NiCo2O4 with oxygen vacancies as better performance electrode material for supercapacitor
作者:
Yan, Dan;Wang, Wei;Luo, Xin;Chen, Chao;Zeng, Yan;...
期刊:
Chemical Engineering Journal ,2018年334:864-872 ISSN:1385-8947
通讯作者:
Zhu, Zhihong
作者机构:
[Yan, Dan; Wang, Wei; Chen, Chao; Zhu, Zhihong; Luo, Xin] Cent China Normal Univ, Inst Nanosci & Nanotechnol, Coll Phys Sci & Technol, Wuhan 430079, Hubei, Peoples R China.;[Zeng, Yan] Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.
通讯机构:
[Zhu, Zhihong] C;Cent China Normal Univ, Inst Nanosci & Nanotechnol, Coll Phys Sci & Technol, Wuhan 430079, Hubei, Peoples R China.
关键词:
Chemical reduction;NiCo 2 O 4;Oxygen vacancies;Supercapacitor
摘要:
In this paper, using a chemical reduction method, oxygen vacancies are introduced into different NiCo2O4 nanostructures, crystal structure analyses and electrochemical property studies on oxygen vacancies are further described by two sets of in situ control experiments. Electrochemical data show that reduced NiCo2O4 electrodes with appropriate oxygen vacancies exhibit a significant improvement on electrical conductivity and capacitance compared to the untreated electrodes. Interestingly, the capacitance of the reduced NiCo2O4 nanosheets electrode (0.5-NiCo2O4 NS-vac) and the reduced NiCo2O4 nanowires electrode (0.5-NiCo2O4 NW-vac) obtained from 0.5 M NaBH4 solution is significantly higher than that of the pristine electrodes, and has increased by 77% and 100.4%, respectively. Due to the introducing of oxygen vacancies in NiCo2O4, part of Co–O and Ni–O bonds in the crystals are destroyed and the crystalline degree of the crystals decreases. However, the reduced NiCo2O4 electrodes still maintain excellent cycling performance after cyclic test. These results indicate that the appropriate oxygen vacancies in NiCo2O4 can be an efficient strategy for enhancing the performance of NiCo2O4. © 2017
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英文
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Copper-Catalyzed Radical Cross-Coupling of Redox-Active Oxime Esters, Styrenes, and Boronic Acids
作者:
Yu, Xiao-Ye;Zhao, Quan-Qing;Chen, Jun;Chen, Jia-Rong* ;Xiao, Wen-Jing*
期刊:
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION ,2018年57(47):15505-15509 ISSN:1433-7851
通讯作者:
Chen, Jia-Rong;Xiao, Wen-Jing
作者机构:
[Zhao, Quan-Qing; Chen, Jia-Rong; Xiao, WJ; Xiao, Wen-Jing; Chen, Jun; Yu, Xiao-Ye] Cent China Normal Univ, Coll Chem, Minist Educ,CCNU uOttawa Joint Res Ctr, Hubei Int Sci & Technol Cooperat Base Pesticide &, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.;[Xiao, Wen-Jing] Lanzhou Univ, State Key Lab Appl Organ Chem, Lanzhou 730000, Gansu, Peoples R China.
通讯机构:
[Chen, JR; Xiao, WJ] C;[Xiao, Wen-Jing] L;Cent China Normal Univ, Coll Chem, Minist Educ,CCNU uOttawa Joint Res Ctr, Hubei Int Sci & Technol Cooperat Base Pesticide &, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.;Lanzhou Univ, State Key Lab Appl Organ Chem, Lanzhou 730000, Gansu, Peoples R China.
关键词:
copper;cross-coupling;photochemistry;radicals;synthetic methods
摘要:
A visible-light-driven, copper-catalyzed three-component radical cross-coupling of oxime esters, styrenes, and boronic acids has been developed. Key steps of this protocol involve catalytic generation of an iminyl radical from a redox-active oxime ester and subsequent C−C bond cleavage to generate a cyanoalkyl radical. Upon its addition to styrene, the newly formed benzylic radical undergoes coupling with a boronic-acid-derived ArCuII complex to achieve 1,1-diarylmethane-containing alkylnitriles. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
语种:
英文
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Iron oxide shell mediated environmental remediation properties of nano zero-valent iron
作者:
Mu, Yi;Jia, Falong;Ai, Zhihui* ;Zhang, Lizhi*
期刊:
Environmental Science: Nano ,2017年4(1):27-45 ISSN:2051-8153
通讯作者:
Ai, Zhihui;Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Mu, Yi; Ai, ZH; Zhang, LZ; Jia, Falong; Ai, Zhihui] Cent China Normal Univ, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Ai, ZH; Zhang, LZ] C;Cent China Normal Univ, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
摘要:
Nano zero-valent iron (nZVI) has attracted much more attention for its potential applications in the fields of environmental contaminant remediation and detoxification. Generally, nZVI consists of a zero-valent iron (Fe0) core and an iron oxide shell structure. As the underlying Fe0 core and the surface oxide shell determine the physical and chemical properties of nZVI, the nature of the oxide shell inevitably affects the organic/inorganic pollutant removal performance of nZVI, which has not been reviewed previously. In this article, we first introduce the synthesis and the oxide shell formation mechanism of core-shell structured nZVI and then discuss various characterization techniques to reveal the structure and chemical composition of the oxide shell. Subsequently, we clarify the roles of the oxide shell in the organic contaminant degradation efficiency and the molecular oxygen activation performance of nZVI and also highlight the effect of the oxide shell on heavy metal removal (including As) with nZVI. In addition, we summarize some oxide shell modification strategies to enhance the capacity and longevity of nZVI. Finally, we discuss the impacts of typical natural groundwater constituents (e.g. cations, anions, organic ligands, and dissolved oxygen) on the reactivity of nZVI and point out some unresolved issues related to the oxide shell dependent contaminant removal properties of nZVI. © The Royal Society of Chemistry.
语种:
英文
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Metal-Organic Framework-Derived Non-Precious Metal Nanocatalysts for Oxygen Reduction Reaction
作者:
Fu, Shaofang;Zhu, Chengzhou* ;Song, Junhua;Du, Dan;Lin, Yuehe*
期刊:
Advanced Energy Materials ,2017年7(19):1700363- ISSN:1614-6832
通讯作者:
Zhu, Chengzhou;Lin, Yuehe
作者机构:
[Zhu, Chengzhou; Song, Junhua; Du, Dan; Fu, Shaofang; Lin, Yuehe; Zhu, CZ; Lin, YH] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.;[Du, Dan] Cent China Normal Univ, Minist Educ PR China, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.;[Du, Dan] Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.
通讯机构:
[Zhu, CZ; Lin, YH] W;Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.
关键词:
electrocatalysis;metal-organic frameworks;non-precious metal catalysts;oxygen reduction reactions;porous nanostructures
摘要:
By virtue of diverse structures and tunable properties, metal-organic frameworks (MOFs) have presented extensive applications including gas capture, energy storage, and catalysis. Recently, synthesis of MOFs and their derived nanomaterials provide an opportunity to obtain competent oxygen reduction reaction (ORR) electrocatalysts due to their large surface area, controllable composition and pore structure. This review starts with the introduction of MOFs and current challenges of ORR, followed by the discussion of MOF-based non-precious metal nanocatalysts (metal-free and metal/metal oxide-based carbonaceous materials) and their application in ORR electrocatalysis. Current issues in MOF-derived ORR catalysts and some corresponding strategies in terms of composition and morphology to enhance their electrocatalytic performance are highlighted. In the last section, a perspective for future development of MOFs and their derivatives as catalysts for ORR is discussed. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
语种:
英文
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New Reaction Pathway Induced by Plasmon for Selective Benzyl Alcohol Oxidation on BiOCl Possessing Oxygen Vacancies
作者:
Li, Hao;Qin, Feng;Yang, Zhiping;Cui, Ximin;Wang, Jianfang* ;...
期刊:
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY ,2017年139(9):3513-3521 ISSN:0002-7863
通讯作者:
Wang, Jianfang;Zhang, Lizhi
作者机构:
[Wang, Jianfang; Li, Hao; Cui, Ximin; Qin, Feng] Chinese Univ Hong Kong, Dept Phys, Shatin, Hong Kong, Peoples R China.;[Zhang, Lizhi; Yang, Zhiping; Li, Hao] Cent China Normal Univ, Inst Environm Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Wang, Jianfang; Zhang, Lizhi] C;Chinese Univ Hong Kong, Dept Phys, Shatin, Hong Kong, Peoples R China.;Cent China Normal Univ, Inst Environm Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
摘要:
Selective organic transformation under mild conditions constitutes a challenge in green chemistry, especially for alcohol oxidation, which typically requires environmentally unfriendly oxidants. Here, we report a new plasmonic catalyst of Au supported on BiOCl containing oxygen vacancies. It photocatalyzes selective benzyl alcohol oxidation with O-2 under visible light through synergistic action of plasmonic hot electrons and holes. Oxygen vacancies on BiOCl facilitate the trapping and transfer of plasmonic hot electrons to adsorbed O-2, producing center dot O-2(-) radicals, while plasmonic hot holes remaining on the Au surface mildly oxidize benzyl alcohol to corresponding carbon-centered radicals. The hypothesized concerted ring addition between these two radical species on the BiOCI surface highly favors the production of benzaldehyde along with an unexpected oxygen atom transfer from O-2 to the product. The results and understanding acquired in this study, based on the full utilization of hot charge carriers in a plasmonic metal deposited on a rationally designed support, will contribute to the development of more active and/or selective plasmonic catalysts for a wide variety of organic transformations.
语种:
英文
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Solar water splitting and nitrogen fixation with layered bismuth oxyhalides
作者:
Li, Jie;Li, Hao;Zhan, Guangming;Zhang, Lizhi*
期刊:
ACCOUNTS OF CHEMICAL RESEARCH ,2017年50(1):112-121 ISSN:0001-4842
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Li, Jie; Li, Hao; Zhan, Guangming] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm & Appl Chem,Coll Chem, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm & Appl Chem,Coll Chem, Wuhan 430079, Peoples R China.
摘要:
CONSPECTUS: Hydrogen and ammonia are the chemical molecules that are vital to Earth's energy, environmental, and biological processes. Hydrogen with renewable, carbon-free, and high combustion-enthalpy hallmarks lays the foundation of next-generation energy source, while ammonia furnishes the building blocks of fertilizers and proteins to sustain the lives of plants and organisms. Such merits fascinate worldwide scientists in developing viable strategies to produce hydrogen and ammonia. Currently, at the forefronts of hydrogen and ammonia syntheses are solar water splitting and nitrogen fixation, because they go beyond the high temperature and pressure requirements of methane stream reforming and Haber-Bosch reaction, respectively, as the commercialized hydrogen and ammonia production routes, and inherit the natural photosynthesis virtues that are green and sustainable and operate at room temperature and atmospheric pressure. The key to propelling such photochemical reactions lies in searching photocatalysts that enable water splitting into hydrogen and nitrogen fixation to make ammonia efficiently. Although the past 40 years have witnessed significant breakthroughs using the most widely studied TiO2, SrTiO3, (Ga1-xZnx)(N1-xOx), CdS, and g-C3N4 for solar chemical synthesis, two crucial yet still unsolved issues challenge their further progress toward robust solar water splitting and nitrogen fixation, including the inefficient steering of electron transportation from the bulk to the surface and the difficulty of activating the N?N triple bond of N2. This Account details our endeavors that leverage layered bismuth oxyhalides as photocatalysts for efficient solar water splitting and nitrogen fixation, with a focus on addressing the above two problems. We first demonstrate that the layered structures of bismuth oxyhalides can stimulate an internal electric field (IEF) that is capable of efficiently separating electrons and holes after their formation and of precisely channeling their migration from the bulk to the surface along the different directions, thus enabling more electrons to reach the surface for water splitting and nitrogen fixation. Simultaneously, their oxygen termination feature and the strain differences between interlayers and intralayers render the easy generation of surface oxygen vacancies (OVs) that afford Lewis-base and unsaturated-unsaturated sites for nitrogen activation. With these rationales as the guideline, we can obtain striking visible-light hydrogen-and ammonia-evolving rates without using any noble-metal cocatalysts. Then we show how to utilize IEF and OV based strategies to improve the solar water splitting and nitrogen fixation performances of bismuth oxyhalide photocatalysts. Finally, we highlight the challenges remaining in using bismuth oxyhalides for solar hydrogen and ammonia syntheses, and the prospect of further development of this research field. We believe that our mechanistic insights could serve as a blueprint for the design of more efficient solar water splitting and nitrogen fixation systems, and layered bismuth oxyhalides might open up new photocatalyst paradigm for such two solar chemical syntheses. © 2016 American Chemical Society.
语种:
英文
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Phosphate Framework Electrode Materials for Sodium Ion Batteries
作者:
Fang, Yongjin;Zhang, Jiexin;Xiao, Lifen;Ai, Xinping;Cao, Yuliang* ;...
期刊:
Advanced Science ,2017年4(5):1600392- ISSN:2198-3844
通讯作者:
Cao, Yuliang
作者机构:
[Zhang, Jiexin; Cao, Yuliang; Fang, Yongjin; Yang, Hanxi; Ai, Xinping] Wuhan Univ, Coll Chem & Mol Sci, Hubei Key Lab Electrochem Power Sources, Wuhan 430072, Peoples R China.;[Xiao, Lifen] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构:
[Cao, Yuliang] W;Wuhan Univ, Coll Chem & Mol Sci, Hubei Key Lab Electrochem Power Sources, Wuhan 430072, Peoples R China.
关键词:
*Na-ion batteries;*electrode materials;*energy storage;*phosphate;*polyanions
摘要:
Sodium ion batteries (SIBs) have been considered as a promising alternative for the next generation of electric storage systems due to their similar electrochemistry to Li-ion batteries and the low cost of sodium resources. Exploring appropriate electrode materials with decent electrochemical performance is the key issue for development of sodium ion batteries. Due to the high structural stability, facile reaction mechanism and rich structural diversity, phosphate framework materials have attracted increasing attention as promising electrode materials for sodium ion batteries. Herein, we review the latest advances and progresses in the exploration of phosphate framework materials especially related to single-phosphates, pyrophosphates and mixed-phosphates. We provide the detailed and comprehensive understanding of structure–composition–performance relationship of materials and try to show the advantages and disadvantages of the materials for use in SIBs. In addition, some new perspectives about phosphate framework materials for SIBs are also discussed. Phosphate framework materials will be a competitive and attractive choice for use as electrodes in the next-generation of energy storage devices. © 2017 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
语种:
英文
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Single-Atom Electrocatalysts
作者:
Zhu, Chengzhou;Fu, Shaofang;Shi, Qiurong;Du, Dan;Lin, Yuehe*
期刊:
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION ,2017年56(45):13944-13960 ISSN:1433-7851
通讯作者:
Lin, Yuehe
作者机构:
[Zhu, Chengzhou; Du, Dan; Fu, Shaofang; Lin, Yuehe; Shi, Qiurong] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.;[Du, Dan] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticides & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
通讯机构:
[Lin, Yuehe] W;Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.
关键词:
electrocatalysis;electrochemistry;energy generation;single-atom catalysts;supported catalysts
摘要:
Recent years have witnessed a dramatic increase in the production of sustainable and renewable energy. However, the electrochemical performances of the various systems are limited, and there is an intensive search for highly efficient electrocatalysts by more rational control over the size, shape, composition, and structure. Of particular interest are the studies on single-atom catalysts (SACs), which have sparked new interests in electrocatalysis because of their high catalytic activity, stability, selectivity, and 100 % atom utilization. In this Review, we introduce innovative syntheses and characterization techniques for SACs, with a focus on their electrochemical applications in the oxygen reduction/evolution reaction, hydrogen evolution reaction, and hydrocarbon conversion reactions for fuel cells (electrooxidation of methanol, ethanol, and formic acid). The electrocatalytic performance is further considered at an atomic level and the underlying mechanisms are discussed. The ultimate goal is the tailoring of single atoms for electrochemical applications. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
语种:
英文
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Recent Advances in Electrochemical Immunosensors
作者:
Wen, Wei;Yan, Xu;Zhu, Chengzhou;Du, Dan* ;Lin, Yuehe*
期刊:
Analytical Chemistry ,2017年89(1):138-156 ISSN:0003-2700
通讯作者:
Du, Dan;Lin, Yuehe
作者机构:
[Zhu, Chengzhou; Yan, Xu; Du, Dan; Wen, Wei; Lin, Yuehe; Du, D; Lin, YH] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.;[Du, Dan] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
通讯机构:
[Du, D; Lin, YH] W;[Du, Dan] C;Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
语种:
英文
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Novel bright-emission small-molecule NIR-II fluorophores for: In vivo tumor imaging and image-guided surgery
作者:
Sun, Yao;Ding, Mingmin;Zeng, Xiaodong;Xiao, Yuling;Wu, Huaping;...
期刊:
CHEMICAL SCIENCE ,2017年8(5):3489-3493 ISSN:2041-6520
通讯作者:
Hong, Xuechuan
作者机构:
[Ding, Mingmin; Qu, Chunrong; Ding, Bingbing; Zhou, Hui; Sun, Yao; Zeng, Xiaodong; Wu, Huaping; Hou, Wei; Xiao, Yuling; Hong, Xuechuan] Wuhan Univ, Sch Pharmaceut Sci, Hubei Prov Key Lab Dev Originated Dis, State Key Lab Virol,Key Lab Combinatorial Biosynt, Wuhan 430071, Peoples R China.;[Sun, Yao] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticides & Chem Biol, Wuhan 430079, Peoples R China.;[Cheng, Zhen] Stanford Univ, Dept Radiol, Bio X Program, MIPS, Stanford, CA 94305 USA.;[Hong, Xuechuan; Er-bu, A. G. A.] Tibet Univ, Med Coll, Lasa 850000, Peoples R China.;[Zhang, Yejun] Suzhou NIR Opt Technol Co Ltd, Suzhou 215123, Peoples R China.
通讯机构:
[Hong, Xuechuan] W;[Hong, Xuechuan] T;Wuhan Univ, Sch Pharmaceut Sci, Hubei Prov Key Lab Dev Originated Dis, State Key Lab Virol,Key Lab Combinatorial Biosynt, Wuhan 430071, Peoples R China.;Tibet Univ, Med Coll, Lasa 850000, Peoples R China.
摘要:
Though high brightness and biocompatible small NIR-II dyes are highly desirable in clinical or translational cancer research, their fluorescent cores are relatively limited and their synthetic processes are somewhat complicated. Herein, we have explored the design and synthesis of novel NIR-II fluorescent materials (H1) without tedious chromatographic isolation with improved fluorescence performance (QY ≈ 2%) by introducing 2-amino 9,9-dialkyl-substituted fluorene as a donor into the backbone. Several types of water-soluble and biocompatible NIR-II probes: SXH, SDH, and H1 NPs were constructed via different chemical strategies based on H1, and then their potential to be used in in vivo tumor imaging and image-guided surgery in the NIR-II region was explored. High levels of uptake were obtained for both passive and active tumor targeting probes SXH and SDH. Furthermore, high resolution imaging of blood vessels on tumors and the whole body of living mice using H1 NPs for the first time has demonstrated precise NIR-II image-guided sentinel lymph node (SLN) surgery. © 2017 The Royal Society of Chemistry.
语种:
英文
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Oxygen Vacancy Associated Surface Fenton Chemistry: Surface Structure Dependent Hydroxyl Radicals Generation and Substrate Dependent Reactivity
作者:
Li, Hao;Shang, Jian;Yang, Zhiping;Shen, Wenjuan;Ai, Zhihui;...
期刊:
Environmental Science & Technology ,2017年51(10):5685-5694 ISSN:0013-936X
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Yang, Zhiping; Li, Hao; Shen, Wenjuan; Ai, Zhihui; Shang, Jian] Cent China Normal Univ, Minist Educ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Minist Educ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要:
Understanding the chemistry of hydrogen peroxide (H2O2) decomposition and hydroxyl radical (•OH) transformation on the surface molecular level is a great challenge for the application of heterogeneous Fenton system in the fields of chemistry, environmental, and life science. We report in this study a conceptual oxygen vacancy associated surface Fenton system without any metal ions leaching, exhibiting unprecedented surface chemistry based on the oxygen vacancy of electron-donor nature for heterolytic H2O2 dissociation. By controlling the delicate surface structure of catalyst, this novel Fenton system allows the facile tuning of •OH existing form for targeted catalytic reactions with controlled reactivity and selectivity. On the model catalyst of BiOCl, the generated •OH tend to diffuse away from the (001) surface for the selective oxidation of dissolved pollutants in solution, but prefer to stay on the (010) surface, reacting with strongly adsorbed pollutants with high priority. These findings will extend the scope of Fenton catalysts via surface engineering and consolidate the fundamental theories of Fenton reactions for wide environmental applications. © 2017 American Chemical Society.
语种:
英文
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Hydroxylamine Promoted Goethite Surface Fenton Degradation of Organic Pollutants
作者:
Hou, Xiaojing;Huang, Xiaopeng;Jia, Falong;Ai, Zhihui;Zhao, Jincai;...
期刊:
Environmental Science & Technology ,2017年51(9):5118-5126 ISSN:0013-936X
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Hou, Xiaojing; Huang, Xiaopeng; Zhao, Jincai; Jia, Falong; Ai, Zhihui] Cent China Normal Univ, Inst Environm & Appl Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Inst Environm & Appl Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要:
In this study, we construct a surface Fenton system with hydroxylamine (NH2OH), goethite (α-FeOOH), and H2O2 (α-FeOOH-HA/H2O2) to degrade various organic pollutants including dyes (methyl orange, methylene blue, and rhodamine B), pesticides (pentachlorophenol, alachlor, and atrazine), and antibiotics (tetracycline, chloramphenicol, and lincomycin) at pH 5.0. In this surface Fenton system, the presence of NH2OH could greatly promote the H2O2 decomposition on the α-FeOOH surface to produce ·OH without releasing any detectable iron ions during the alachlor degradation, which was different from some previously reported heterogeneous Fenton counterparts. Moreover, the ·OH generation rate constant of this surface Fenton system was 102-104 times those of previous heterogeneous Fenton processes. The interaction between α-FeOOH and NH2OH was investigated with using attenuated total reflectance Fourier transform infrared spectroscopy and density functional theory calculations. The effective degradation of organic pollutants in this surface Fenton system was ascribed to the efficient Fe(III)/Fe(II) cycle on the α-FeOOH surface promoted by NH2OH, which was confirmed by X-ray photoelectron spectroscopy analysis. The degradation intermediates and mineralization of alachlor in this surface Fenton system were then systematically investigated using total organic carbon and ion chromatography, liquid chromatography-mass spectrometry, and gas chromatography-mass spectrometry. This study offers a new strategy to degrade organic pollutants and also sheds light on the environmental effects of goethite. © 2017 American Chemical Society.
语种:
英文
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Manipulating Adsorption–Insertion Mechanisms in Nanostructured Carbon Materials for High-Efficiency Sodium Ion Storage(Open Access)
作者:
Qiu, Shen;Xiao, Lifen;Sushko, Maria L.;Han, Kee Sung;Shao, Yuyan;...
期刊:
Advanced Energy Materials ,2017年7(17):1700403- ISSN:1614-6832
通讯作者:
Cao, Yuliang;Liu, Jun
作者机构:
[Cao, Yuliang; Qiu, Shen; Yang, Hanxi; Ai, Xinping] Wuhan Univ, Coll Chem & Mol Sci, Hubei Key Lab Electrochem Power Sources, Wuhan 430072, Hubei, Peoples R China.;[Xiao, Lifen] Cent China Normal Univ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.;[Sushko, Maria L.; Xiao, Lifen; Shao, Yuyan; Han, Kee Sung; Liu, Jun] Pacific Northwest Natl Lab, Richland, WA 99352 USA.;[Yan, Mengyu; Mai, Liqiang] Wuhan Univ Technol, Sch Mat Sci & Engn, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Hubei, Peoples R China.;[Feng, Jiwen; Liang, Xinmiao] Chinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Hubei, Peoples R China.
通讯机构:
[Cao, Yuliang] W;[Liu, Jun] P;Wuhan Univ, Coll Chem & Mol Sci, Hubei Key Lab Electrochem Power Sources, Wuhan 430072, Hubei, Peoples R China.;Pacific Northwest Natl Lab, Richland, WA 99352 USA.
关键词:
anodes;hard carbon;mechanism;nanostructures;sodium-ion batteries
摘要:
Hard carbon is one of the most promising anode materials for sodium-ion batteries, but the low Coulombic efficiency is still a key barrier. In this paper, a series of nanostructured hard carbon materials with controlled architectures is synthesized. Using a combination of in situ X-ray diffraction mapping, ex situ nuclear magnetic resonance (NMR), electron paramagnetic resonance, electrochemical techniques, and simulations, an “adsorption–intercalation” mechanism is established for Na ion storage. During the initial stages of Na insertion, Na ions adsorb on the defect sites of hard carbon with a wide adsorption energy distribution, producing a sloping voltage profile. In the second stage, Na ions intercalate into graphitic layers with suitable spacing to form NaC x compounds similar to the Li ion intercalation process in graphite, producing a flat low voltage plateau. The cation intercalation with a flat voltage plateau should be enhanced and the sloping region should be avoided. Guided by this knowledge, nonporous hard carbon material has been developed which has achieved high reversible capacity and Coulombic efficiency to fulfill practical application. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
语种:
英文
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Graphene-like 2D nanomaterial-based biointerfaces for biosensing applications
作者:
Zhu, Chengzhou;Du, Dan* ;Lin, Yuehe*
期刊:
Biosensors and Bioelectronics ,2017年89(Pt 1):43-55 ISSN:0956-5663
通讯作者:
Du, Dan;Lin, Yuehe
作者机构:
[Zhu, Chengzhou; Du, Dan; Lin, Yuehe; Du, D; Lin, YH] Minist Educ PR China, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;[Zhu, Chengzhou; Du, Dan; Lin, Yuehe; Du, D; Lin, YH] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.;[Zhu, Chengzhou; Du, Dan; Lin, Yuehe] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.
通讯机构:
[Du, D; Lin, YH] M;[Du, D; Lin, YH] C;Minist Educ PR China, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
关键词:
*Biointerfaces;*Electrochemical biosensors;*Fluorescent biosensors;*Graphene;*Graphene-like 2D materials
摘要:
Due to their unique structures and multifunctionalities, two-dimensional (2D) nanomaterials have aroused increasing interest in the construction of the novel biointerfaces for biosensing applications. Efforts in constructing novel biointerfaces led to exploit the more versatile and tunable graphene-like 2D nanomaterials (e.g. graphitic carbon nitride, boron nitride, transition metal dichalcogenides, and transition metal oxides) with various structural and compositional characteristics. This review highlights recent efforts in the design of graphene-like 2D nanomaterials and their derived biointerfaces and exploitation of their research on fluorescent sensors and a series of electrochemical sensors, including amperometric, electrochemiluminescence, photoelectrochemical and field-effect transistor sensors. Finally, we discuss some critical challenges and future perspectives in this field. © 2016
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英文
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Beyond sulfide-centric catalysis: Recent advances in the catalytic cyclization reactions of sulfur ylides
作者:
Lu, Liang-Qiu* ;Li, Tian-Ren;Wang, Qiang;Xiao, Wen-Jing*
期刊:
CHEMICAL SOCIETY REVIEWS ,2017年46(14):4135-4149 ISSN:0306-0012
通讯作者:
Lu, Liang-Qiu;Xiao, Wen-Jing
作者机构:
[Lu, LQ; Xiao, WJ; Lu, Liang-Qiu; Li, Tian-Ren; Xiao, Wen-Jing; Wang, Qiang] Cent China Normal Univ, Coll Chem, CCNU uOttawa Joint Res Ctr, Key Lab Pesticide & Chem Biol,Minist Educ, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.
通讯机构:
[Lu, LQ; Xiao, WJ] C;Cent China Normal Univ, Coll Chem, CCNU uOttawa Joint Res Ctr, Key Lab Pesticide & Chem Biol,Minist Educ, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.
摘要:
Great achievements in the asymmetric cyclization reactions of sulfur ylides have been reached by using chiral sulfides; however, this method usually suffers from the high loading of chiral sulfides. Over the past decade, new catalysis technologies beyond chiral sulfide-based catalysis have been gradually applied to the cyclizations of sulfur ylides. These technologies, including organocatalysis, organometallic catalysis and photocatalysis, can avoid the use of stoichiometric chiral pools and enable the development of new cyclization reactions of sulfur ylides. In this tutorial review, recent advances in this rapidly developing field will be highlighted with particular emphases on the catalytic mechanism and the development of new reactions, new reagents and new concepts. © 2017 The Royal Society of Chemistry.
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英文
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Ascorbic acid/Fe@Fe2 O3 : A highly efficient combined Fenton reagent to remove organic contaminants
作者:
Hou, Xiaojing;Huang, Xiaopeng;Ai, Zhihui* ;Zhao, Jincai;Zhang, Lizhi*
期刊:
Journal of Hazardous Materials ,2016年310:170-178 ISSN:0304-3894
通讯作者:
Ai, Zhihui;Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Hou, Xiaojing; Huang, Xiaopeng; Zhao, Jincai; Ai, ZH; Zhang, LZ; Ai, Zhihui] Cent China Normal Univ, Inst Environm Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Ai, ZH; Zhang, LZ] C;Cent China Normal Univ, Inst Environm Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词:
Alachlor;Ascorbic acid;Degradation;Fe@Fe(2)O(3) core-shell nanowires;Fenton reaction
摘要:
In this study, we demonstrate that the combination of ascorbic acid and Fe@Fe<inf>2</inf>O<inf>3</inf>core-shell nanowires (AA/Fe@Fe<inf>2</inf>O<inf>3</inf>) offers a highly efficient Fenton reagent. This combined Fenton reagent exhibited extremely high activity on the decomposition of H<inf>2</inf>O<inf>2</inf>to produce OH for the degradation of various organic contaminants, including rhodamine B, methylene blue, alachlor, atrazine, siduron, lincomycin, and chloroamphenicol. The contaminant degradation constants in the AA/Fe@Fe<inf>2</inf>O<inf>3</inf>/H<inf>2</inf>O<inf>2</inf>Fenton systems were 38-53 times higher than those in the conventional homogeneous Fenton system (Fe(II)/H<inf>2</inf>O<inf>2</inf>) at pH 3.8. Moreover, the OH generation rate constant in the AA/Fe@Fe<inf>2</inf>O<inf>3</inf>/H<inf>2</inf>O<inf>2</inf>Fenton system was 1-3 orders of magnitudes greater than those of heterogeneous Fenton systems developed with other iron-containing materials (α-FeOOH, α-Fe<inf>2</inf>O<inf>3</inf>, FeOCl, and so on). The high activity of AA/Fe@Fe<inf>2</inf>O<inf>3</inf>was attributed to the effective Fe(III)/Fe(II) cycle and the iron-ascorbate complex formation to stabilize ferrous ions with desirable and steady concentrations. During the AA/Fe@Fe<inf>2</inf>O<inf>3</inf>/H<inf>2</inf>O<inf>2</inf>Fenton process, ascorbic acid served as a reducing and complexing reagent, enabling the reuse of Fe@Fe<inf>2</inf>O<inf>3</inf>nanowires. We systematically investigated the alachlor and ascorbic acid degradation and found that they could be effectively degraded in the AA/Fe@Fe<inf>2</inf>O<inf>3</inf>/H<inf>2</inf>O<inf>2</inf>system, accompanying with 100% of dechlorination and 92% of denitrification. This study sheds light on the importance of Fe(III)/Fe(II) cycle for the design of high efficient Fenton system and provides an alternative pathway for the organic contaminants removal. ©2016 Elsevier B.V.
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英文
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Giant Enhancement of Internal Electric Field Boosting Bulk Charge Separation for Photocatalysis
作者:
Li, Jie;Cai, Lejuan;Shang, Jian;Yu, Ying;Zhang, Lizhi*
期刊:
Advanced Materials ,2016年28(21):4059-4064 ISSN:0935-9648
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Li, Jie; Cai, Lejuan; Shang, Jian] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Li, Jie; Yu, Ying] Cent China Normal Univ, Coll Phys Sci & Technol, Inst Nanosci & Nanotechnol, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词:
bulk-charge separation;doping;internal electric field;photocatalysis;water oxidation
摘要:
A study was conducted to demonstrate giant enhancement of internal electric field (IEF) boosting bulk charge separation (BCS) for photocatalysis. The study synthesized C-doped Bi3O4 Cl nanosheets with reported carbon doping strategy. These nanosheets had {001} facets on their top and bottom, {110} facets on their four lateral surfaces, and {010} facets at their four corners. Their elemental mapping images and time-resolved X-ray photoelectron spectroscopy revealed the homogeneous distribution of carbon dopants within Bi3O4.
语种:
英文
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Oxygen Vacancy Structure Associated Photocatalytic Water Oxidation of BiOCl
作者:
Li, Hao;Shang, Jian;Zhu, Huijun;Yang, Zhiping;Ai, Zhihui;...
期刊:
ACS CATALYSIS ,2016年6(12):8276-8285 ISSN:2155-5435
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Yang, Zhiping; Li, Hao; Ai, Zhihui; Shang, Jian; Zhu, Huijun] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm & Appl Chem,Coll Chem, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm & Appl Chem,Coll Chem, Wuhan 430079, Peoples R China.
关键词:
water oxidation;photocatalysis;BiOCl;oxygen vacancies;facet dependence
摘要:
A central issue in understanding photocatalytic water splitting on a stoichiometric or defective nanostructured oxide surface is its adsorption mode and related reactivity. More than just improving the adsorption of water on oxide surfaces, we demonstrate in this work that surface oxygen vacancies (OVs) also offer a possibility of activating water toward thermodynamically enhanced photocatalytic water oxidation, while the water activation state, as reflected by its capability to trap holes, strongly depends on the structures of OVs. Utilizing well-ordered BiOCl single-crystalline surfaces, we reveal that dissociatively adsorbed water on the OV of the (010) surface exhibits higher tendency to be oxidized than the molecularly adsorbed water on the OV of the (001) surface. Analysis of the geometric atom arrangement shows that the OV of the BiOCl (010) surface can facilitate barrierless O-H bond breaking in the first proton removal reaction, which is sterically hindered on the OV of the BiOCl (001) surface, and also allow more localized electrons transfer from the OV to the dissociatively adsorbed water, leading to its higher water activation level for hole trapping. These findings highlight the indispensable role of crystalline surface structure on water oxidation and may open up avenues for the rational design of highly efficient photocatalysts via surface engineering. (Chemical Equation Presented). © 2016 American Chemical Society.
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英文
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Recent advances in electrochemical biosensors based on graphene two-dimensional nanomaterials
作者:
Song, Yang;Luo, Yanan;Zhu, Chengzhou;Li, He;Du, Dan* ;...
期刊:
Biosensors and Bioelectronics ,2016年76:195-212 ISSN:0956-5663
通讯作者:
Du, Dan
作者机构:
[Du, Dan; Song, Yang; Lin, Yuehe; Luo, Yanan] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Coll Chem, Wuhan 430079, Hubei Province, Peoples R China.;[Zhu, Chengzhou; Li, He; Du, Dan; Song, Yang; Lin, Yuehe; Luo, Yanan] Washington State Univ, Dept Mech & Mat Engn, Pullman, WA 99164 USA.;[Du, Dan; Lin, Yuehe] Washington State Univ, Paul G Allen Sch Global Anim Hlth, Pullman, WA 99164 USA.;[Du, Dan] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Hubei Province, Peoples R China.
通讯机构:
[Du, Dan] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Hubei Province, Peoples R China.
关键词:
DNA sensors;Electrochemical biosensor;Enzyme-based biosensors;Graphene;Immunosensors;Two-dimensional nanomaterials
摘要:
Graphene as a star among two-dimensional nanomaterials has attracted tremendous research interest in the field of electrochemistry due to their intrinsic properties, including the electronic, optical, and mechanical properties associated with their planar structure. The marriage of graphene and electrochemical biosensors has created many ingenious biosensing strategies for applications in the areas of clinical diagnosis and food safety. This review provides a comprehensive overview of the recent advances in the development of graphene based electrochemical biosensors. Special attention is paid to graphene-based enzyme biosensors, immunosensors, and DNA biosensors. Future perspectives on high-performance graphene-based electrochemical biosensors are also discussed. © 2015 Elsevier B.V.
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英文
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Efficient Visible Light-Driven Splitting of Alcohols into Hydrogen and Corresponding Carbonyl Compounds over a Ni-Modified CdS Photocatalyst
作者:
Chai, Zhigang;Zeng, Ting-Ting;Li, Qi;Lu, Liang-Qiu;Xiao, Wen-Jing* ;...
期刊:
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY ,2016年138(32):10128-10131 ISSN:0002-7863
通讯作者:
Xu, Dongsheng;Xiao, Wen-Jing
作者机构:
[Li, Qi; Xu, Dongsheng; Chai, Zhigang] Peking Univ, Beijing Natl Lab Mol Sci, Coll Chem & Mol Engn, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100871, Peoples R China.;[Lu, Liang-Qiu; Xiao, Wen-Jing; Zeng, Ting-Ting] Cent China Normal Univ, Coll Chem, Key Lab Pesticides & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Xu, Dongsheng] P;[Xiao, Wen-Jing] C;Peking Univ, Beijing Natl Lab Mol Sci, Coll Chem & Mol Engn, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100871, Peoples R China.;Cent China Normal Univ, Coll Chem, Key Lab Pesticides & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
摘要:
Splitting of alcohols into hydrogen and corresponding carbonyl compounds has potential applications in hydrogen production and chemical industry. Herein, we report that a heterogeneous photocatalyst (Ni-modified CdS nanoparticles) could efficiently split alcohols into hydrogen and corresponding aldehydes or ketones in a stoichiometric manner under visible light irradiation. Optimized apparent quantum yields of 38%, 46%, and 48% were obtained at 447 nm for dehydrogenation of methanol, ethanol, and 2-propanol, respectively. In the case of dehydrogenation of 2-propanol, a turnover number of greater than 44-000 was achieved. To our knowledge, these are unprecedented values for photocatalytic splitting of liquid alcohols under visible light to date. Besides, the current catalyst system functions well with other aliphatic and aromatic alcohols, affording the corresponding carbonyl compounds with good to excellent conversion and outstanding selectivity. Moreover, mechanistic investigations suggest that an interface between Ni nanocrystal and CdS plays a key role in the reaction mechanism of the photocatalytic splitting of alcohol. © 2016 American Chemical Society.
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英文
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