Hydrothermal Carbon-Mediated Fenton-Like Reaction Mechanism in the Degradation of Alachlor: Direct Electron Transfer from Hydrothermal Carbon to Fe(III)
作者：
Qin, Yaxin;Zhang, Lizhi* ;An, Taicheng*
期刊：
ACS Applied Materials & Interfaces ,2017年9(20):17115-17124 ISSN：1944-8244
通讯作者：
An, Taicheng;Zhang, Lizhi
作者机构：
[An, Taicheng; Qin, Yaxin] Guangdong Univ Technol, Sch Environm Sci & Engn, Inst Environm Hlth & Pollut Control, Guangzhou Key Lab Environm Catalysis & Pollut Con, Guangzhou 510006, Guangdong, Peoples R China.;[Zhang, Lizhi; Qin, Yaxin] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[An, Taicheng] G;[Zhang, Lizhi] C;Guangdong Univ Technol, Sch Environm Sci & Engn, Inst Environm Hlth & Pollut Control, Guangzhou Key Lab Environm Catalysis & Pollut Con, Guangzhou 510006, Guangdong, Peoples R China.;Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词：
hydrothermal carbon;fenton-like reaction;Fe(III)/Fe(II) cycle;electron transfer mechanism;alachlor degradation
摘要：
As Fenton systems suffer from the undesirable Fe(III)/Fe(II) cycle, great efforts were made to realize the effective reduction of Fe(III) to Fe(II). The effects of hydrothermal carbon (HTC) on the Fe(III)/H<inf>2</inf>O<inf>2</inf>Fenton-like reaction and the subsequent degradation of alachlor in water was systematically investigated, and the results indicated that HTC could enhance alachlor degradation in Fe(III)/H<inf>2</inf>O<inf>2</inf>by promoting the Fe(III)/Fe(II) cycle via electron transfer from HTC to Fe(III) ions. The apparent alachlor degradation rate constant in the HTC-G/Fe(III)/H<inf>2</inf>O<inf>2</inf>system (7.02 ×10<sup>-2</sup>min<sup>-1</sup>) was about 3 times higher than that in the Fe(III)/H<inf>2</inf>O<inf>2</inf>system (2.25 ×10<sup>-2</sup>min<sup>-1</sup>). The electron spin resonance spectra analysis revealed that HTC consists of abundant carbon-centered persistent free radicals to act as the electron donor. Meanwhile, the hydroxyl groups on the surface of HTC also played an important role in the enhanced alachlor degradation because the decrease in the surface hydroxyl groups on HTC significantly decreased the degradation of alachlor. On the basis of these results, an Fe(III) complex with surface hydroxyl groups on HTC was proposed to favor the electron transfer from the hydroxyl groups to Fe(III), and then, the simultaneously produced Fe(II) could accelerate the catalytic decomposition of H<inf>2</inf>O<inf>2</inf>to facilitate alachlor degradation. These findings shed new light on the possible roles of carbon materials in a natural aquatic environment and provide a new pathway for environmental pollutant control and remediation of organic contaminants by HTC. ©2017 American Chemical Society.
语种：
英文
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铋系光催化剂去除环境污染物
作者：
Ding, Xing;Yang, Xianglong;Xiong, Zhongliang;Chen, Hao* ;Zhang, Lizhi*
期刊：
化学进展 ,2017年29(9):1115-1126 ISSN：1005-281X
通讯作者：
Chen, Hao;Zhang, Lizhi
作者机构：
[Ding, Xing; Yang, Xianglong; Xiong, Zhongliang; Chen, Hao] Huazhong Agr Univ, Coll Sci, Wuhan 430070, Hubei, Peoples R China.;[Zhang, Lizhi; Ding, Xing] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Chen, Hao] H;[Zhang, Lizhi] C;Huazhong Agr Univ, Coll Sci, Wuhan 430070, Hubei, Peoples R China.;Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词：
铋系半导体;可见光;光催化;环境污染物
摘要：
铋系半导体材料是近年来研究较热的一类新型光催化剂,因其具有独特的层状结构和合适的禁带宽度,而表现出了良好的太阳光催化性能,在环境污染物去除方面展现出极大的潜力。本文综述了近年来铋系光催化剂(氧化铋、硫化铋、钨酸铋、钼酸铋、钒酸铋、卤氧化铋等)在环境污染物去除方面的最新研究进展,介绍了几类常见的铋系半导体材料及其制备方法,归纳和总结了铋系光催化剂在大气净化、有机废水处理、重金属离子处理和杀菌等方面的应用,同时对今后铋系光催化剂在环境污染去除方面的应用进行了展望。
语种：
中文
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Enhanced aerobic degradation of 4-chlorophenol with iron-nickel nanoparticles
作者：
Shen, Wenjuan;Mu, Yi;Wang, Bingning;Ai, Zhihui* ;Zhang, Lizhi
期刊：
Applied Surface Science ,2017年393:316-324 ISSN：0169-4332
通讯作者：
Ai, Zhihui
作者机构：
[Wang, Bingning; Zhang, Lizhi; Mu, Yi; Shen, Wenjuan; Ai, Zhihui] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm Chem,Coll Chem, Wuhan 430079, Peoples R China.
通讯机构：
[Ai, Zhihui] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm Chem,Coll Chem, Wuhan 430079, Peoples R China.
关键词：
4-Chlorophenol;Iron-nickel bimetallic nanoparticles;Molecular oxygen activation;Reactive oxygen species
摘要：
In this study, we demonstrate that the bimetallic iron-nickel nanoparticles (nZVIN) possessed an enhanced performance in comparison with nanoscale zero-valent iron (nZVI) on aerobic degradation of 4-chlorophenol (4-CP). The 4-CP degradation rate constant in the aerobic nZVIN process (nZVIN/Air) was 5 times that in the classic nZVI counterpart system (nZVI/Air). Both reactive oxygen species measurement and inhibition experimental results suggested that hydroxyl radicals were the major active species contributed to aerobic 4-CP degradation with nZVI, on contrast, superoxide radicals predominated the 4-CP degradation in the nZVIN/Air process. High performance liquid chromatography and gas chromatography-mass spectrometer analysis indicated the intermediates of the nZVI/Air system were p-benzoquinone and hydroquinone, which were resulted from the bond cleavage between the chlorine and carbon atom in the benzene ring by hydroxyl radicals. However, the primary intermediates of 4-CP found in the nZVIN/Air system were phenol via the direct dechlorination by superoxide radicals, accompanying with the formation of chloride ions. On the base of experimental results, a superoxide radicals mediated enhancing mechanism was proposed for the aerobic degradation of 4-CP in the nZVIN/Air system. This study provides new insight into the role of bimetallic nickel on enhancing removal of organic pollutants with nZVI. © 2016 Elsevier B.V.
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 Shifted Oxygen Reduction Pathway on Fe@Fe2O3 Core-Shell Nanowires for Enhanced Reactive Oxygen Species Generation and Aerobic 4-Chlorophenol Degradation
作者：
Mu, Yi;Ai, Zhihui;Zhang, Lizhi*
期刊：
Environmental Science & Technology ,2017年51(14):8101-8109 ISSN：0013-936X
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Mu, Yi; 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：
Phosphate ions widely exist in the environment. Previous studies revealed that the adsorption of phosphate ions on nanoscale zerovalent iron would generate a passivating oxide shell to block reactive sites and thus decrease the direct pollutant reduction reactivity of zerovalent iron. Given that molecular oxygen activation process is different from direct pollutant reduction with nanoscale zerovalent iron, it is still unclear how phosphate ions will affect molecular oxygen activation and reactive oxygen species generation with nanoscale zerovalent iron. In this study, we systematically studied the effect of phosphate ions on molecular oxygen activation with Fe@Fe2O3 nanowires, a special nanoscale zerovalent iron, taking advantages of rotating ring disk electrochemical analysis. It was interesting to find that the oxygen reduction pathway on Fe@Fe2O3 nanowires was gradually shifted from a four-electron reduction pathway to a sequential one-electron reduction one, along with increasing the phosphate ions concentration from 0 to 10 mmol·L-1. This oxygen reduction pathway change greatly enhanced the molecular oxygen activation and reactive oxygen species generation performances of Fe@Fe2O3 nanowires, and thus increased their aerobic 4-chlorophenol degradation rate by 10 times. These findings shed insight into the possible roles of widely existed phosphate ions in molecular oxygen activation and organic pollutants degradation with nanoscale zerovalent iron. © 2017 American Chemical Society.
语种：
英文
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生物启发的光催化氮气还原新模型
作者：
李浩;张礼知
作者机构：
[李浩; 张礼知] 华中师范大学化学学院
会议名称：
第九届全国环境催化与环境材料学术会议-助力两型社会快速发展的环境催化与环境材料
会议时间：
2015-11-2
会议地点：
中国湖南长沙
会议论文集名称：
第九届全国环境催化与环境材料学术会议-助力两型社会快速发展的环境催化与环境材料会议论文集(NCECM 2015)
摘要：
<正>尽管Haber-Bosch过程是人工固氮的最主要的途径,但其高能耗的特性一直在驱使人们寻找更加温和的固氮途径。而生物固氮则可以通过固氮酶在温和条件下实现固氮反应,一个很重要的原因就是其含有一个非常重要的N2吸附活化位点,即钼铁辅因子。1本工作从生物固氮的基本原理出发,希望在半导体表面引入氧空位来模拟钼铁辅因子,旨在对吸附N2进行一定程度的活化,从而降低其被光催化还原所需要的能量。
语种：
中文
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In Situ Carbon Homogeneous Doping on Ultrathin Bismuth Molybdate: A Dual-Purpose Strategy for Efficient Molecular Oxygen Activation
作者：
Wang, Shengyao;Ding, Xing;Zhang, Xuehao;Pang, Hong;Hai, Xiao;...
期刊：
Advanced Functional Materials ,2017年27(47):1703923- ISSN：1616-301X
通讯作者：
Chen, Hao;Ye, Jinhua
作者机构：
[Ding, Xing; Wang, Shengyao; Chen, Hao; Zhang, Xuehao] Huazhong Agr Univ, Key Lab Environm Correlat Dietol, Minist Educ, Coll Sci, Wuhan 430070, Hubei, Peoples R China.;[Ye, Jinhua; Pang, Hong; Hai, Xiao; Wang, Shengyao; Zhou, Wei; Song, Hui] Natl Inst Mat Sci, Int Ctr Mat Nanoarchitecton WPI MANA, 1-1 Namiki, Tsukuba, Ibaraki 3050044, Japan.;[Ye, Jinhua; Pang, Hong; Hai, Xiao; Song, Hui] Hokkaido Univ, Grad Sch Chem Sci & Engn, Sapporo, Hokkaido 0600814, Japan.;[Zhang, Lizhi; Zhan, Guangming] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Ye, Jinhua] Tianjin Univ, Sch Mat Sci & Engn, TU NIMS Int Collaborat Lab, Tianjin 300072, Peoples R China.
通讯机构：
[Chen, Hao; Ye, Jinhua] H;[Ye, Jinhua] N;[Ye, Jinhua] T;Huazhong Agr Univ, Key Lab Environm Correlat Dietol, Minist Educ, Coll Sci, Wuhan 430070, Hubei, Peoples R China.;Natl Inst Mat Sci, Int Ctr Mat Nanoarchitecton WPI MANA, 1-1 Namiki, Tsukuba, Ibaraki 3050044, Japan.
关键词：
Bi2MoO6;C-doping;molecular oxygen activation;NO removal;ultrathin 2D materials
摘要：
Solar-driven activation of molecular oxygen, which harnesses light to produce reactive oxygen species for the removal of pollutants, is the most green and low-cost approach for environmental remediation. The energy coupling between photons, excitons, and oxygen is the crucial step in this reaction and still remains a challenge. In this study, a dual-purpose strategy for enhanced molecular oxygen activation is established by in situ carbon homogeneous doping on ultrathin Bi2MoO6 nanosheets for the first time. The C-doped ultrathin 2D material exhibits an enlarged bandgap straddling the electrochemical potential of O2 /•O2 − and H2O /•OH, without any attenuation of light absorption. An internal electric field and shortened carrier-transportation distance are also found in the longitude orientation of the nanosheets ([001] axis), leading to a higher density of effective photogenerated carriers localized on the exposed {001} surface. As applied for the nitric oxide removal, the reactive rate over the ultrathin C-doped Bi2MoO6 nanosheets is 4.3 times higher than that over the bulk counterparts as a result of the increasing reactive oxygen species. This new proof-of-concept strategy not only realizes the band structure engineering and charge transportation regulation but also paves a new way to construct highly efficient photocatalytic materials. © 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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Ascorbate-Promoted Surface Iron Cycle for Efficient Heterogeneous Fenton Alachlor Degradation with Hematite Nanocrystals
作者：
Huang, Xiaopeng;Hou, Xiaojing;Jia, Falong;Song, Fahui;Zhao, Jincai;...
期刊：
ACS Applied Materials & Interfaces ,2017年9(10):8751-8758 ISSN：1944-8244
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Hou, Xiaojing; Huang, Xiaopeng; Zhao, Jincai; Jia, Falong; Song, Fahui] Cent China Normal Univ, Minist Educ, Coll Chem, 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, Coll Chem, Inst Environm Chem,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
关键词：
surface iron cycle;heterogeneous Fenton oxidation;alachlor degradation;ascorbate ions;hematite nanocrystals
摘要：
This study reports the H2O2 activation with different hematite nanocrystals and ascorbate ions for the herbicide alachlor degradation at pH 5. We found that hematite nanoplates (HNPs) exposed with {001} facets exhibited better catalytic performance than hematite nanocubes (HNCs) exposed with {012} facets, which was attributed to the formation of inner-sphere iron-ascorbate complexes on the hematite facets. The 3-fold undercoordination Fe cations of {001} facet favors the formation of inner-sphere iron-ascorbate complexes, while the 5-fold undercoordination Fe cations of {012} facet has stereo-hindrance effect, disfavoring the complex formation. The surface area normalized alachlor degradation rate constant (23.3 × 10-4 min-1 L m-2) of HNPs-ascorbate Fenton system was about 2.6 times that (9.1 × 10-4 min-1 L m-2) of HNCs-ascorbate counterpart. Meanwhile, the 89.0% of dechlorination and 30.0% of denitrification in the HNPs-ascorbate Fenton system were also significantly higher than those (60.9% and 13.1%) of the HNCs-ascorbate one. More importantly, the reductive dissolution of hematite by ascorbate was strongly coupled with the subsequent H2O2 decomposition by surface bound ferrous ions through surface iron cycle on the hematite facets in the hematite-ascorbate Fenton systems. This coupling could significantly inhibit the conversion of surface bound ferrous ions to dissolved ones, and thus account for the stability of hematite nanocrystals. This work sheds light on the internal relationship between iron geochemical cycling and contaminants degradation, and also inspires us to utilize surface iron cycle of widely existent hematite for environmental remediation. © 2017 American Chemical Society.
语种：
英文
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Efficient electroreduction of CO2 on bulk silver electrode in aqueous solution via the inhibition of hydrogen evolution
作者：
Quan, Fengjiao;Xiong, Mubing;Jia, Falong* ;Zhang, Lizhi
期刊：
Applied Surface Science ,2017年399:48-54 ISSN：0169-4332
通讯作者：
Jia, Falong
作者机构：
[Quan, Fengjiao; Zhang, Lizhi; Xiong, Mubing; Jia, Falong] Cent China Normal Univ, Inst Environm Chem, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构：
[Jia, Falong] C;Cent China Normal Univ, Inst Environm Chem, Coll Chem, Wuhan 430079, Peoples R China.
关键词：
Carbon dioxide;Electrocatalytic reduction;Hydrogen evolution;Silver electrode
摘要：
Electrochemical CO 2 reduction provides a desirable pathway to convert greenhouse gas into useful chemicals. It is a great challenge to reduce CO 2 efficiently in aqueous solution, especially on commercial bulk metal electrodes. Here, we report substantial improvement in CO 2 reduction on bulk silver electrode through the introduction of ionic surfactant in aqueous electrolyte. The hydrogen evolution on the electrode surface is greatly suppressed by the surfactant, while the catalytic ability of silver towards CO 2 reduction is maintained. The Faradaic efficiency for CO is greatly enhanced from 50% to 95% after the addition of this low-cost surfactant. This study may provide new pathways towards efficient CO 2 reduction through the inhibition of proton reduction. © 2016
语种：
英文
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Photocatalytic performance of different exposed crystal facets of BiOCl
作者：
Li, Hao;Zhang, Lizhi*
期刊：
Current Opinion in Green and Sustainable Chemistry ,2017年6:48-56 ISSN：2452-2236
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Li, Hao] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Inst Environm Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
摘要：
Bismuth oxychloride (BiOCl) is a typical V–VI–VII ternary oxide material of low toxicity and high earth abundance nature. The past ten years have witnessed tremendous efforts in utilizing BiOCl as a versatile catalysts for photocatalytic applications, including pollutant removal, water splitting, CO2 reduction, N2 fixation and organic transformation. Remarkably, photocatalytic performance of BiOCl shows high dependency on its exposed crystal facets. In this brief review, we highlight the recent progress on the photocatalysis of different exposed crystal facets of BiOCl, focusing on the facet-dependent internal electric field manipulation, sensitization, carbon doping, and plasmonic hot carriers utilization. Understanding of the facet-dependent photocatalysis of BiOCl will offer new guidelines for the rational design of novel catalysts. © 2017
语种：
英文
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Photochemistry of Hydrochar: Reactive Oxygen Species Generation and Sulfadimidine Degradation
作者：
Chen, Na;Huang, Yahui;Hou, Xiaojing;Ai, Zhihui;Zhang, Lizhi*
期刊：
Environmental Science & Technology ,2017年51(19):11278-11287 ISSN：0013-936X
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Huang, Yahui; Hou, Xiaojing; Chen, Na; Ai, Zhihui] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
摘要：
Biochar, mainly including pyrochar produced via pyrolysis of biomass at moderate temperatures of 350-700 °C and hydrochar formed by hydrothermal carbonization in a range of 150-350 °C, has received increasing attention because of its significant environmental impacts. It is known that pyrochar can generate reactive oxygen species even in the dark owing to the presence of persistent free radicals, but hydrochar is far less studied. In this study, we systematically investigate the photochemistry of hydrochar and check its effects on the sulfadimidine degradation. Different from pyrochar derived from the same biomass, hydrochar could generate much more H2O2 and •OH under daylight irradiation, which could enhance the sulfadimidine degradation rate six times more than that found in the dark. Raman spectroscopy, Fourier transform infrared spectroscopy, electron paramagnetic resonance, and X-ray photoelectron spectroscopy were employed to elucidate this interesting phenomenon. Characterization results revealed that the higher reactive oxygen species generation ability of hydrochar under solar light irradiation was attributed to its abundant photoactive surface oxygenated functional groups. This study clarifies the differences of pyrochar and hydrochar on organic pollutant degradation, and also sheds light on environmental effects of hydrochar. © 2017 American Chemical Society.
语种：
英文
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可见光下BiOCl氧空位浓度调控的胺到亚胺的选择性氧化
作者：
毛成梁;李浩;商健;张礼知
作者机构：
[毛成梁; 李浩; 商健; 张礼知] 农药与化学生物学教育部重点实验室华中师范大学化学学院
会议名称：
第九届全国环境催化与环境材料学术会议-助力两型社会快速发展的环境催化与环境材料
会议时间：
2015-11-2
会议地点：
中国湖南长沙
会议论文集名称：
第九届全国环境催化与环境材料学术会议-助力两型社会快速发展的环境催化与环境材料会议论文集(NCECM 2015)
摘要：
<正>亚胺作为药物和精细化学品等领域重要的合成中间体,引起了人们广泛的合成兴趣。半导体光催化着眼于利用空气中的分子氧将胺氧化为亚胺并且已经取得了较好效果。然而在制药工业中,氧化反应由于存在原子利用率低、反应选择性差等问题而很少被使用。因而理解光催化高选择性的机理就有了重要意义。
语种：
中文
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铜离子促进Fe@Fe_2O_3纳米线活化分子氧降解阿特拉津的研究
作者：
Jia Falong;Liu Juan;Zhang Lizhi*
期刊：
化学学报 ,2017年75(6):602-607 ISSN：0567-7351
通讯作者：
Zhang Lizhi
作者机构：
[Zhang Lizhi; Liu Juan; Jia Falong] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Zhang Lizhi] C;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
关键词：
阿特拉津;降解;Fe@Fe_2O_3纳米线;分子氧活化;铜离子
摘要：
阿特拉津是一种持久性含氯有机污染物,难以生物降解,因此有必要开发高效技术清除环境中残留的阿特拉津.近来纳米铁材料的发展为降解阿特拉津提供了一种可供选择的新方法,但降解过程中纳米铁活性逐渐减弱的问题仍需改进.本论文研究了铜离子(Cu~(2+))存在条件下Fe@Fe_2O_3纳米线活化分子氧降解阿特拉津的过程,并探讨了Cu~(2+)的作用机理.研究结果表明,少量Cu~(2+)的存在就可以显著促使Fe@Fe_2O_3生成溶解态Fe(II),从而有助于分子氧活化并产生更多·OH等活性氧物种.在降解过程中,阿特拉津首先被氧化,进而发生脱氯上羟基反应、侧链氧化以及脱侧链反应.
语种：
中文
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纳米零价铁活化分子氧原理及降解有机污染物性能增强策略
作者：
Mu Yi;Jia Falong;Ai Zhihui* ;Zhang Lizhi*
期刊：
化学学报 ,2017年75(6):538-543 ISSN：0567-7351
通讯作者：
Ai Zhihui;Zhang Lizhi
作者机构：
[Zhang Lizhi; Jia Falong; Ai, ZH; Zhang, LZ; Mu Yi; Ai Zhihui] Cent China Normal Univ, Inst Appl & Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Ai, ZH; Zhang, LZ] C;Cent China Normal Univ, Inst Appl & Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
关键词：
纳米零价铁;分子氧活化;活性氧物种;高级氧化技术
摘要：
纳米零价铁直接还原降解有机污染物运行长效性差,且不能矿化有机污染物.利用纳米零价铁还原活化分子氧生成活性氧物种可以氧化甚至矿化有机污染物.在最近的研究中,作者提出了纳米零价铁活化分子氧的双途径机理,即铁核电子转移到氧化铁壳表面的双电子还原活化分子氧途径和氧化铁表面结合态亚铁离子的单电子还原活化分子氧途径,阐释了纳米零价铁核壳结构依赖的分子氧活化降解有机污染物性能机制及性能增强策略.证实在纳米零价铁活化分子氧体系添加少量亚铁离子能在零价铁表面形成更多的结合态亚铁,显著增强纳米铁表界面活性氧物种生成量;同时,在纳米零价铁活化分子氧体系中引入少量有机或无机配体亦可提高活性氧物种产生效率,从而增强有机污染物降解性能.最后讨论了典型环境因素如pH值、共存离子、天然有机物等影响纳米零价铁活化分子氧降解有机污染物性能的规律.
语种：
中文
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Nitrogen dioxide radicals mediated mineralization of perfluorooctanoic acid in aqueous nitrate solution with UV irradiation
作者：
Li, Aimin;Zhang, Zhe;Li, Peifeng;Cai, Lejuan;Zhang, Lizhi* ;...
期刊：
Chemosphere ,2017年188(Dec.):367-374 ISSN：0045-6535
通讯作者：
Zhang, Lizhi;Gong, Jingming
作者机构：
[Zhang, Lizhi; Gong, Jingming; Zhang, LZ; Gong, JM; Li, Aimin; Zhang, Zhe; Li, Peifeng; Cai, Lejuan] Cent China Normal Univ, Coll Chem, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Zhang, LZ; Gong, JM] C;Cent China Normal Univ, Coll Chem, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词：
Nitrogen dioxide radicals;Photodegradation;Perfluorooctanoic acid;Nitrate;Hydroxyl radical scavenger
摘要：
Effective decomposition of perfluorooctanoic acid (PFOA) has received increasing attention in recent years because of its global occurrence and resistance to most conventional treatment processes. In this study, the complete mineralization of PFOA was achieved by the UV-photolysis of nitrate aqueous solution (UV/Nitrate), where the in-situ generated nitrogen dioxide radicals (center dot NO2) efficiently mediated,the degradation of PFOA. In particular, when the twinborn hydroxyl radicals were scavenged, the production of more center dot NO2 radicals realized the complete mineralization of PFOA. DFT calculations further confirm the feasibility of PFOA removal with center dot NO2. Near-stoichiometric equivalents of fluoride released rather than the related intermediates were detected in solution after decomposition of PEOA, further demonstrating the complete degradation of PFOA. Possible PFOA degradation pathways were proposed on the basis of experimental results. This work offers an efficient strategy for the complete mineralization of per fluorinated chemicals, and also sheds light on the indispensable roles of nitrogen dioxide radicals for environmental pollutants removal. (C) 2017 Elsevier Ltd. All rights reserved.
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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Electrospun template directed molecularly imprinted nanofibers incorporated with BiOI nanoflake arrays as photoactive electrode for photoelectrochemical detection of triphenyl phosphate
作者：
Yang, Xiaomin;Li, Xin;Zhang, Lizhi;Gong, Jingming*
期刊：
Biosensors and Bioelectronics ,2017年92:61-67 ISSN：0956-5663
通讯作者：
Gong, Jingming
作者机构：
[Zhang, Lizhi; Gong, Jingming; Yang, Xiaomin; Li, Xin] Cent China Normal Univ, Minist Educ, Coll Chem, Inst Appl & Environm Chem,Key Lab Pesticide & Che, Wuhan 430079, Peoples R China.
通讯机构：
[Gong, Jingming] C;Cent China Normal Univ, Minist Educ, Coll Chem, Inst Appl & Environm Chem,Key Lab Pesticide & Che, Wuhan 430079, Peoples R China.
关键词：
*Electrospinning;*Electrospun template directed molecular imprinting technique;*Photoelectrochemical sensor;*Triphenyl phosphate
摘要：
Triphenyl Phosphate (TPhP), as a typical model of organophosphorus flame retardants (OPFRs), has been regarded as emerging environmental contaminants of health concern. In this study, a rapid and highly sensitive visible-light-response PEC sensor has been developed for the detection of Triphenyl Phosphate (TPhP) using electrospun template directed molecularly imprinted nanofibers modified BiOI nanoflake arrays (BiOINFs) as a photoactive electrode. The molecularly imprinted electrospun nanofibers (labeled as MI-ESNFs) were carefully characterized by scanning electron microscopy (SEM), UV spectra, FTIR spectra measurements and various electrochemical techniques. Under the optimized experimental conditions, the photoelectrochemical response was linearly proportional to the logarithm value of TPhP concentrations in the range of 0.01ngmL−1 to 500ngmL−1. Meanwhile, the sensor exhibited high selectivity and stability. © 2017 Elsevier B.V.
语种：
英文
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Efficient removal of bromate with core-shell Fe@Fe2O3 nanowires
作者：
Shen, Wenjuan;Lin, Fangjing;Jiang, Xu;Li, Hefei;Ai, Zhihui* ;...
期刊：
Chemical Engineering Journal ,2017年308:880-888 ISSN：1385-8947
通讯作者：
Ai, Zhihui
作者机构：
[Zhang, Lizhi; Li, Hefei; Lin, Fangjing; Jiang, Xu; Shen, Wenjuan; Ai, Zhihui] Cent China Normal Univ, Inst Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构：
[Ai, Zhihui] C;Cent China Normal Univ, Inst Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
关键词：
Bromate;Molecular oxygen;Removal mechanism;Surface bound Fe(II);[email protected]2O3 nanowires
摘要：
In this study, we systematically investigated the removal of bromate (BrO3−) with core-shell Fe@Fe2O3 nanowires at neutral pH, especially the effects of surface bound ferrous ions and molecular oxygen. In the presence of Fe@Fe2O3 nanowires, bromate was reduced to Br− efficiently with the generation of HOBr intermediates. Bromide species analyses and nanowires characterizations indicated that surface bound ferrous ions of core-shell Fe@Fe2O3 nanowires could effectively promote the BrO3− removal. Meanwhile, molecular oxygen competed electrons from both Fe2+ and Fe0 to generate reactive oxygen species of [rad]O2−, H2O2, and [rad]OH during the bromate removal process. Among the generated reactive oxygen species, [rad]O2− and H2O2 favored of bromate removal, but [rad]OH inhibited. We proposed a bromate removal mechanism with core-shell Fe@Fe2O3 nanowires, which suggested that the effect of surface bound Fe(II) and molecular oxygen was taken into consideration when using nZVI for bromate remediation in waters. This study can not only deepen our understanding on the bromate removal with zero valent iron, and also shed light on the design of high performance bromate removal materials. © 2016
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.
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英文
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