作者： Mao, Chengliang;Yu, Linghao;Li, Jie;Zhao, Jincai;Zhang, Lizhi*

期刊： Applied Catalysis B: Environmental,2018年224:612-620 ISSN：0926-3373

通讯作者： Zhang, Lizhi

作者机构： [Yu, Linghao; Zhang, Lizhi; Mao, Chengliang; Zhao, Jincai; Li, Jie] 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.

关键词： Ammonia synthesis;Disordered titanium oxide;Incorporated hydrogen;LSPR;Oxygen vacancies;Photocatalysis;Solar thermal catalysis

摘要： Haber–Bosch thermal ammonia synthesis is of energy-intensive nature. Using solar energy for ammonia synthesis is idealized for both energy and environment problems, but remains great challenges. Generally, the diffuse solar flux and inefficient utilization cannot meet the energy demand for NH3 production. Here we develop a solar thermal avenue, realizing highly efficient solar ammonia synthesis over K/Ru/TiO2-xHx. The supported Ru is efficient for nitrogen activation because of the electron donation from TiO2-xHx and free from H2 poisoning, because the interfacial TiO2-xHx accepts H atoms from Ru and then delivers them to the Ru activated N2 to form Ti-NHx (x = 1–3) even at room temperature. When only irradiated with sunlight, this catalyst absorbs sunlight in the whole UV–vis-NIR region and reaches 360 °C by its plasmonic behavior, exhibiting a Haber–Bosch thermocatalysis-comparable NH3 generation rate. This solar thermal approach with K/Ru/TiO2-xHx provides a promising renewable way for ammonia synthesis. © 2017 Elsevier B.V.

语种： 英文

作者： Shen, Wenjuan;Wang, Bingning;Jia, Falong;Ai, Zhihui*;Zhang, Lizhi*

期刊： Chemical Engineering Journal,2018年335:720-727 ISSN：1385-8947

通讯作者： Ai, Zhihui;Zhang, Lizhi

作者机构： [Wang, Bingning; Zhang, Lizhi; Ai, ZH; Zhang, LZ; Shen, Wenjuan; Jia, Falong; Ai, Zhihui] Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Hubei, Peoples R China.

通讯机构： [Ai, ZH; Zhang, LZ] C;Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Hubei, Peoples R China.

关键词： Active hydrogen;Atrazine;Core-shell [email protected]2O3 nanowires;Degradation;S-triazine ring

摘要： In general, the final product of atrazine (ATR) degradation by reactive oxygen species is cyanuric acid bearing a stable s-triazine ring, which is not further oxidized under mild conditions. In this study, we demonstrate that the presence of Ni(II) can increase the aerobic ATR degradation rate of core–shell Fe@Fe2O3 nanowires (CSFN) by 6 times and also achieve the cleavage of recalcitrant s-triazine ring. The cleavage of s-triazine ring in this novel system was confirmed by the measurements of formic acid and nitrite acid. On the basis of experimental results, a feasible mechanism was proposed to account for the promoted aerobic ATR degradation and the facile s-triazine ring cleavage as follows. First, Ni(II) adsorbed on the surface of CSFN was reduced to nickel metal, which favored the generation of active hydrogen (•H). The in-situ generated •H then reduced ATR to 4-ethylamino-6-isopropylamino-1,3,5-triazine intermediate of easy ring opening property, rather than the recalcitrant cyanuric acid. Finally, this ATR degradation pathway change promoted the aerobic ATR degradation and benefited the s-triazine ring cleavage. This study clarifies the importance of degradation pathway on the ring-opening of organic pollutants, and also provides a mild method to remove s-triazine herbicides with molecular oxygen and zero-valent iron. © 2017 Elsevier B.V.

语种： 英文

作者： Li, Hao;Shang, Huan;Cao, Xuemei;Yang, Zhiping;Ai, Zhihui*;...

期刊： Environmental Science & Technology,2018年52(15):8659-8665 ISSN：0013-936X

通讯作者： Ai, Zhihui;Zhang, Lizhi

作者机构： [Zhang, Lizhi; Yang, Zhiping; Shang, Huan; Li, Hao; Ai, Zhihui; Ai, ZH; Zhang, L; Cao, Xuemei] Cent China Normal Univ, Inst Appl & Environm Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.

通讯机构： [Ai, ZH; Zhang, L] C;Cent China Normal Univ, Inst Appl & Environm Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.

摘要： It is of a great challenge to seek for semiconductor photocatalysts with prominent reactivity to remove kinetically inert dilute NO without NO2 emission. In this study, complete visible light NO oxidation mediated by O2 is achieved over a defect-engineered BiOCl with selectivity exceeding 99%. Well-designed oxygen vacancies on the prototypical (001) surface of BiOCl favored the possible formation of geometric-favorable superoxide radicals (•O2 -) in a side-on bridging mode under ambient condition, which thermodynamically suppressed the terminal end-on •O2 - associated NO2 emission in case of higher temperatures, and thus selectively oxidized NO to nitrate. These findings can help us to understand the intriguing surface chemistry of photocatalytic NO oxidation and design highly efficient NOx removal systems. © 2018 American Chemical Society.

语种： 英文

作者： Yang, Weiwei;Chen, Min;Xiao, Wen;Guo, Yanbing*;Ding, Jun;...

期刊： Environmental Science & Technology,2018年52(24):14110-14118 ISSN：0013-936X

通讯作者： Guo, Yanbing

作者机构： [Zhang, Lizhi; Yang, Weiwei; Guo, Yanbing] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[He, Hong; Chen, Min] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100085, Peoples R China.;[Ding, Jun; Xiao, Wen] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 119260, Singapore.

通讯机构： [Guo, Yanbing] 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： In this study, molecular insights into NO-promoted SO2 oxidation on model TiO2 with well-defined (001), (010), and (101) facets are investigated in the laboratory. The adsorbed SO2 is significantly promoted to transform into sulfate by the coexisting NO on the three facets. The appearance of active oxygen species indicates an active oxygen species-initiated NO oxidation. The resulting NO2 acts as an oxidant to convert adsorbed sulfite on hydroxyls to sulfate species. The (101) facet presents the best performance in the NO-promoted sulfate formation possibly owing to its desirable structure to accommodate SO3 2-, NO2, and molecular water. The uptake coefficient (γt) of SO2 increases by the coexistence of NO on the (001) facet at 0% RH and is relative humidity (RH) dependent, which first decreases from 0% RH to 32% RH but then increases in the range of 32%-80% RH. The probable explanation is the combined contribution of the blocking effect of water and the hydration of SO2. The finding in this study provides insight into the possibility of its occurrence on common mineral dusts and requires further investigation. Copyright © 2018 American Chemical Society.

语种： 英文

作者： 刘伟;艾智慧;张礼知

作者机构： [刘伟; 艾智慧; 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>洛克沙胂作为一种多功能的有机砷添加剂,因其具有促生长、抗球虫、治痢疾、沉积色素等作用,被广泛应用于家禽或生猪养殖产业。但是,畜禽自身对洛克沙胂吸收很少,大部分会经粪尿排出体外。经光照、微生物等作用,有机砷很容易转化为无机砷并流入自然水体,从而导致地下水砷污染。为此,世界卫生组织及欧盟等组织规定其在饮用水中最高浓度不超

语种： 中文

作者： Ding, Xing;Wang, Shengyao;Shen, Wanqiu;Mu, Yi;Wang, Li;...

期刊： Water Research,2017年112:9-18 ISSN：0043-1354

通讯作者： Zhang, Lizhi;Chen, Hao

作者机构： [Zhang, Lizhi; Wang, Li; Ding, Xing; Shen, Wanqiu; Mu, Yi] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Ding, Xing; Wang, Shengyao; Chen, Hao] Huazhong Agr Univ, Coll Sci, Wuhan 430070, Peoples R China.;[Wang, Li] Hubei Engn Univ, Coll Chem & Mat Sci, Xiaogan 432000, Peoples R China.

通讯机构： [Zhang, Lizhi] C;[Chen, Hao] H;Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;Huazhong Agr Univ, Coll Sci, Wuhan 430070, Peoples R China.

关键词： *Atrazine;*Boron-doped diamond;*Electrochemical advanced oxidation;*Fe@Fe(2)O(3)/ACF electrode;*Fenton

摘要： In this study, an electrochemical/electro-Fenton oxidation (EC/EF) system was designed to degrade atrazine, by utilizing boron-doped diamond (BDD) and Fe@Fe2O3 core-shell nanowires loaded active carbon fiber (Fe@Fe2O3/ACF) as the anode and the cathode, respectively. This EC/EF system exhibited much higher degradation rate, decholorination and mineralization efficiency of atrazine than the electrochemical (EC) and electrochemical/traditional electro-Fenton (EC/TEF) oxidation counterpart systems without Fe@Fe2O3 core-shell nanowires. Active species trapping experiment revealed that Fe@Fe2O3 could activate molecular oxygen to produce more OH through Fenton reaction, which favored the atrazine degradation. High performance liquid chromatography, high performance liquid chromatography-mass spectrometry and gas chromatography-mass spectrometry were applied to probe the decomposition and mineralization of atrazine during this novel EC/EF process, which revealed that two intermediates of triazinons (the isomerization of hydroxylated atrazine) were generated during the electrochemical/electro-Fenton oxidation of atrazine in the presence of Fe@Fe2O3 core-shell nanowires. The experimental and theoretical calculation results suggested that atrazine might be degraded via a triazinon ring opening mechanism, while the presence of Fe@Fe2O3 notably accelerated the decholorination process, and produced more hydroxylated products to promote the generation of trazinons and the subsequent ring cleavage as well as the final complete mineralization. This work provides a deep insight into the triazine ring opening mechanism and the design of efficient electrochemical advanced oxidation technologies (EAOTs) for persistent organic pollutant removal.

语种： 英文

作者： Huang, Xiaopeng;Hou, Xiaojing;Song, Fahui;Zhao, Jincai;Zhang, Lizhi*

期刊： Journal of Physical Chemistry C,2017年121(2):1113-1121 ISSN：1932-7447

通讯作者： Zhang, Lizhi

作者机构： [Zhang, Lizhi; Hou, Xiaojing; Huang, Xiaopeng; Zhao, Jincai; Song, Fahui] 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： The interaction between ascorbate and hematite facets was systematically investigated with attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy, density functional theory (DFT) calculation, and kinetics model. Results of ATR-FTIR spectroscopy and DFT calculation suggested formation of nonprotonated inner-sphere bidentate mononuclear and monodentate mononuclear iron-ascorbate complexes on the hematite {001} and {012} facets, respectively. The estimated reductive dissolution rate constants at pH 5.0 were (4.04 &plusmn;0.16) &times;10^-4and (1.59 &plusmn;0.14) &times;10^-4min^-1for hematite nanoplates and nanocubes, respectively, indicating that the bidentate mononuclear iron-ascorbate complexes on the {001} facets favored the hematite reductive dissolution process than the monodentate mononuclear iron-ascorbate counterparts on the {012} facets. These results also revealed that the hematite facet reduction with ascorbate was strongly dependent on the iron-ascorbate complexes formed on the hematite facets. This study provides new insights into the reductive interaction between ascorbate and hematite facets and also shed light on the environmental effects of hematite at the atomic level. &copy;2017 American Chemical Society.

语种： 英文

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

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

作者： 张礼知;张伟贤

期刊： 化学学报,2017年75(6):519-520 ISSN：0567-7351

作者机构： [张礼知] Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan, 430079, China;[张伟贤] State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai, 200092, China

关键词： 环境化学;大气气溶胶;氧化还原;电子受体;零价铁;天然水体;电子供体;生物利用度;动植物体;重金属去除

摘要： <正>铁是地壳元素中丰度第四的过渡金属元素,广泛存在于大气气溶胶、天然水体、土壤和动植物体内.更为重要的是,铁易发生氧化还原反应,在生物地球化学循环过程中扮演着极其重要的角色.此外,铁拥有π特征的d轨道电子使其很容易与C、O、N和S等元素形成配合物,是绝大多数生物的电子供体或电子受体.自然界中,铁的存在形态以及生物利用度与体系的氧化还原

语种： 中文

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 &times;10^-2min^-1) was about 3 times higher than that in the Fe(III)/H<inf>2</inf>O<inf>2</inf>system (2.25 &times;10^-2min^-1). 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. &copy;2017 American Chemical Society.

语种： 英文

作者： 刘伟;艾智慧;张礼知

作者机构： 华中师范大学化学学院农药与化学生物学教育部重点实验室

会议名称： 中国化学会第28届学术年会

会议时间： 20120413

会议地点： 中国四川成都

会议论文集名称： 中国化学会第28届学术年会第2分会场摘要集

关键词： 泡沫镍;三维电极;电Fenton;超氧负离子

语种： 中文

作者： Tian, Yu;Shen, Wenjuan;Jia, Falong;Ai, Zhihui*;Zhang, Lizhi*

期刊： Chemical Engineering Journal,2017年330:1075-1081 ISSN：1385-8947

通讯作者： Ai, Zhihui;Zhang, Lizhi

作者机构： [Zhang, Lizhi; Ai, ZH; Zhang, LZ; Shen, Wenjuan; Tian, Yu; Jia, Falong; Ai, Zhihui] Cent China Normal Univ, Inst Environm & Appl 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 Environm & Appl Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.

关键词： Atrazine;Cleavage of s-triazine ring;Photochemical;Sulfite

摘要： Regarding the abundant solar energy on the earth, photochemical method is the most attractive approach for the decomposition of atrazine pollutant which is widely existed in surface water. In this study, we report that the presence of sulfite can alter the photochemical atrazine degradation pathway to cleave its s-triazine ring. Density functional theory calculation results first suggested that a reductive process might be highly possible to break the s-triazine ring of atrazine by comparing the highest occupied molecular orbital-lowest unoccupied molecular orbital energy gap values of six possible atrazine degradation intermediates. The subsequent experimental results reveal that the presence of sulfite shifted a direct atrazine hydroxylated dechlorination pathway to an indirect photo-degradation route with the aid of hydrated electrons and hydrogen atoms, which were produced from the photolysis of sulfite solution under UV irradiation. This rational degradation pathway change increased the atrazine degradation and dechlorination rates by 4.3 times, and also effectively cleaved s-triazine ring, as confirmed by the generation of ammonium ions and small molecule acids during the degradation of 2,4-diamino-1,3,5-triazine with this sulfite promoted photochemical reduction process. This study provides a mild strategy to completely mineralize atrazine, and also sheds light on how the degradation pathway could affect the s-triazine ring cleavage. © 2017 Elsevier B.V.

语种： 英文

作者： Liu, Wei;Ai, Zhihui;Dahlgren, Randy A.;Zhang, Lizhi*;Wang, Xuedong*

期刊： Chemical Engineering Journal,2017年330:1232-1239 ISSN：1385-8947

通讯作者： Wang, Xuedong;Zhang, Lizhi

作者机构： [Liu, Wei; Dahlgren, Randy A.; Wang, Xuedong] Wenzhou Med Univ, Key Lab Watershed Sci & Hlth Zhejiang Prov, Wenzhou 325035, Peoples R China.;[Zhang, Lizhi; Liu, Wei; Ai, Zhihui] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm Chem,Coll Chem, Wuhan 430079, Hubei, Peoples R China.

通讯机构： [Wang, Xuedong] W;[Zhang, Lizhi] C;Wenzhou Med Univ, Key Lab Watershed Sci & Hlth Zhejiang Prov, Wenzhou 325035, Peoples R China.;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm Chem,Coll Chem, Wuhan 430079, Hubei, Peoples R China.

关键词： Adsorption/reduction;Effect of acidity;Magnetic Fe3S4 nanosheets;Roxarsone;Structural sulfide

摘要： Roxarsone (ROX) is an organoarsenic compound that is widely used as an additive in swine and poultry feed to inhibit disease and promote growth. Due to its low metabolism in animals, it is excreted in animal urine and feces leading to its widespread contamination of soils and aquatic ecosystems. Herein, we demonstrated that ROX can be adsorbed and subsequently reduced by a common iron sulfide (greigite - Fe3S4) in the pH range of 3.6 to 8.6. ROX removal processes followed a pseudo-second-order kinetic model that was strongly pH dependent. The nitro group of ROX was reduced by structural sulfide rather than dissolved sulfide or ferrous iron to generate an amino-group containing product, 4-hydroxy-3-aminophenylarsonic acid (HAPA). At neutral to alkaline pH values ROX and HAPA are preferentially adsorbed rather than reduced on the Fe3S4 surface. The interaction between ROX and Fe3S4 was minimally affected by interactions with coexisting cations, anions and natural organic matter (humic acid). These novel findings provide new insights for understanding the transformation mechanism of ROX by iron sulfides minerals, and have practical application for designing efficient systems for advanced treatment of ROX. © 2017 Elsevier B.V.

语种： 英文

作者： 董国辉;张礼知

作者机构： 华中师范大学化学学院农药与化学生物学教育部重点实验室

会议名称： 第十三届全国太阳能光化学与光催化学术会议

会议时间： 2012-10-26

会议地点： 中国湖北武汉

会议论文集名称： 第十三届全国太阳能光化学与光催化学术会议学术论文集

关键词： 氮化碳;六价铬;插层;光催化;可见光

语种： 中文

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

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

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

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

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