the first time realizes the in vivo detection of •OH. The nanoprobe is composed of two moieties: upconversion nanoparticles with sandwich structure and bared surface as the energy donor; and mOG, a modified azo dye with tunable light absorption, as both the energy acceptor and the •OH recognizing ligand. The as-constructed nanoprobe exhibited ultrahigh sensitivity (with the quantification limit down to 1.2 femtomolar, several orders of magnitude lower than that of most previous •OH probes), good biocompatibility, and specificity. It was successfully used for monitoring [•OH] levels in live cells and tissues.
Co-reporter:Lingyu Zeng, Shiyu Chen, Tian Xia, Wei Hu, Chunya Li, and Zhihong Liu
Analytical Chemistry 2015 Volume 87(Issue 5) pp:3004
Publication Date(Web):February 6, 2015
DOI:10.1021/acs.analchem.5b00172
Hydrogen persulfide and polysulfide (H2Sn) are newly discovered intracellular reactive species considered to have high protein S-sulfhydration efficiency. The detection of H2Sn in living systems is essential for studying their functions but is quite challenging. In this work, we report a two-photon excited fluorescent probe, QSn, capable of tracking H2Sn in living organisms. QSn exhibited turn-on two-photon fluorescence response upon reaction with H2Sn. With a favorable photophysical property, high specificity, and low cytotoxicity, QSn was able to recognize exogenous H2Sn in living cells. More importantly, it realized for the first time the visualization of endogenous H2Sn generated in cells overexpressing cystathionine β-synthase and cystathionine γ-lyase, the enzymes responsible for producing endogenous H2Sn. Taking advantage of two-photon microscopy, the probe was also applied to achieve H2Sn detection in zebrafish embryos and to observe H2Sn distribution in living organisms.
Co-reporter:Jin Chen, Lingyu Zeng, Tian Xia, Shuang Li, Tengfei Yan, Song Wu, Guofu Qiu, and Zhihong Liu
Analytical Chemistry 2015 Volume 87(Issue 16) pp:8052
Publication Date(Web):July 22, 2015
DOI:10.1021/acs.analchem.5b02032
Malondialdehyde (MDA) is a significant biomarker of oxidative stress. Variations of MDA level in biological systems often represent pathological changes that are related with many types of diseases. Although a variety of techniques have been developed for MDA detection, the probing of this biomarker in living cells remains unexplored. Herein, we report a turn-on fluorescent probe, MDAP-1, with a synergistic photoinduced electron transfer (PET)-hydrogen bonding mechanism, which for the first time realizes MDA sensing under physiological conditions with excellent sensitivity and specificity. The probe responds to MDA with a fluorescence enhancement factor (FEF) of up to >170-fold and a large Stokes shift (∼180 nm). Further biological evaluations show that MDAP-1 is able to detect both endogenous and exogenous MDA in living cells. It can be used to track the generation of MDA under oxidative stress, as stimulated by H2O2. We believe the results of this work will be helpful to the studies of MDA-related biological events and the elucidation of the underlying pathological mechanism in the future.
Co-reporter:Yaohua Li, Zhengjun Wu and Zhihong Liu  
Analyst 2015 vol. 140(Issue 12) pp:4083-4088
Publication Date(Web):07 Apr 2015
DOI:10.1039/C5AN00357A
We herein report a sensitive and selective immunosensor for carcinoembryonic antigen (CEA) based on the joint use of upconversion phosphors (UCPs) and magnetic beads (MBs). UCPs as the signal probe were designed with a core–shell structure which provided a 40-fold enhancement of the luminescence intensity. Poly(acrylic acid) (PAA)-modified UCPs were covalently conjugated with the anti-CEA antibody (coating), and streptavidin functionalized magnetic beads were combined with another biotin-tagged anti-CEA antibody. With the assistance of a magnet, the as-formed immune sandwich in the presence of CEA can be readily separated from the assay matrix. The immunosensor showed a linear dynamic range for CEA within 0.05–20 ng mL−1 in a buffered aqueous solution, and 0.1–20 ng mL−1 in a human serum sample. The sensor was highly specific to CEA. Our results have suggested the potential application of the UCP-MB based immunoassay for CEA in clinical analysis.
Co-reporter:Yan Xiao;Lingyu Zeng;Tian Xia;Zhengjun Wu;Dr. Zhihong Liu
Angewandte Chemie 2015 Volume 127( Issue 18) pp:5413-5417
Publication Date(Web):
DOI:10.1002/ange.201500008

Abstract

Herein we report that few-atom silver nanoclusters (Ag NCs) can be effective energy acceptors for upconversion phosphors (UCPs). A luminescence resonance energy transfer (LRET) probe for biothiols was constructed by decorating UCPs with dithiol-stabilized Ag NCs. Owing to the unique properties of ultrasmall NCs, properties which bridge the gap between those of small molecules and those of nanoparticles, the use of approximately 1.9 nm Ag NCs as energy acceptors endows the probe with high energy-transfer efficiency, good biocompatibility, and flexibility. The UCP–Ag NC nanoprobe enables rapid and robust target assay in solutions. It was also uploaded into living cells and used to detect intracellular biothiol levels with high discrimination. Moreover, the probe shows transportability in vivo and can be used for tissue imaging. The facile growth of few-atom metal NCs on diverse templates may enable the development of various nanoprobes combining UCPs and metal NCs.

Co-reporter:Yan Xiao;Lingyu Zeng;Tian Xia;Zhengjun Wu;Dr. Zhihong Liu
Angewandte Chemie International Edition 2015 Volume 54( Issue 18) pp:5323-5327
Publication Date(Web):
DOI:10.1002/anie.201500008

Abstract

Herein we report that few-atom silver nanoclusters (Ag NCs) can be effective energy acceptors for upconversion phosphors (UCPs). A luminescence resonance energy transfer (LRET) probe for biothiols was constructed by decorating UCPs with dithiol-stabilized Ag NCs. Owing to the unique properties of ultrasmall NCs, properties which bridge the gap between those of small molecules and those of nanoparticles, the use of approximately 1.9 nm Ag NCs as energy acceptors endows the probe with high energy-transfer efficiency, good biocompatibility, and flexibility. The UCP–Ag NC nanoprobe enables rapid and robust target assay in solutions. It was also uploaded into living cells and used to detect intracellular biothiol levels with high discrimination. Moreover, the probe shows transportability in vivo and can be used for tissue imaging. The facile growth of few-atom metal NCs on diverse templates may enable the development of various nanoprobes combining UCPs and metal NCs.

Co-reporter:Hui Li;De-en Sun ; Zhihong Liu
Chemistry - A European Journal 2015 Volume 21( Issue 13) pp:4944-4948
Publication Date(Web):
DOI:10.1002/chem.201406633

Abstract

An ultrasensitive biosensing platform for DNA and protein detection is constructed based on the luminescence quenching ability of plasmonic palladium nanoparticles (PdNPs). By growing the particles into large sizes (ca. 30 nm), the plasmonic light absorption of PdNPs is broadened and extended to the visible range with extinction coefficients as high as 109 L mol−1 cm−1, enabling complete quenching of fluorescent dyes that emit at diverse ranges and that are tagged to bioprobes. Meanwhile the nonspecific quenching of the dyes (not bound to probes) is negligible, leading to extremely low background signal. Utilizing the affinity of PdNPs towards bioprobes, such as single-stranded (ss) DNA and polypeptide molecules, which is mainly assigned to the coordination interaction, nucleic acid assays with a quantification limit of 3 pM target DNA and protein assay are achieved with a simple mix-and-detect strategy based on the luminescence quenching-and-recovery protocol. This is the first demonstration of biosensing employing plasmonic absorption of nanopalladium, which offers pronounced sensing performances and can be reasonably expected for wide applications.

Co-reporter:Tengfei Yan, Jin Chen, Song Wu, Zhiqiang Mao, and Zhihong Liu
Organic Letters 2014 Volume 16(Issue 12) pp:3296-3299
Publication Date(Web):June 12, 2014
DOI:10.1021/ol5012949
A fluorescence chemsensor for carbon monoxide (CO), based on transformation of weakly fluorescent iodide to strong fluorescent amino product upon reacting with CO, shows abilities of quantitative measurement of CO in air at a level of 50–1000 ppm and real-time and on-site monitoring for CO flammation/explosion.
Co-reporter:Lingyu Zeng, Shiyu Chen, Tian Xia, Cheng Zhong and Zhihong Liu  
Chemical Communications 2014 vol. 50(Issue 76) pp:11139-11142
Publication Date(Web):30 Jul 2014
DOI:10.1039/C4CC05010J
We have reported a new strategy to design two-photon (2P) fluorescent probes for simultaneous elevation of the 2P absorption cross-section (δ) and quantum yield (ϕ). The target-induced hydrogen bond-chelated ring enhances molecular planarity, leading to the enhancement of δ; meanwhile, the photo-induced electron transfer (PET) “on–off” process modulates ϕ.
Co-reporter:Yan Xiao, Zhengjun Wu, Kwok-Yin Wong and Zhihong Liu  
Chemical Communications 2014 vol. 50(Issue 37) pp:4849-4852
Publication Date(Web):25 Mar 2014
DOI:10.1039/C4CC01154F
Novel hairpin DNA probes are designed and constructed based on target-induced in situ generation of luminescent silver nanoclusters. This design allows specific and versatile detection of diverse targets with easy operation and low cost.
Co-reporter:Yunxia Yuan, Shufang Wu, Fan Shu and Zhihong Liu  
Chemical Communications 2014 vol. 50(Issue 9) pp:1095-1097
Publication Date(Web):20 Nov 2013
DOI:10.1039/C3CC47755J
An ultrathin MnO2 nanosheet is established as a label-free two-dimensional nanoplatform for homogeneous biosensing. Two biosensors based on an MnO2 nanosheet with favourable performances are constructed for OTA and Cat D using different probes and following different sensing principles.
Co-reporter:Xiaohu Dong, Cheol Ho Heo, Shiyu Chen, Hwan Myung Kim, and Zhihong Liu
Analytical Chemistry 2014 Volume 86(Issue 1) pp:308
Publication Date(Web):December 16, 2013
DOI:10.1021/ac403226h
A two-photon fluorescent probe (QNO) for nitric oxide is reported. The probe is designed with a photoinduced electron transfer (PeT) mechanism and shows 12-fold fluorescence enhancement toward NO. Adopting a quinoline derivative as the fluorophore, QNO has a large two-photon action cross section value of 52 GM and long-wavelength emission. It also features high selectivity, low cytotoxicity, and pH insensitivity. By utilizing two-photon microscopy (TPM), QNO can detect NO in live cells and live tissues at a depth of 90–180 μm.
Co-reporter:Yunxia Yuan, Runqing Li, and Zhihong Liu
Analytical Chemistry 2014 Volume 86(Issue 7) pp:3610
Publication Date(Web):March 10, 2014
DOI:10.1021/ac5002096
Layered WS2 nanosheet is a kind of two-dimensional (2D) covalent-network solid material with remarkable structural and electronic properties that has attracted increasing interest in recent years. In this work, we propose a one-step sonication-assisted exfoliation method to prepare water-soluble WS2 nanosheet and demonstrate its application as a biosensing platform. The synthesis route is simple and straightforward. We reveal that single-strand DNA (ssDNA) chains can readily be adsorbed on the nanosheet, leading to complete and fast quenching of a fluorescent dye tagged to the DNA chain. The adsorbed ssDNA is detachable from the nanosheet upon the interaction with other biomolecules, resulting in the restoration of the fluorescence. The 2D WS2 nanosheet thus acts as an efficient platform for assembling of bioprobes. Because of the extraordinarily high quenching efficiency, which is the synergic result of both excited-state energy transfer and static quenching, the WS2 platform affords minimal background and high sensitivity. Our attempt will extend the application of this material to biosensing and probing areas.
Co-reporter:Zhiqiang Mao, Liang Hu, Xiaohu Dong, Cheng Zhong, Bi-Feng Liu, and Zhihong Liu
Analytical Chemistry 2014 Volume 86(Issue 13) pp:6548
Publication Date(Web):May 30, 2014
DOI:10.1021/ac501947v
Zn2+ plays vital roles in regulating physiological and pathological processes. A number of diseases are associated with the disruption of intracellular free Zn2+ homeostasis, and the relationship is still uncovered. Thus, it is important to monitor intracellular free Zn2+ ions in real time, which is still challenging due to the low content of intracellular free Zn2+. In this work, we report on the design and synthesis of a new two-photon (2P) fluorescent probe, QZn, based on quinoline derivative for intracellular free Zn2+. Theoretical calculations were carried out to rationalize the design. The probe displayed a moderate 2P action cross section value of 51 GM at 820 nm and up to 10-fold fluorescence enhancement upon Zn2+ binding. The detection limit of Zn2+ was 15.1 pM, which presented a pronounced sensitivity toward Zn2+ and indicated that QZn would be competent for detecting the low-content intracellular Zn2+. By using two-photon microscopy, QZn was capable of monitoring the fluctuation of intracellular free zinc ions in real time.
Co-reporter:Liya Hu, Jingyu Wang, Jianxiong Zhang, Qiuyan Zhang and Zhihong Liu  
RSC Advances 2014 vol. 4(Issue 1) pp:420-427
Publication Date(Web):06 Nov 2013
DOI:10.1039/C3RA44421J
Colloidal N-doped TiO2 nanocrystals are successfully synthesized by low-temperature direct nitridization in triethylamine solution during hydrolysis of tetrabutyl titanate, followed by acidic peptization at 70 °C. Through adjusting the acid concentration and peptization time, the N-doped samples consisting of different proportions of anatase and rutile phases are obtained. Several characterization techniques including X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and UV-vis diffuse reflectance spectroscopy are employed to determine the crystal phase, morphology, degree of nitrogen incorporation and optical properties of the products. The high resolution XPS spectrum of the N 1s region confirms the substitutional nitrogen doping of lattice oxygen in TiO2 crystals. For comparison, it is found that most of the N species are chemisorbed on the surface of TiO2 particles if the N-source is introduced after crystallization. The light response in the range of 400–500 nm is obviously improved by N doping, which facilitates the absorption of photons to produce e−–h+ pairs under visible irradiation. On the other hand, nitrogen doping also inhibits the recombination of the photoinduced carriers and therefore increases the quantum efficiency of the TiO2 photocatalyst. As a result, the as-synthesized N-doped TiO2 nanomaterials exhibit higher photocatalytic activity both in the UV- and visible-light region in contrast to the non-doped TiO2. The hybrid containing 63.1% anatase shows the highest photocatalytic activity, which is due to a synergistic effect between anatase and rutile.
Co-reporter:Hui Li, De-en Sun, Yajie Liu, Zhihong Liu
Biosensors and Bioelectronics 2014 Volume 55() pp:149-156
Publication Date(Web):15 May 2014
DOI:10.1016/j.bios.2013.11.079
•An aptasensor is constructed to detect kanamycin based on upconversion fluorescence resonance energy transfer.•The conformation change of kanamycin aptamer into a hairpin structure after interacting with the target is accompanied by the alteration of energy-transfer efficiency.•The aptasensor for kanamycin detection is ultrasensitive.•The aptasensor is robust in human serum samples indicating its prospect of practical applications.We developed an ultrasensitive fluorescence resonance energy transfer (FRET) aptasensor for kanamycin detection, using upconversion nanoparticles (UCNPs) as the energy donor and graphene as the energy acceptor. Oleic acid modified upconversion nanoparticles were synthesized through a hydrothermal process followed by a ligand exchange with hexanedioic acid. The kanamycin aptamer (5'-NH2-AGATGGGGGTTGAGGCTAAGCCGA-3') was tagged to UCNPs through an EDC–NHS protocol. The π–π stacking interaction between the aptamer and graphene brought UCNPs and graphene in close proximity and hence initiated the FRET process resulting in quenching of UCNPs fluorescence. The addition of kanamycin to the UCNPs–aptamer–graphene complex caused the fluorescence recovery because of the blocking of the energy transfer, which was induced by the conformation change of aptamer into a hairpin structure. A linear calibration was obtained between the fluorescence intensity and the logarithm of kanamycin concentration in the range from 0.01 nM to 3 nM in aqueous buffer solution, with a detection limit of 9 pM. The aptasensor was also applicable in diluted human serum sample with a linear range from 0.03 nM to 3 nM and a detection limit of 18 pM. The aptasensor showed good specificity towards kanamycin without being disturbed by other antibiotics. The ultrahigh sensitivity and pronounced robustness in complicated sample matrix suggested promising prospect of the aptasensor in practical applications.
Co-reporter:Zhen Li, Mengyuan He, Dangdang Xu, Zhihong Liu
Journal of Photochemistry and Photobiology C: Photochemistry Reviews 2014 Volume 18() pp:1-17
Publication Date(Web):March 2014
DOI:10.1016/j.jphotochemrev.2013.10.002
Co-reporter:Yuhui Wang, Zhengjun Wu, and Zhihong Liu
Analytical Chemistry 2013 Volume 85(Issue 1) pp:258
Publication Date(Web):November 27, 2012
DOI:10.1021/ac302659b
We report a new upconversion fluorescence resonance energy transfer (UC-FRET) biosensor using poly-m-phenylenediamine (PMPD) nanospheres as the energy acceptor in this paper. A single-stranded DNA (ssDNA) tagged with a sulfydryl group at the 5′-terminus was covalently linked to poly(ethylenimine) (PEI) functionalized upconversion phosphors (UCPs, the energy donor). Because of the π-rich electronic structure of PMPD, self-assembly of the donor and the acceptor was achieved through the π–π stacking interaction between ssDNA and PMPD. The fluorescence of the donor was quenched by the acceptor in a PMPD-concentration-dependent manner. A maximum quenching degree of 90% was acquired, which was among the highest levels of all previous reports. Upon the formation of double-stranded DNA (dsDNA) between the target DNA and the probe DNA, the energy acceptor was separated from the donor due to the weakened interaction between dsDNA and PMPD. The fluorescence of UCPs was accordingly restored, and a linear response was obtained with the target concentration ranging from 0.1 to 6.0 nM. The limit of detection was calculated as 0.036 nM, which was a highly competitive sensitivity. The sensor also showed high precision, pronounced specificity, and the applicability to complicated sample matrix (human serum). The UCPs–PMPD FRET sensing platform takes advantages of both the optical merits of the upconversion donors and the superquenching ability and good water-solubility of the aromatic polymer nanoparticles. This study will open the opportunity to develop a new class of UC-FRET biosensors.
Co-reporter:Yan Xiao, Fan Shu, Kwok-Yin Wong, and Zhihong Liu
Analytical Chemistry 2013 Volume 85(Issue 18) pp:8493
Publication Date(Web):August 28, 2013
DOI:10.1021/ac402125g
We studied the energy transfer (ET) property of ultrasmall Ag nanoclusters (Ag NCs) and exploited its biosensing application for the first time. A hybridized DNA duplex model was designed to study the energy transfer process from fluorescent energy donors to Ag NCs. By changing the DNA duplex model and the number of hybridized pairs, the separation distance between the energy donor and Ag NCs was adjusted to investigate the distance dependence and possible mechanisms involved in the ET process, which was assigned to Förster resonance energy transfer (FRET). Using Ag NCs with different photophysical properties as energy acceptors, FRET-based biosensing platforms with two different energy donors were constructed utilizing either the off–on or ratiometric fluorescence signaling. This study will provide the basis for understanding energy transfer properties of Ag NCs and bring to light the universal application of these properties in bio/chemo sensing.
Co-reporter:Mengyuan He and Zhihong Liu
Analytical Chemistry 2013 Volume 85(Issue 24) pp:11691
Publication Date(Web):December 3, 2013
DOI:10.1021/ac403693g
A paper-based microfluidic device with upconversion fluorescence assay (named as UC-μPAD) is proposed. The device is fabricated on a normal office printing sheet with a simple plotting method. Upconversion phosphors (UCPs) tagged with specific probes are spotted to the test zones on the μPAD, followed by the introduction of assay targets. Upconversion fluorescence measurements are directly conducted on the test zones after the completion of the probe-to-target reactions, without any post-treatments. The UC-μPAD features very easy fabrication and operation, simple and fast detection, low cost, and high sensitivity. UC-μPAD is a promising prospect for a clinical point-of-care test.
Co-reporter:Yu Li, Xiaohu Dong, Cheng Zhong, Zhihong Liu, Jingui Qin
Sensors and Actuators B: Chemical 2013 Volume 183() pp:124-128
Publication Date(Web):5 July 2013
DOI:10.1016/j.snb.2013.03.112
A new water-soluble two-photon probe CuL2 for pyrophosphate anion (PPi) is designed and synthesized, and shows turn-on fluorescence with high sensitivity and selectivity. The probe CuL2 can selectively detect small amount of PPi particularly in the presence of a large excess of PO43− and ATP. The association constant of CuL2 and PPi is about 105.2, and its detection limit is 3.2 × 10−8 M. To the best of our knowledge, this is the first water-soluble two-photon fluorescent turn-on probe for PPi.
Co-reporter:Lingyu Zeng;Yunxia Yuan;Pei Shen; Kwok-Yin Wong; Zhihong Liu
Chemistry - A European Journal 2013 Volume 19( Issue 25) pp:8063-8067
Publication Date(Web):
DOI:10.1002/chem.201300332
Co-reporter:Yunxia Yuan and Zhihong Liu  
Chemical Communications 2012 vol. 48(Issue 60) pp:7510-7512
Publication Date(Web):29 May 2012
DOI:10.1039/C2CC33289B
The energy transfer efficiency from up-converting donors was significantly enhanced by constructing beacon sensors, which led to increased sensitivities in DNA recognition and protein determination.
Co-reporter:Yuhui Wang, Pei Shen, Chunya Li, Yanying Wang, and Zhihong Liu
Analytical Chemistry 2012 Volume 84(Issue 3) pp:1466
Publication Date(Web):January 10, 2012
DOI:10.1021/ac202627b
Matrix metalloproteinase-2 (MMP-2) is a very important biomarker in blood. Presently, sensitive and selective determination of MMP-2 directly in blood samples is still a challenging job because of the high complexity of the sample matrix. In this work, we reported a new homogeneous biosensor for MMP-2 based on fluorescence resonance energy transfer (FRET) from upconversion phosphors (UCPs) to carbon nanoparticles (CNPs). A polypeptide chain (NH2-GHHYYGPLGVRGC-COOH) comprising both the specific MMP-2 substrate domain (PLGVR) and a π-rich motif (HHYY) was designed and linked to the surface of UCPs at the C terminus. The FRET process was initiated by the π–π interaction between the peptide and CNPs, which thus quenched the fluorescence of the donor. Upon the cleavage of the substrate by the protease at the amide bond between Gly and Val, the donor was separated from the acceptor while the π-rich motif stayed on the acceptor. As a result, the fluorescence of the donor was restored. The fluorescence recovery was found to be proportional to the concentration of MMP-2 within the range from 10–500 pg/mL in an aqueous solution. The quantification limit of this sensor was at least 1 order of magnitude lower than that of other reported assays for MMP-2. The sensor was used to determine the MMP-2 level directly in human plasma and whole blood samples with satisfactory results obtained. Owing to the hypersensitivity of the method, clinical samples of only less than 1 μL were needed for accurate quantification, which can be meaningful in MMP-2-related clinical and bioanalytical applications.
Co-reporter:Xiaohu Dong, Ji Hee Han, Cheol Ho Heo, Hwan Myung Kim, Zhihong Liu, and Bong Rae Cho
Analytical Chemistry 2012 Volume 84(Issue 19) pp:8110
Publication Date(Web):September 11, 2012
DOI:10.1021/ac302210v
We report two-photon probes (FMg1 and FMg2) that can selectively detect intracellular free Mg2+ ([Mg2+]i) in live cells and tissues by two-photon microscopy. Combined with BCaM, a two-photon probe for near-membrane Ca2+ ([Ca2+]m), FMg2 allows dual-color imaging of Mg2+/Ca2+ activities in live cells and [Mg2+]i /[Ca2+]m distributions in live tissues at a depth of 100–200 μm.
Co-reporter:Yongyou Liu, Xiaohu Dong, Jian Sun, Cheng Zhong, Boheng Li, Ximeng You, Bifeng Liu and Zhihong Liu  
Analyst 2012 vol. 137(Issue 8) pp:1837-1845
Publication Date(Web):08 Feb 2012
DOI:10.1039/C2AN16254G
A novel two-photon excited fluorescent probe for cadmium (named as TPCd) was designed and synthesized utilizing a prodan (6-acetyl-2-methoxynaphthalene) derivative as the two-photon fluorophore and an o-phenylenediamine derivative as the Cd2+ chelator, which possessed favorable photophysical properties and good water-solubility. The probe was designed with a photoinduced electron transfer (PET) mechanism and thus was weakly fluorescent itself. After binding with Cd2+ which blocked the PET process, the fluorescence intensity of the probe was enhanced by up to 15-fold under one-photon excitation (OPE) and 27-fold under two-photon excitation (TPE), respectively. The two-photon action cross-section (Φδ) of the TPCd–Cd complex at 740 nm reached 109 GM compared to 3.6 GM for free TPCd, indicating the promising prospect of the probe in two-photon application. TPCd chelated Cd2+ with 1:1 stoichiometry, and the apparent dissociation constant (Kd) was 6.1 × 10−5 M for the one-photon mode and 7.2 × 10−5 M for the two-photon mode. The probe responded to Cd2+ over a wide linear range from 0.1 to 30 μM with a detection limit of 0.04 μM. High selectivity of the probe towards Cd2+ was acquired in Tris-HCl/sodium phosphate buffer. The probe was pH-independent in the biologically relevant pH range and non-toxic to living cells at reasonable concentration levels, warranting its in vivo applications. Through two-photon microscopy imaging, the probe was successfully applied to detect Cd2+ uptake in living HepG2 cells.
Co-reporter:Lingzhi Liu, Hui Li, Ting Qiu, Guohua Zhou, Kwok-Yin Wong, Zhike He and Zhihong Liu  
Chemical Communications 2011 vol. 47(Issue 9) pp:2622-2624
Publication Date(Web):13 Jan 2011
DOI:10.1039/C0CC04712K
A new molecular beacon (MB) driven by two-photon excitation (TPE) using quantum dots as energy donor is constructed, which provides reduced direct excitation of acceptor and is free of interferences from autofluorescence or scattering light in a complicated biological matrix.
Co-reporter:Yuhui Wang, Lei Bao, Zhihong Liu, and Dai-Wen Pang
Analytical Chemistry 2011 Volume 83(Issue 21) pp:8130
Publication Date(Web):September 16, 2011
DOI:10.1021/ac201631b
We presented a new aptamer biosensor for thrombin in this work, which was based on fluorescence resonance energy transfer (FRET) from upconverting phosphors (UCPs) to carbon nanoparticles (CNPs). The poly(acrylic acid) (PAA) functionalized UCPs were covalently tagged with a thrombin aptamer (5′-NH2- GGTTGGTGTGGTTGG-3′), which bound to the surface of CNPs through π–π stacking interaction. As a result, the energy donor and acceptor were taken into close proximity, leading to the quenching of fluorescence of UCPs. A maximum fluorescence quenching rate of 89% was acquired under optimized conditions. In the presence of thrombin, which induced the aptamer to form quadruplex structure, the π–π interaction was weakened, and thus, the acceptor was separated from the donor blocking the FRET process. The fluorescence of UCPs was therefore restored in a thrombin concentration-dependent manner, which built the foundation of thrombin quantification. The sensor provided a linear range from 0.5 to 20 nM for thrombin with a detection limit of 0.18 nM in an aqueous buffer. The same linear range was obtained in spiked human serum samples with a slightly higher detection limit (0.25 nM), demonstrating high robustness of the sensor in a complex biological sample matrix. As a practical application, the sensor was used to monitor thrombin level in human plasma with satisfactory results obtained. This is the first time that UCPs and CNPs were employed as a donor–acceptor pair to construct FRET-based biosensors, which utilized both the photophysical merits of UCPs and the superquenching ability of CNPs and thus afforded favorable analytical performances. This work also opened the opportunity to develop biosensors for other targets using this UCPs-CNPs system.
Co-reporter:Lingzhi Liu, Xiaohu Dong, Yan Xiao, Wenlong Lian and Zhihong Liu  
Analyst 2011 vol. 136(Issue 10) pp:2139-2145
Publication Date(Web):18 Mar 2011
DOI:10.1039/C0AN00933D
In the present work, a two-photon excited fluorescent chemosensor for Cu2+ was prepared. The probe was constructed on the basis of internal charge transfer (ICT) principle with macrocyclic dioxotetraamine as the Cu2+ receptor. The good water-solubility of the molecule enabled recognition and assay of Cu2+ ions in biological media. The photophysical properties of the chemosensor were investigated in detail, exhibiting favorable fluorescence quantum yield and moderate two-photon absorption cross-section. The studies on binding thermodynamics demonstrated the formation of 1:1 complex between the chemosensor and Cu2+ and an association constant of ca. 1.04 × 105 M−1. Due to the rational design of the molecular structure, the sensor was highly specific to Cu2+, which ensured high selectivity in Cu2+ determination. Upon Cu2+ binding, the intramolecular charge-transfer extent within the chromophore was weakened resulting in a remarkable quenching of fluorescence, based on which quantitative determination of Cu2+ was performed. Good linearity was obtained between the fluorescence quenching value and Cu2+ concentration ranging from 0.04 to 2.0 μM in aqueous solution. Benefiting from the merits of two-photon excitation, the chemosensor was free of interference from background luminescence in serum. A homogeneous quantitative determination of Cu2+ was achieved in the serum medium with a linear range of 0.04 to 2.0 μM. Considering the structural flexibility of the sensor, this work also opens up the possibility to construct other two-photon excited chemosensors for direct homogeneous assay of various molecules/ions in complicated biological sample matrices.
Co-reporter:Yuhui Wang, Ruxiu Cai and Zhihong Liu  
CrystEngComm 2011 vol. 13(Issue 6) pp:1772-1774
Publication Date(Web):21 Jan 2011
DOI:10.1039/C0CE00708K
Controlled synthesis of NaYF4: Yb, Er nanocrystals with upconversion fluorescence is achieved in aqueous solution by adjusting solvent composition (ethanol-to-water volume ratio) and F−/Ln3+molar ratio via a facile hydrothermal method.
Co-reporter:Li Qu, Xiaohu Dong, Cheng Zhong, Zhihong Liu, Jingui Qin
Chemical Physics Letters 2011 Volume 513(1–3) pp:103-107
Publication Date(Web):6 September 2011
DOI:10.1016/j.cplett.2011.07.081

Abstract

Two new arylalkyne ligands L1 (D–π–D′ type) and L2 (D–π–A type), and their coordinated Platinum(II) diimine diacetylides 1 (D–π–D′–π–[Pt]–π–D′–π–D type) and 2 (D–π–A–π–[Pt]–π–A–π–D type) were designed and synthesized (where D represents electron donating group and A represents electron accepting group). Photophysical properties measurements indicated that 2 displayed orange-red fluorescence with relatively high fluorescence quantum yield and strong two-photon absorption (2PA) cross-section. The influence of metal on the electronic structure and property was investigated by theoretical calculations and cyclic voltammograms.

Co-reporter:Jianhong Peng, Yuhui Wang, Jialan Wang, Xin Zhou, Zhihong Liu
Biosensors and Bioelectronics 2011 Volume 28(Issue 1) pp:414-420
Publication Date(Web):15 October 2011
DOI:10.1016/j.bios.2011.07.057
In this work, a new glucose sensor based on up-converting fluorescence resonance energy transfer (UC-FRET) was developed. Up-converting phosphors (UCPs, NaYF4: Yb, Er), which were covalently labeled with Concanavalin A (ConA), were used as the energy donor with thiolated β-cyclodextrins (SH-β-CDs) functionalized gold nanoparticles as the energy acceptor. Due to the combination between ConA and SH-β-CDs, the energy donor and the acceptor were brought to close proximity, resulting in the quenching of the fluorescence of UCPs by gold nanoparticles. In the presence of glucose which competed with SH-β-CDs towards the binding sites of ConA, the biosensor (UCPs–ConA–SH-β-CDs-Au) was decomposed and the energy donor was separated from the acceptor. Therefore, the fluorescence of UCPs was restored dependent on the concentration of glucose. The increase of UCPs fluorescence intensity was proportional to glucose concentration within the range from 0.4 μM to 10 μM in aqueous buffer, with a limit of detection (LOD) of 0.043 μM. A same linear range of glucose concentration was obtained in a human serum matrix (which was pretreated and thus contained no glucose) with a slightly higher LOD (0.065 μM). The glucose sensor was applied to real human serum samples with the results consistent with that of a classic hexokinase (HK) method, indicating that the UC-FRET biosensor was competent for directly sensing glucose in serum samples without optical interference, which benefited from the near infrared (NIR) excitation nature of UCPs. The results of this work suggested that the UC-FRET technique could be a promising alternative for detecting biomolecules in complex biological sample matrixes for diagnostic purposes.
Co-reporter:Cuiling Zhang;Yunxia Yuan;Shiming Zhang;Yuhui Wang ; Zhihong Liu
Angewandte Chemie International Edition 2011 Volume 50( Issue 30) pp:6851-6854
Publication Date(Web):
DOI:10.1002/anie.201100769
Co-reporter:Cuiling Zhang;Yunxia Yuan;Shiming Zhang;Yuhui Wang ; Zhihong Liu
Angewandte Chemie 2011 Volume 123( Issue 30) pp:6983-6986
Publication Date(Web):
DOI:10.1002/ange.201100769
Co-reporter:Lingzhi Liu, Xiaohu Dong, Wenlong Lian, Xiaoniu Peng, Zhihong Liu, Zhike He and Ququan Wang
Analytical Chemistry 2010 Volume 82(Issue 4) pp:1381
Publication Date(Web):January 15, 2010
DOI:10.1021/ac902467w
Recently, we have successfully developed a two-photon excitation fluorescence resonance energy transfer (TPE-FRET)-based homogeneous immunoassay using two-photon excitable small organic molecule as the energy donor. In the present work, the newly emerging TPE-FRET technique was extended to the determination of oligonucleotide. A new TPE molecule with favorable two-photon action cross section was synthesized [2-(2,5-bis(4-(dimethylamino)styryl)-1H-pyrrol-1-yl)acetic acid, abbreviated as TP-COOH], with the tagged reactive carboxyl group allowing facile conjugation with streptavidin (SA). Employing the TP-COOH molecule as energy donor and black hole quencher 1 (BHQ-1) as acceptor, a TPE-FRET-based homogeneous competitive hybridization model was constructed via a biotin−streptavidin bridge. Through the hybridization between a biotinylated single-stranded DNA (ssDNA) and a BHQ-1-linked ssDNA, and the subsequent capture of the as-formed hybrid by TP-COOH labeled SA, the donor fluorescence was quenched due to the FRET between TP-COOH and BHQ-1. Upon the competition between a target ssDNA and the quencher-linked ssDNA toward the biotinylated oligonucleotide, the donor fluorescence was recovered in a target-dependent manner. Good linearity was obtained with the target oligonucleotide ranging from 0.08 to 1.52 μM. The method was applied to spiked serum and urine samples with satisfying recoveries obtained. The results of this work verified the applicability of TPE-FRET technique in hybridization assay and confirmed the advantages of TPE-FRET in complicated matrix.
Co-reporter:Jingyu Wang, Xijiang Han, Cheng Liu, Wei Zhang, Ruxiu Cai and Zhihong Liu
Crystal Growth & Design 2010 Volume 10(Issue 5) pp:2185
Publication Date(Web):February 18, 2010
DOI:10.1021/cg901429u
The successful adjustment of phase composition and morphology of anatase/rutile TiO2 nanocomposites is achieved via a soft chemical strategy, which involves no templates, hydrothermal treatments, or calcinations. The process consists of a NaOH treatment of the hydrolysate of titanium tetra-n-butoxide and a subsequent acidic peptization of the H-titanate intermediate. The effects of the acid peptization time, acid volume, and the NaOH-treatment time on the properties of products are systematically investigated. For the first time, the two-way phase transition between anatase and rutile is realized through adjusting the acid peptization time, which provides a promising way to control the phase ratio in preparing TiO2 anatase/rutile composites. The mechanism of the phase transitions and crystal growth under such soft chemical processes is discussed in detail, and the evolution of the phase composition is illustrated according to dissolution−reassembly equilibrium.
Co-reporter:Juan Wang, Juan Long, Zhihong Liu, Wangze Wu, Chengguo Hu
Biosensors and Bioelectronics (15 May 2017) Volume 91() pp:
Publication Date(Web):15 May 2017
DOI:10.1016/j.bios.2016.12.029
•A simple deposition method for producing uniform Bi2S3 films was established.•A label-free and light-addressable PEC sensor was constructed on the Bi2S3 films.•The sensor can achieve sensitive multiplexed detection on a single electrode.•The sensor possesses properties of high throughput and self-calibration ability.The sensitive and label-free detection of multiple biomarkers on a single electrode by photoelectrochemical (PEC) sensors based on light addressing strategies is very attractive for developing portable and high-throughput biosensing systems. The essential prerequisite of this proposal is the employment of uniform photovoltaic material modified electrodes with high conversion efficiency. Herein, a novel two-step constant potential deposition method for the rapid fabrication of bismuth sulfide film modified ITO electrodes (Bi2S3/ITO) was established. The produced Bi2S3/ITO, with excellent uniformity and high conversion efficiency in visible light ranges, was further modified with gold nanoparticles (AuNPs) and then divided into separated identical sensing zones by insulative paints. The adsorption-based immobilization of antibodies of three tumor markers, i.e., a-fetoprotein (AFP), carcinoembryonic antigen (CEA) and cancer antigen 19-9 (CA19-9), onto different sensing zones of the electrode and the further blocking with BSA established a label-free and light-addressable PEC sensor (LF-LAPECS), which can achieve the rapid and sensitive detection of these biomarkers with wide linear ranges, low detection limits and self-calibration ability. Moreover, the detection throughput can be conveniently improved by enlarging the size of the substrate electrode and increasing the number of separated sensing zones. The present work thus demonstrates the promising applications of PEC techniques for developing sensitive, time-saving, cost-effective and high-throughput biosensing methods.
Co-reporter:Lingyu Zeng, Shiyu Chen, Tian Xia, Cheng Zhong and Zhihong Liu
Chemical Communications 2014 - vol. 50(Issue 76) pp:NaN11142-11142
Publication Date(Web):2014/07/30
DOI:10.1039/C4CC05010J
We have reported a new strategy to design two-photon (2P) fluorescent probes for simultaneous elevation of the 2P absorption cross-section (δ) and quantum yield (ϕ). The target-induced hydrogen bond-chelated ring enhances molecular planarity, leading to the enhancement of δ; meanwhile, the photo-induced electron transfer (PET) “on–off” process modulates ϕ.
Co-reporter:Lingzhi Liu, Hui Li, Ting Qiu, Guohua Zhou, Kwok-Yin Wong, Zhike He and Zhihong Liu
Chemical Communications 2011 - vol. 47(Issue 9) pp:NaN2624-2624
Publication Date(Web):2011/01/13
DOI:10.1039/C0CC04712K
A new molecular beacon (MB) driven by two-photon excitation (TPE) using quantum dots as energy donor is constructed, which provides reduced direct excitation of acceptor and is free of interferences from autofluorescence or scattering light in a complicated biological matrix.
Co-reporter:Zhiqiang Mao, Wenqi Feng, Zhen Li, Lingyu Zeng, Weijie Lv and Zhihong Liu
Chemical Science (2010-Present) 2016 - vol. 7(Issue 8) pp:NaN5235-5235
Publication Date(Web):2016/04/26
DOI:10.1039/C6SC01313A
As a pivotal signalling molecule involved in various physiological and pathological processes, nitric oxide (NO) has motivated increasing interest in the last few decades. Although a considerable number of fluorescent probes have been developed for NO imaging, the in situ tracking of this gas molecule in biological events remains a big challenge, mainly because of the relatively short excitation and/or emission wavelengths, which are subject to background interference and lowered collection efficiency in deep-tissue imaging. Herein, we report a far-red emissive (650 nm) two-photon (TP) excitable NRNO probe, using Nile Red as the TP fluorophore, for NO detection and imaging both in vitro and in vivo. The NRNO probe shows a fast (within 180 s) and specific fluorescence response toward NO with a limit of detection (LOD) as low as 46 nM. The excellent properties of NRNO enable it to sensitively detect both exogenously and endogenously generated NO in living cells. The “NIR in” and “far-red out” lights lead to improved penetrating ability, thus endowing the probe with high resolution for the illumination of deep tissues. It is therefore able to visualize the NO generation in a lipopolysaccharide (LPS)-mediated inflammation process for the first time. Our results demonstrate that NRNO could be a practical tool for studying the NO-related biological events. Moreover, this study also suggests the possibility of using Nile Red and its derivatives to develop far-red emissive TP probes, which is an important, yet undeveloped area.
Co-reporter:Yunxia Yuan and Zhihong Liu
Chemical Communications 2012 - vol. 48(Issue 60) pp:NaN7512-7512
Publication Date(Web):2012/05/29
DOI:10.1039/C2CC33289B
The energy transfer efficiency from up-converting donors was significantly enhanced by constructing beacon sensors, which led to increased sensitivities in DNA recognition and protein determination.
Co-reporter:Yan Xiao, Zhengjun Wu, Kwok-Yin Wong and Zhihong Liu
Chemical Communications 2014 - vol. 50(Issue 37) pp:NaN4852-4852
Publication Date(Web):2014/03/25
DOI:10.1039/C4CC01154F
Novel hairpin DNA probes are designed and constructed based on target-induced in situ generation of luminescent silver nanoclusters. This design allows specific and versatile detection of diverse targets with easy operation and low cost.
Co-reporter:Yunxia Yuan, Shufang Wu, Fan Shu and Zhihong Liu
Chemical Communications 2014 - vol. 50(Issue 9) pp:NaN1097-1097
Publication Date(Web):2013/11/20
DOI:10.1039/C3CC47755J
An ultrathin MnO2 nanosheet is established as a label-free two-dimensional nanoplatform for homogeneous biosensing. Two biosensors based on an MnO2 nanosheet with favourable performances are constructed for OTA and Cat D using different probes and following different sensing principles.
Co-reporter:Xuefeng Li, Hao Ren, Zhijuan Zou, Jiaojiao Sun, Jingyu Wang and Zhihong Liu
Chemical Communications 2016 - vol. 52(Issue 3) pp:NaN456-456
Publication Date(Web):2015/10/06
DOI:10.1039/C5CC07372C
Molecularly grafted carbon nitride (CN) nanosheets, matching well with the emission energy of upconversion phosphors (UCPs), were acquired for the first time. As a result of energy gap engineering, the assembled composites successfully realized the full use of visible-NIR light and afforded much higher activity than any CN- or UCP-based photocatalyst ever reported.
Co-reporter:Zhiqiang Mao, Hong Jiang, Zhen Li, Cheng Zhong, Wei Zhang and Zhihong Liu
Chemical Science (2010-Present) 2017 - vol. 8(Issue 6) pp:NaN4538-4538
Publication Date(Web):2017/04/20
DOI:10.1039/C7SC00416H
In situ fluorescence imaging of nitric oxide (NO) is a powerful tool for studying the critical roles of NO in biological events. However, the selective imaging of NO is still a challenge because most currently available fluorescent probes rely on the o-phenylenediamine (OPD) recognition site, which reacts with both NO and some abundant reactive carbonyl species (RCS) (such as dehydroascorbic acid and methylglyoxal) and some reactive oxygen/nitrogen species (ROS/RNS). To address this problem, a new fluorescent probe, NCNO, based on the N-nitrosation of aromatic secondary amine was designed to bypass the RCS, ROS, and RNS interference. As was expected, the probe NCNO could recognize NO with pronounced selectivity and sensitivity among ROS, RNS, and RCS. The probe was validated by detecting NO in live cells and deep tissues owing to its two-photon excitation and red-light emission. It was, hence, applied to monitor NO in ischemia reperfusion injury (IRI) in mice kidneys by two-photon microscopy for the first time, and the results vividly revealed the profile of NO generation in situ during the renal IRI process.
Glycine,N-[2-[2-[2-[bis(carboxymethyl)amino]-5-(2,7-difluoro-6-hydroxy-3-oxo-3H-xanthen-9-yl)phenoxy]ethoxy]-4-methylphenyl]-N-(carboxymethyl)-
1,2-Ethanediamine, N,N-bis(2-pyridinylmethyl)-
C N
Benzenemethanamine, 4-amino-, monohydrochloride
Hydroxyl
Propanedial
Methyl (3s,4r)-3-benzoyloxy-8-methyl-8-azabicyclo[3.2.1]octane-4-carboxylate