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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

The mechanism for promoted oxygenation of V(IV) by goethite: Positive effect of surface hydroxyl groups

Xingyun Hu,Xianjia Peng,Linghao Kong,Feng Zhu

The most toxic and mobile form of vanadium (V) is V(V). Thus, the oxidation of V is a subject of considerable importance since the process may increase environmental risks of V. V(IV) is known to be stable when pH < 4.5. However, in this study, stable V(IV) was oxidized almost completely in goethite suspension within 60 min at pH 2.0 and pH 4.0, correspondingly, only 25%–30% and 15%–20% of V(IV) were oxidized in equimolar Fe 3+ solution and the blank solution, respectively. The promoted oxidation of V(IV) by FeOOH is attributed to the formation of the complex, VO(OFe<) + or VO(OFe<) 2 . On the one hand, the formation of the complex caused higher pH in the interface of solid FeOOH and corresponding lower conditional potential of V(V)/V(IV) than those in bulk solutions, which facilitates the oxidation of V(IV). On the other hand, the surface group OFe < may serve as a medium that facilitating the electron transfer from V(IV) ions to dissolved oxygen molecules, also favoring the oxidation of V(IV). This study not only deepens our understanding of the transfer, transformation, and risk of V in environments, but also provides a reference to speculate the fate of similar elements in environments.

研究领域: 环境化学 · 地球化学 · 水污染控制 · 金属形态转化 · 界面过程
✓ 已验证 DOI 高影响因子
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DALTON TRANSACTIONS · 2015 ·Vol. 44 ·期 17 ·8278-8283 · IF 4.197

A functional ruthenium(II) complex for imaging biothiols in living bodies

Zhiqiang Ye,Quankun Gao,Xin An,Bo Song,Jingli Yuan

A unique ruthenium(II) complex, [Ru(bpy)2(DNS-bpy)](PF6)2 [bpy: 2,2′-bipyridine, DNS-bpy: 4-(2,4-dinitrophenylthio)-2,2′-bipyridine], that can act as a probe for the recognition and luminescence sensing of biothiols has been designed and synthesized. Due to the presence of effective photo-induced electron transfer (PET) from the potent electron donor (Ru-bpy centre) to the strong electron acceptor (2,4-dinitrophenyl moiety), the Ru(II) complex itself is weakly luminescent. Reaction of [Ru(bpy)2(DNS-bpy)](PF6)2 with biothiols leads to the replacement of the 2,4-dinitrophenyl moiety by biothiols, which results in the loss of PET within the complex, to allow recovery of the MLCT-based emission of the Ru(II) complex with an 80-fold increase in luminescence intensity. Taking advantage of the high specificity and sensitivity, and the excellent photophysical properties of Ru(II) complexes, [Ru(bpy)2(DNS-bpy)](PF6)2 was successfully applied to the luminescence imaging of biothiols in living Daphnia magna. The results demonstrated the practical applicability of [Ru(bpy)2(DNS-bpy)](PF6)2 as a luminescent probe for the monitoring of biothiols in living bodies.

研究领域: 分析化学 · 分子生物学 · 化学生物学 · 生物成像 · 无机化学
✓ 已验证 DOI 高影响因子
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MICROCHEMICAL JOURNAL · 2022 · IF 5.304

The parallel fluorescence determination of iron(III), terbium(III) and europium(III) ions using the coal-derived carbon dot

Xu Chu,Tao Chen,Yan Cao

This paper reports a simple, rapid and sensitive fluorescence sensor for the parallel determination of iron (III) (Fe 3+ ), terbium (III) (Tb 3+ ) and europium (III) (Eu 3+ ) ions using Carbon Dot (CD) serving as a fluorescence probe. The Carbon Dot (CD), which was synthesized via an acid-cutting method using anthracite coal as the carbon source, was found to have rich carboxyl and hydroxyl groups on its surface. The fluorescence of the as-prepared CD can be selectively quenched by the Fe 3+ ion via non-radiative electron-transfer, and furthermore, the as-prepared CD can also sensitize the luminescence of both Tb 3+ and Eu 3+ ions through the antenna effect and enhance the fluorescence of Tb 3+ and Eu 3+ by more than several orders of magnitude. Therefore, the as-prepared CD was applied as a fluorescence probe towards the parallel determination of Fe 3+ , Tb 3+ and Eu 3+ and exhibited detection limits in 0.019, 0.10 and 0.79 μM, respectively. The fluorescence quenching mechanism and energy transfer mechanism were also studied in details.

研究领域: 分析化学 · 环境监测 · 纳米材料 · 荧光探针 · 生物传感
✓ 已验证 DOI 高影响因子
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Progress in Natural Science-Materials International · 2019 ·Vol. 29 ·期 4 ·379-383 · IF 3.31

Photo-improved hydrogen evolution reaction activity of the Pt/CdS electrocatalyst

Yongsheng Fu,Jun Li,Jianguo Li

The effect of CdS content on the photo-induced improvement of hydrogen evolution reaction activity of the Pt/CdS electrocatalyst was investigated. Although the electrons transferred from CdS to Pt in the Pt/CdS electrocatalyst increased with the CdS content under illumination, the electrochemical active surface area of the Pt/CdS electrocatalyst decreased with the CdS content, resulting that the photo-induced improvement of hydrogen evolution reaction activity of the Pt/CdS electrocatalyst decreased with the CdS content.

研究领域: 材料科学 · 催化化学 · 物理化学 · 纳米材料 · 能源化学
✓ 已验证 DOI 高影响因子
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BIOINORGANIC CHEMISTRY AND APPLICATIONS · 2016 ·Vol. 2016 ·期 1 ·3585781 · IF 1.488

Reversible Oxygenation of α-Amino Acid–Cobalt(II) Complexes

Xincun Zhang,Fan Yue,Hui Li,Yan Huang,Yi Zhang,Hongmei Wen,Jide Wang

We systematically investigated the reversibility, time lapse, and oxygenation-deoxygenation properties of 15 natural α -amino acid–Co(II) complexes through UV-vis spectrophotometer, polarographic oxygen electrode, and DFT calculations, respectively, to explore the relationship between the coordinating structure and reversible oxygenation of α -amino acid–Co(II) complexes. Results revealed that the α -amino acid structure plays a key role in the reversible oxygenation properties of these complexes. The specific configuration of the α -amino acid group affects the electron of Co(II) transfer to the π ⁎ orbit of O 2 ; this phenomenon also favors the reversible formation and dissociation of Co–O 2 bond when O 2 coordinates with Co(II) complexes. Therefore, the co-coordination of amino and carboxyl groups is a determinant of Co complexes to absorb O 2 reversibly. The group adjacent to the α -amino acid unit evidently influences the dioxygen affinity and antioxidation ability of the complexes. The presence of amino (or imino) and hydroxy groups adjacent to the α -amino acid group increases the oxygenation-deoxygenation rate and the number of reversible cycles. Our findings demonstrate a new mechanism to develop reversible oxygenation complexes and to reveal the oxygenation of oxygen carriers.

研究领域: 无机生物化学 · 金属蛋白化学 · 分子生物学 · 配位化学 · 氧化还原生物学
✓ 已验证 DOI 高影响因子
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY · 2012 ·Vol. 50 ·期 24 ·4995-4999 · IF 3.919

SET-LRP of acrylonitrile catalyzed by tin powder

Zhihai Hao,Hou Chen,Delong Liu,Lijun Fan

Sn(0)-mediated single electron transfer-living radical polymerization (SET-LRP) of acrylonitrile (AN) with carbon tetrachloride (CCl 4 ) as initiator and hexamethylenetetramine (HMTA) as ligand in N, N -dimethylformamide (DMF) was studied. The polymerization obeyed first order kinetic. The molecular weight of polyacrylonitrile (PAN) increased linearly with monomer conversion and PAN exhibited narrow molecular weight distributions. Increasing the content of Sn(0) resulted in an increase in the molecular weight and the molecular weight distribution. Effects of ligand and initiator were also investigated. The block copolymer PAN- b -polymethyl methacrylate with molecular weight at 126,130 and polydispersity at 1.36 was successfully obtained. © 2012 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2012

研究领域: 高分子化学 · 聚合反应 · 功能高分子 · 材料化学 · 有机合成
✓ 已验证 DOI 高影响因子
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TETRAHEDRON · 2014 ·Vol. 70 ·期 47 ·9033-9040 · IF 2.817

Substituent effects on the redox potentials of dihydroxybenzenes: theoretical and experimental study

Tao Liu,Meng-Meng Liu,Xiao-Wen Zheng,Chong-Yang Du,Xiang-Yang Cui,Lu Wang,Ling-Li Han,Zhang-Yu Yu

The redox reactions of p -hydroquinone and pyrocatechol undergo a two-proton-two-electron process in aqueous solution. We calculated their redox potentials at the B3LYP/6-311+G(d,p) level, and verified the values by employing cyclic voltammetry experiments. Then we selected seven substituent groups (–F, –Cl, –OH, –COOH, –CN, –NH 2 , and –NO 2 groups) to systematically investigate the substituent effect , including the sort, position, and number of the substituent, on the redox potentials of p -hydroquinone and pyrocatechol. The calculated results show that –NH 2 and –OH groups can decrease the redox potentials, while –F, –Cl, –COOH, –CN, and –NO 2 groups increase the potential values of p -hydroquinone and pyrocatechol. The calculations can accurately predict the substituent effects on the redox potentials of pyrocatechol and p -hydroquinone. We would expect that the accurate calculation results for the model systems could be applied in the prediction of electrode potentials of other molecules.

研究领域: 物理有机化学 · 电化学 · 计算化学 · 分子设计 · 生物电化学
✓ 已验证 DOI 高影响因子
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RSC Advances · 2018 ·Vol. 8 ·期 66 ·38003-38012 · IF 2.936

Construction of myoglobin–amphiphilic alginate caprylamide–graphene composite modified electrode for the direct electron transfer between redox proteins and electrode and electrocatalysis of myoglobin

Xiuqiong Chen,Huiqiong Yan,Wei Sun,Guangying Chen,Changjiang Yu,Wen Feng,Qiang Lin

To achieve the dispersion of the hydrophobic graphene (GR), the amphiphilic alginate caprylamide (ACA) was synthesized to fabricate electroactive Nafion/Mb–ACA–GR/CILE for the accurate determination of trichloroacetic acid (TCA). SEM observation, FT-IR and UV-Vis spectroscopic analysis indicated that ACA could tightly immobilize Mb and GR on the electrode surface by constructing biointerfaces, which not only provided Mb a suitable microenvironment to maintain its biological activity, but also shortened the distances between the active centers of Mb with carbon ionic liquid electrode (CILE), thus promoting the electron transfer rate. The electrochemical characterization of Nafion/Mb–ACA–GR/CILE showed that the direct electron transfer of Mb was realized on the modified electrode, which was attributed to the high electrical conductivity and excellent electrocatalytic activity of GR and good biocompatibility of ACA. Moreover, Nafion/Mb–ACA–GR/CILE exhibited good electrocatalytic activity towards TCA with the linear range from 2.5 to 47.3 mmol L−1 and lower KMapp value of 8.3 mmol L−1. Moreover, the modified electrode also revealed good stability, reproducibility and accurate detection of tap-water, exhibiting great potential for the applications as the third-generation electrochemical biosensors.

研究领域: 生物医学工程 · 电化学传感 · 纳米生物技术 · 分子生物学 · 分析化学 · 生物传感器
✓ 已验证 DOI 高影响因子
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EES Catalysis · 2023 ·Vol. 1 ·期 3 ·312-321 · IF 0

Facet-engineered photoelectrochemical nanocatalysts toward fast kinetic lithium–air batteries

Yiqiao Wang,Siyuan Pan,Huan Li,Dewang Li,Yong Guo,Sijia Chi,Chuannan Geng,Shichao Wu,Quan-Hong Yang

Despite lithium–air batteries having unprecedented theoretical energy supremacy, rambling Li2O2 growth typically impedes O2 diffusion and electron transfer, causing low capacity, poor charging kinetics and short cycle life. Herein, we propose synergistic catalysis in the cathode by engineering the crystal facet of Fe2O3 nanoplates and introducing a visible light-excited photochemical effect. The growth of Li2O2 is regulated with a uniform distribution, mitigating local product aggregation and thus reducing the barriers of O2 diffusion and electron transfer. The improved reaction kinetics lead to ∼420% capacity improvement, low charge potential, superior rate performance, and long-term stability (300 cycles) in actual air. We reveal a mechanism that photoelectrons around each catalyst node and the resultant homogeneous internal electric field increase charge transfer, decrease soluble intermediates, and enable high electrochemical reversibility of amorphous Li2O2 with an ordered process. This study provides inspiring insights for future research into controlling product ordering in Li–air batteries.

研究领域: 电化学 · 纳米材料科学 · 能源化学 · 催化化学 · 电池技术
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BIOSENSORS & BIOELECTRONICS · 2011 ·Vol. 30 ·期 1 ·112-117 · IF 5.361

One-step “green” preparation of graphene nanosheets and carbon nanospheres mixture by electrolyzing graphite rob and its application for glucose biosensing

Huanshun Yin,Yunlei Zhou,Xiaomeng Meng,Kun Shang,Shiyun Ai

The graphene nanosheets and carbon nanospheres mixture (GNS–CNS) was prepared by electrolyzing graphite rob in KNO 3 solution under constant current, which was characterized by TEM, AFM, SEM, FT-IR, XRD, XPS, TGA and UV–vis. The nano-mixture can keep stable in water for more than one month. Based on this kind of mixture material, a novel electrochemical biosensing platform for glucose determination was developed. Cyclic voltammetry of glucose oxidase (GOD) immobilized on GNS–CNS/GCE exhibited a pair of well-defined quasi-reversible redox peaks at −0.488   V ( E pa ) and −0.509   V ( E pc ) by direct electron transfer between the protein and the electrode. The charge-transfer coefficient ( α ) was 0.51, the electron transfer rate constant was 2.64   s −1 and the surface coverage of HRP was 3.18   ×   10 −10   mol   cm −2 . The immobilized GOD could retain its bioactivity and catalyze the reduction of dissolved oxygen. The glucose biosensor has a linear range from 0.4 to 20   mM with detection limit of 0.1   mM. Moreover, the biosensor exhibits acceptable reproducibility and storage stability. The fabricated biosensor was further used to determine glucose in human plasma sample with the recoveries from 96.83% to 105.52%. Therefore, GOD/GNS–CNS/GCE could be promisingly applied to determine blood sugar concentration in the practical clinical analysis.

研究领域: 分析化学 · 纳米生物技术 · 电化学传感 · 生物医学工程 · 临床检验
✓ 已验证 DOI 高影响因子
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2018 ·Vol. 20 ·期 44 ·28068-28074 · IF 3.906

Photo-induced dual passivation via Usanovich acid–base on surface defects of methylammonium lead triiodide perovskite

Yue Yu,Sushu Wan,Daocheng Hong,Yuxi Tian

Post-fabrication defect passivation of organometal halide perovskites has become an efficient way to improve their photophysical properties, but the underlying mechanisms are still in debate. In this work, we used p-benzoquinone (p-BQ) to generate surface defects on methylammonium lead triiodide perovskite (MAPbI3), and found that a Usanovich acid–base (O2, acetone or acetonitrile) treatment can effectively passivate those defects and lead to photoluminescence (PL) enhancement. The passivation effect arose from partial neutralization of defect charges via electron transfer between passivation reagents and relevant defects. O2 accepted photo-generated electrons, formed negatively charged oxygen species and attached to the I vacancy site to reduce its PL quenching efficiency by neutralising the defects positive charge. Likewise, acetone accepted photo-generated holes, formed positively charged species and partially neutralised the defects negative charge. The reduced trapping ability of defects caused PL enhancement. In addition, the observed photo-catalysed oxidation of acetone by O2 on the crystal surface supported the single electron transfer mechanism, and showed the potential of MAPbI3 as a photo-catalyst.

研究领域: 材料科学 · 光物理学 · 半导体材料 · 表面化学 · 光电功能材料
✓ 已验证 DOI 高影响因子
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Plasma Processes and Polymers · 2011 ·Vol. 8 ·期 10 ·923-931 · IF 1.643

Plasma Polymerized Pyrrole Films for Biological Applications: Correlation Between Protein Adsorption Properties and Characteristics

Zhihong Zhang,Jun Dou,Fufeng Yan,Xianjun Zheng,Xili Li,Shaoming Fang

The present work describes the fabrication, characterization, and optimization of plasma polymerized pyrrole films, PPpy, prepared by continuous wave for application as the adhesion layers of bovine serum albumin (BSA). Plasma conditions used throughout the work produced significant differences in the chemical, physical, and electrochemical properties of the resultant PPpy films. Structural analysis and property characterizations of PPpy were carried out using Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and electrochemical workstation. Surface plasmon resonance spectroscopy was used to investigate the adsorption kinetics of BSA onto PPpy films. Moreover, when immersed in solutions or after BSA adsorption, the differences of electron transfer at the interfaces between the PPpy and the electrolyte solutions were determined by electro impedance spectroscopy. While there is a clear dependence of the protein adsorption affinity on the plasma polymerization condition employed during the film preparation. The relationship between film structure, electrochemical properties, polymer stability in aqueous buffer, and protein binding affinities are discussed.

研究领域: 生物材料 · 表面科学 · 生物医学工程 · 分子生物学 · 分析化学 · 生物传感器
✓ 已验证 DOI 高影响因子
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