表面铁循环调控及其环境意义
作者：
张礼知
作者机构：
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 武汉430079
会议名称：
第九届全国环境化学大会
会议时间：
20171019
会议地点：
杭州
会议论文集名称：
第九届全国环境化学大会论文集
摘要：
铁广泛存在大气气溶胶、天然水体、土壤和动植物体内,其普遍存在及氧化还原特性使其在自然界生物地球化学循环和生物体的化学演变过程扮演着重要角色.
语种：
中文
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基于表面铁循环调控的高效表面Fenton反应体系构建
作者：
侯晓静;黄小鹏;贾法龙;艾智慧;赵进才;...
作者机构：
华中师范大学化学学院 武汉430079
会议名称：
第九届全国环境化学大会
会议时间：
20171019
会议地点：
杭州
会议论文集名称：
第九届全国环境化学大会论文集
摘要：
实现高效铁循环是提高 Fenton 氧化技术效率的关键所在.在传统 Fenton(Fe2+/H2O2)体系中,亚铁离子和双氧水(H2O2)反应(76 M-1s-1)产生强氧化性羟基自由基(·OH)和三价铁离子,而三价铁离子与 H2O2 反应(0.02 M-1s-1)再生成亚铁的过程是非常缓慢的,使得体系中铁循环效率较低,导致 H2O2 不能持续分解利用率低.
语种：
中文
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Boosted photoelectrochemical immunosensing of metronidazole in tablet using coral-like g-C3N4 nanoarchitectures
作者：
Li, Xin;Yuan, Yijin;Pan, Xinmeng;Zhang, Lizhi;Gong, Jingming*
期刊：
Biosensors and Bioelectronics ,2019年123:7-13 ISSN：0956-5663
通讯作者：
Gong, Jingming
作者机构：
[Zhang, Lizhi; Gong, Jingming; Yuan, Yijin; Pan, Xinmeng; Li, Xin] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Gong, Jingming] C;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
关键词：
Coral-like g-C(3)N(4);Metronidazole;Nanoarchitectured design;Oral medicine sample;Photoelectrochemical immunoassay
摘要：
A simple, facile and sensitive photoelectrochemical (PEC) bioassay protocol for metronidazole (MNZ) detection in common oral medicine samples has been proposed under visible-light irradiation, where novel hierarchical coral-like g-C 3 N 4 nanoarchitectures (cg-C 3 N 4 ) have been first explored as PEC sensing platform. Featured with the unique nanostructures (e.g., interlaced porous network architecture, and open boundaries), the as-formed cg-C 3 N 4 nanoarchitectures not only efficiently inhibit the recombination of photogenerated electron-hole but also enable the immobilization of capture antibodies as well as the antibody-antigen binding efficiency fluently, thus amplifying the photocurrent response. This newly constructed PEC immunoassay displays excellent performance for MNZ determination with high sensitivity and selectivity. Under the optimal condition, this bioassay protocol exhibits a linear range of 0.01–100 µM with a detection limit of 0.005 µM at signal to noise ratio of 3. The resulting PEC immunoassay has been proved to be applicable for sensing MNZ in common oral medicine samples. © 2018 Elsevier B.V.
语种：
英文
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Oxygen Vacancies Promoted the Selective Photocatalytic Removal of NO with Blue TiO2 via Simultaneous Molecular Oxygen Activation and Photogenerated Hole Annihilation
作者：
Shang, Huan;Li, Meiqi;Li, Hao;Huang, Shun;Mao, Chengliang;...
期刊：
Environmental Science & Technology ,2019年53(11):6444-6453 ISSN：0013-936X
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Shang, Huan; Mao, Chengliang; Li, Hao; Ai, ZH; Zhang, LZ; Huang, Shun; Ai, Zhihui; Li, Meiqi] 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：
[Ai, ZH; Zhang, LZ] 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：
Semiconductor photocatalytic technology has great potential for the removal of dilute gaseous NO in indoor and outdoor atmospheres but suffers from unsatisfactory NO-removal selectivity due to undesirable NO2 byproduct generation. In this study, we demonstrate that the 99% selectivity of photocatalytic NO oxidation toward nitrate can be achieved over blue TiO2 bearing oxygen vacancies (OVs) under visible-light irradiation. First-principles density functional theory calculation and experimental results suggested that the OVs of blue TiO2 with localized electrons could facilitate the molecular oxygen activation through single-electron pathways to generate ·O2- and simultaneously promote the photogenerated hole annihilation. The generated ·O2- directly converted NO to nitrate, while the hole annihilation inhibited the side-reaction between holes and NO to avoid toxic NO2 byproduct formation, resulting in the highly selective removal of NO. This study reveals the dual functions of OVs in defective photocatalysts and also provides fundamental guidance for the selective purification of NO with photocatalytic technology. © 2019 American Chemical Society.
语种：
英文
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Robust and well-controlled TiO2-Al2O3 binary nanoarray-integrated ceramic honeycomb for efficient propane combustion
作者：
Xiong, Juxia;Luo, Zhu;Yang, Ji;Guo, Yanbing* ;Piyadasa, Adimali;...
期刊：
CrystEngComm ,2019年21(17):2727-2735 ISSN：1466-8033
通讯作者：
Guo, Yanbing;Gao, Pu-Xian
作者机构：
[Zhang, Lizhi; Yang, Weiwei; Guo, Yanbing; Yang, Ji; Deng, Hongtao; Xiong, Juxia; Luo, Zhu; Hu, Siyu; Fang, Yarong] Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Hubei, Peoples R China.;[Piyadasa, Adimali; Gao, Pu-Xian; Hoang, Son; Wang, Sibo] Univ Connecticut, Dept Mat Sci & Engn, Storrs, CT 06269 USA.;[Piyadasa, Adimali; Gao, Pu-Xian; Hoang, Son; Wang, Sibo] Univ Connecticut, Inst Mat Sci, Storrs, CT 06269 USA.
通讯机构：
[Guo, Yanbing] C;[Gao, Pu-Xian] U;Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Hubei, Peoples R China.;Univ Connecticut, Dept Mat Sci & Engn, Storrs, CT 06269 USA.;Univ Connecticut, Inst Mat Sci, Storrs, CT 06269 USA.
摘要：
The catalytic total oxidation of short-chain alkanes released from automobile exhausts is still a big challenge in volatile organic compound (VOC) elimination. The significant degradation of catalytic activity after hydrothermal aging is a widely existing issue. Herein, we report a facile one-pot hydrothermal method to successfully grow TiO2-Al2O3 binary nanoarrays on the 3D channel surfaces of ceramic honeycombs. Such a binary nanoarray was heterogeneously integrated on the cordierite honeycomb channel surface with closely separated nanowire arrays of anatase-TiO2 and mesoporous γ-Al2O3, which exhibited excellent robustness under mechanical vibration and thermal and hydrothermal aging. Moreover, propane conversion with the Pt/TiO2-Al2O3 binary nanoarray catalyst rapidly reached 80% at a temperature as low as 224 °C, suggesting that the binary nanoarray catalyst is a promising candidate for practical applications. © 2019 The Royal Society of Chemistry.
语种：
英文
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Liquid Nitrogen Activation of Zero-Valent Iron and Its Enhanced Cr(VI) Removal Performance
作者：
Hu, Yue;Peng, Xing;Ai, Zhihui;Jia, Falong* ;Zhang, Lizhi*
期刊：
Environmental Science & Technology ,2019年53(14):8333-8341 ISSN：0013-936X
通讯作者：
Jia, Falong;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Peng, Xing; Hu, Yue; Ai, Zhihui; Jia, Falong; Zhang, LZ] 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：
[Jia, FL; Zhang, LZ] 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, we report that liquid nitrogen treatment is a promising zero-valent iron activation method that does not remove the iron oxide shell; this can improve the apparent Cr(VI) removal rate constant of zero-valent iron by about 4-120 times, depending on the particle sizes and the suppliers of zero-valent iron. It was found that liquid nitrogen, with its low temperature of 77 K, could crack the iron oxide shell of zero-valent iron to produce abundant fractures because of the different thermal expansion coefficients of iron oxide and iron. These fractures provided suitable mass transfer channels for the inward transfer of water/oxygen molecules to the iron core and the subsequent in situ generation of Fe(II) for the reduction of Cr(VI) to Cr(III). More importantly, systematic characterizations confirmed the generation of an Fe(III)/Cr(III)/Cr(VI) composite on the surface of zero-valent iron during the removal, suggesting its environmental benignancy. This study provides a novel physical zero-valent iron activation method, sheds light on the importance of the iron oxide shell of zero-valent iron on Cr(VI) removal, and clarifies the intrinsic Cr(VI) removal mechanism of zero-valent iron. © 2019 American Chemical Society.
语种：
英文
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Oxygen Vacancy-Mediated Photocatalysis of BiOCl: Reactivity, Selectivity, and Perspectives
作者：
Li, Hao;Li, Jie;Ai, Zhihui;Jia, Falong;Zhang, Lizhi*
期刊：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION ,2018年57(1):122-138 ISSN：1433-7851
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Li, Hao; Li, Jie; Ai, Zhihui; Jia, Falong] Cent China Normal Univ, Coll Chem, Inst Environm 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 Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词：
BiOCl;nitrogen fixation;oxygen activation;photocatalysis;water splitting
摘要：
Semiconductor photocatalysis is a trustworthy approach to harvest clean solar light for energy conversions, while state-of-the-art catalytic efficiencies are unsatisfactory because of the finite light response and/or recombination of robust charge carriers. Along with the development of modern material characterization techniques and electronic-structure computations, oxygen vacancies (OVs) on the surface of real photocatalysts, even in infinitesimal concentration, are found to play a more decisive role in determining the kinetics, energetics, and mechanisms of photocatalytic reactions. This Review endeavors to clarify the inherent functionality of OVs in photocatalysis at the surface molecular level using 2D BiOCl as the platform. Structure sensitivity of OVs on reactivity and selectivity of photocatalytic reactions is intensely discussed via confining OVs onto prototypical BiOCl surfaces of different structures. The critical understanding of OVs chemistry can help consolidate and advance the fundamental theories of photocatalysis, and also offer new perspectives and guidelines for the rational design of catalysts with satisfactory performance. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
语种：
英文
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Visible light driven selective oxidation of amines to imines with BiOCl: Does oxygen vacancy concentration matter?
作者：
Mao, Chengliang;Cheng, Honggang;Tian, Hao;Li, Hao;Xiao, Wen-Jing;...
期刊：
Applied Catalysis B: Environmental ,2018年228:87-96 ISSN：0926-3373
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Mao, Chengliang; Zhao, Jincai; Cheng, Honggang; Li, Hao; Xiao, Wen-Jing] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Xu, Hu; Tian, Hao] South Univ Sci & Technol China, Dept Phys, Shenzhen 518055, 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, Peoples R China.
关键词：
Bismuth oxychloride;Molecular oxygen activation;Oxygen vacancies;Photocatalysis;Selective amines oxidation
摘要：
The relationship between oxygen vacancy (OV) concentration of semiconductors and their photocatalytic performances is far from clarified. In this study, by tuning the OV concentration of BiOCl (001) surface via a novel H<inf>2</inf>O<inf>2</inf>treatment coupled infrared irradiation method, we demonstrate that OV concentration of BiOCl (001) surface strongly determine its surface atomic and electronic structures to modulate the photocatalytic pathways. Being of shorter Bi–Bi and Bi–O bond lengths as well as more electrons being less localized, BiOCl (001) surface with higher OV concentration favored molecular oxygen activation to generate O<inf>2</inf><sup>2−</sup>via a two-electron transfer pathway, while the generated O<inf>2</inf><sup>2−</sup>could prevent the over oxidation of amines and thus achieve high selectivity in the oxidation of amines to imines. Similar phenomena were also observed for other semiconductor photocatalysts such as TiO<inf>2</inf>and Nb<inf>2</inf>O<inf>5</inf>, suggesting the generality of oxygen vacancy concentration mediated selectivity enhancement. These findings shed light on the relationship between the oxygen vacancy concentration and the surface structure of semiconductor photocatalysts and offer a novel pathway to realize photocatalytic selective oxidation of amines to imines.<br/> ©2018 Elsevier B.V.
语种：
英文
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Surface Fe(II)/Fe(III) Cycle Promoted Ultra-Highly Sensitive Electrochemical Sensing of Arsenic(III) with Dumbbell-Like Au/Fe3O4 Nanoparticles
作者：
Li, Shan-Shan;Zhou, Wen-Yi;Jiang, Min;Guo, Zheng;Liu, Jin-Huai;...
期刊：
Analytical Chemistry ,2018年90(7):4569-4577 ISSN：0003-2700
通讯作者：
Huang, Xing-Jiu;Zhang, Lizhi
作者机构：
[Li, Shan-Shan; Guo, Zheng; Liu, Jin-Huai; Jiang, Min; Zhou, Wen-Yi; Huang, Xing-Jiu] Chinese Acad Sci, Key Lab Environm Opt & Technol, Hefei 230031, Anhui, Peoples R China.;[Li, Shan-Shan; Guo, Zheng; Liu, Jin-Huai; Jiang, Min; Zhou, Wen-Yi; Huang, Xing-Jiu] Chinese Acad Sci, Inst Intelligent Machines, Hefei 230031, Anhui, Peoples R China.;[Li, Shan-Shan; Guo, Zheng; Liu, Jin-Huai; Jiang, Min; Zhou, Wen-Yi; Huang, Xing-Jiu] Univ Sci & Technol China, Hefei 230026, Anhui, Peoples R China.;[Zhang, Lizhi] Cent China Normal Univ, Inst Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Huang, Xing-Jiu; Zhang, Lizhi] C;[Huang, Xing-Jiu] U;Chinese Acad Sci, Key Lab Environm Opt & Technol, Hefei 230031, Anhui, Peoples R China.;Chinese Acad Sci, Inst Intelligent Machines, Hefei 230031, Anhui, Peoples R China.;Univ Sci & Technol China, Hefei 230026, Anhui, Peoples R China.
摘要：
Developing a new ultrasensitive interface to detect As(III) is highly desirable because of its seriously toxic and low concentration in drinking water. Recently, Fe3O4 nanoparticles of high adsorption toward As(III) become very promising to be such an interface, which is still limited by the poor understanding of their surface physicochemical properties. Herein, we report that dumbbell-like Au/Fe3O4 nanoparticles, when being modified the screen-printed carbon electrode, can serve as an efficient sensing interface for As(III) detection with an excellent sensitivity of 9.43 μA ppb-1 and a low detection limit of 0.0215 ppb. These outstanding records were attributed to the participation of Fe(II)/Fe(III) cycle on Fe3O4 surface in the electrochemical reaction of As(III) redox, as revealed by X-ray photoelectron spectroscopy, X-ray absorption near edge structure, and extended X-ray absorption fine structure. This work provides new insight into the mechanism of electroanalysis from the viewpoint of surface active atoms, and also helps to predict the construction of ultrahighly sensitive electrochemical sensors for other heavy metal ions with nonprecious redox active materials. © 2018 American Chemical Society.
语种：
英文
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Efficient light-driven CO2 hydrogenation on Ru/CeO2 catalysts
作者：
Quan, Fengjiao;Zhan, Guangming;Mao, Chengliang;Ai, Zhihui;Jia, Falong* ;...
期刊：
Catalysis Science & Technology ,2018年8(24):6503-6510 ISSN：2044-4753
通讯作者：
Jia, Falong
作者机构：
[Quan, Fengjiao; Zhang, Lizhi; Mao, Chengliang; Zhan, Guangming; Ai, Zhihui; Jia, Falong] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.;[Liu, Shiyuan; Gu, Honggang] Huazhong Univ Sci & Technol, State Key Lab Digital Mfg Equipment & Technol, Wuhan 430074, Hubei, Peoples R China.
通讯机构：
[Jia, Falong] 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：
Light-driven heterogeneous catalysis provides a promising way to accomplish chemical reactions by the use of light energy, which reduces the consumption of chemical energy sources. Here, we show that Ru/CeO2 catalysts exhibit high activity for the hydrogenation of CO2 to methane under illumination only, reaching high CO2 conversion (over 99.9%) and selectivity of methane (∼100%) at low temperature. In sharp contrast, less CO2 is converted at the same temperature when a traditional heating model is used. As revealed by the results, the enhanced conversion rate under illumination should not only be attributed to the light-induced thermo-heating. Further investigations by in situ IR analysis and theoretical calculation provide comprehensive understanding of the reaction mechanism, and the important role of light is revealed. It is expected that the combination of catalysts and light may afford new perspectives for CO2 hydrogenation. © 2018 The Royal Society of Chemistry.
语种：
英文
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High-Throughput Signal-On Photoelectrochemical Immunoassay of Lysozyme Based on Hole-Trapping Triggered by Disintegrating Bioconjugates of Dopamine-Grafted Silica Nanospheres
作者：
Li, Xin;Wang, Xinlei;Zhang, Lizhi;Gong, Jingming*
期刊：
ACS SENSORS ,2018年3(8):1480-1488 ISSN：2379-3694
通讯作者：
Gong, Jingming
作者机构：
[Zhang, Lizhi; Gong, Jingming; Wang, Xinlei; Li, Xin] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Gong, Jingming] C;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
关键词：
photoelectrochemical immunoassay;high-throughput;bioconjugate disintegration;dopamine-grafted silica nanosphere;lysozyme
摘要：
A unique split-type photoelectrochemical (PEC) immunoassay has been constructed for detection of low-abundance biocompounds (lysozyme, Lyz, used in this case) via a new trigger strategy by disintegrating bioconjugates of dopamine-grafted silica nanospheres (DA@SiO2NSs) for signal amplification. The preferred electron donor assembly of DA@SiO2NSs is first used as a molecular printboard for positioning anti-Lyz secondary antibody (Ab2) through an amide reaction. With specific immunoreactions in a high-binding microplate, a sandwich immunoassay, the DA@SiO2NSs-based bioconjugate is achieved. By initiating the disintegration of the bioconjugates via acid etching, numerous electron donors of DA are released, thus efficiently triggering hole-trapping with amplified signals obtained. The smart integration of ZnIn2S4-based heterojunctions as photoactive material, a split-type detection mode, and a new trigger strategy by disintegrating the DA@SiO2NSs-based bioconjugate offer an attractive high-throughput signal-on PEC immunoassay for detection of Lyz. Such an unusual PEC sensor exhibits an outstanding linear response to the concentration in the range between 0.002 and 500 ng mL-1, and the detection limit is as low as 0.6 ppt (S/N = 3). The as-fabricated assay is cost-effective and sensitive. It has been successfully used for measuring Lyz in real samples, which demonstrates great promise for practical applications. © Copyright 2018 American Chemical Society.
语种：
英文
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Atomically manipulated proton transfer energizes water oxidation on silicon carbide photoanodes
作者：
Li, Hao;Shang, Huan;Shi, Yuchen;Yakimova, Rositsa;Syvajarvi, Mikael;...
期刊：
Journal of Materials Chemistry A ,2018年6(47):24358-24366 ISSN：2050-7488
通讯作者：
Sun, Jianwu
作者机构：
[Syvajarvi, Mikael; Shi, Yuchen; Li, Hao; Yakimova, Rositsa; Sun, Jianwu] Linkoping Univ, Dept Phys Chem & Biol, S-58183 Linkoping, Sweden.;[Zhang, Lizhi; Shang, Huan] 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：
[Sun, Jianwu] L;Linkoping Univ, Dept Phys Chem & Biol, S-58183 Linkoping, Sweden.
摘要：
Surmounting the sluggish water oxidation kinetics beyond the hole-dominated thermodynamic effect is a topic of great scientific interest to establish fully renewable hydrogen technology from solar-powered water splitting. Herein, we demonstrate that the bottleneck of photoelectrochemical water oxidation can be overcome via atomic manipulation of proton transfer on the polar surfaces of silicon carbide (SiC) photoanodes. On the typical carbon-face SiC, where proton-coupled electron transfer governed the interfacial hole transfer for water oxidation, substantial energy loss was inevitable due to the highly activated proton-transfer steps. Via preferentially exposing the silicon-face, we enabled surface-catalyzed barrierless O-H breaking with a facile proton exchange and migration character. This mechanistically shifted the rate limiting step of water oxidation from sluggish proton-coupled electron transfer to a more energy-favorable electron transfer. The proof-of-concept study introduced here may open up new possibilities to design sophisticated photoelectrodes for an unbiased solar water splitting cell via surface engineering. © 2018 The Royal Society of Chemistry.
语种：
英文
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Molecular O2 Activation over Cu(I)-Mediated C=N Bond for Low-Temperature CO Oxidation
作者：
Hu, Siyu;Xiao, Wen;Yang, Weiwei;Yang, Ji;Fang, Yarong;...
期刊：
ACS Applied Materials & Interfaces ,2018年10(20):17167-17174 ISSN：1944-8244
通讯作者：
Guo, Yanbing
作者机构：
[Long, Juxia; Zhang, Lizhi; Deng, Hongtao; Luo, Zhu; Yang, Weiwei; Guo, Yanbing; Hu, Siyu; Yang, Ji; Fang, Yarong] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Ding, Jun; Xiao, Wen] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, 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.
关键词：
CO oxidation;CuTCNQ NWs;DFT calculations;in situ DRIFTS;molecular O2 activation
摘要：
The activation of molecular oxygen (O2) is extremely crucial in heterogeneous oxidations for various industrial applications. Here, a charge-transfer complex CuTCNQ nanowire (CuTCNQ NW) array grown on the copper foam was first reported to show CO catalytic oxidation activity at a temperature below 200 °C with the activated O2 as an oxidant. The molecular O2 was energetically activated over the Cu(I)-mediated C=N bond with a lower energy of -1.167 eV and preferentially reduced to •O2- through one-electron transfer during the activation process by density functional theory calculations and electron paramagnetic resonance. The theoretical calculations indicated that the CO molecule was oxidized by the activated O2 on the CuTCNQ NW surface via the Eley-Rideal mechanism, which had been further confirmed by in situ diffuse reflectance infrared Fourier transform spectra. These results indicated that the local C=N bond electron-state engineering could effectively improve the molecular O2 activation efficiency, which facilitates the low-temperature CO catalytic oxidation. The findings reported here enhance our understanding on the molecular oxygen activation pathway over metal-organic nanocatalysts and provide a new avenue for rational design of novel low-cost, organic-based heterogeneous catalysts. Copyright © 2018 American Chemical Society.
语种：
英文
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Fenton oxidation of organic contaminants with aquifer sediment activated by ascorbic acid
作者：
Hou, Xiaojing;Huang, Xiaopeng;Li, Mengliang;Zhang, Yunshang;Yuan, Songhu;...
期刊：
Chemical Engineering Journal ,2018年348:255-262 ISSN：1385-8947
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Hou, Xiaojing; Li, Mengliang; Huang, Xiaopeng; Zhao, Jincai; Zhang, Yunshang; Ai, ZH; Zhang, LZ; Ai, Zhihui] Cent China Normal Univ, Inst Environm & Appl Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.;[Yuan, Songhu] China Univ Geosci, State Key Lab Biogeol & Environm Geol, Wuhan 430074, 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：
Aquifer sediment;Ascorbic acid;Groundwater;In situ chemical oxidation;Organic contaminants
摘要：
In this study, we report the desirable conversion of H2O2 to [rad]OH with aquifer sediment activated by ascorbic acid. Although aquifer sediment contained various iron minerals, such as goethite, hematite, montmorillonite, muscovite, chlorite and phlogopite, it could not efficiently activate H2O2 to produce [rad]OH. Interestingly, the presence of ascorbic acid dramatically promoted the [rad]OH conversion efficiency of H2O2 by aquifer sediment to remediate organic contaminants in groundwater, which was ascribed to the efficient iron cycle of aquifer sediment induced by ascorbic acid. Among these minerals in sediment, goethite and hematite were more reactive than other minerals to activate H2O2 in the presence of ascorbic acid. Although the initial pH could affect the [rad]OH conversion efficiency of H2O2, H2O2 could be decomposed by aquifer sediment at pH 3-11 after the introduction of ascorbic acid. Along with the complete degradation of organic contaminants, the final pH of solution increased to 8.3, which was close to the initial pH (8.9) of groundwater. Moreover, packed column of aquifer sediment could also catalyze the H2O2 conversion to [rad]OH for the removal of different organic contaminants with adding ascorbic acid, suggesting a new strategy for in situ chemical oxidation remediation of organic contaminated groundwater. © 2018 Elsevier B.V.
语种：
英文
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Facet-dependent contaminant removal properties of hematite nanocrystals and their environmental implications
作者：
Huang, Xiaopeng;Hou, Xiaojing;Zhang, Xin;Rosso, Kevin M.* ;Zhang, Lizhi*
期刊：
Environmental Science: Nano ,2018年5(8):1790-1806 ISSN：2051-8153
通讯作者：
Zhang, Lizhi;Rosso, Kevin M.
作者机构：
[Zhang, Lizhi; Hou, Xiaojing; Huang, Xiaopeng] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Zhang, Xin; Rosso, Kevin M.; Huang, Xiaopeng] Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99352 USA.
通讯机构：
[Zhang, Lizhi] C;[Rosso, Kevin M.] P;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99352 USA.
摘要：
Hematite nanocrystals are ubiquitous in natural environments, and because of their strong sorption properties these particles can influence the mobility and fate of toxic elements such as hexavalent chromium and arsenic. It is now well established that sorption onto hematite is morphology dependent, because its hexagonal structure imparts distinct interfacial chemistry to individual facets. It is also well known that interaction of these facets with ferrous iron can impart powerful catalytic reduction capacity at these interfaces. However, the underlying mechanisms for facet-specific sorption and reductive transformation of specific metals remains poorly understood at the molecular scale. In this article, we first briefly review the synthesis of size and morphologically well-defined hematite nanocrystals and their corresponding growth mechanisms. We then summarize recent advances in understanding interactions between hematite facets and ferrous iron, as well as their impact on the geochemical cycles of some elements and contaminants. We emphasize the reductive dissolution of hematite facets and elucidate corresponding environmental implications. Furthermore, we focus on facet-dependent adsorption of model environmental contaminants. Finally, we highlight the importance of hematite nanocrystals for remediation and provide suggestions for improving understanding of their roles in the environment. © The Royal Society of Chemistry.
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英文
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Mn2+ promoted Cr(VI) reduction with oxalic acid: The indispensable role of In-situ generated Mn3+
作者：
Mu, Yi;Jiang, Xu;Ai, Zhihui* ;Jia, Falong;Zhang, Lizhi*
期刊：
Journal of Hazardous Materials ,2018年343:356-363 ISSN：0304-3894
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Mu, Yi; Jiang, Xu; Ai, ZH; Zhang, LZ; Ai, Zhihui; Jia, Falong] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm & Appl Chem,Coll Chem, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Ai, ZH; Zhang, LZ] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm & Appl Chem,Coll Chem, Wuhan 430079, Hubei, Peoples R China.
关键词：
Cr(VI) reduction;Mn(2+);Ternary complex;in-situ generated Mn(3+);oxalic acid
摘要：
In this study, we demonstrate that Mn(2+) can greatly promote the Cr(VI) reduction by oxalic acid at pH<5 via an induction period and a subsequent auto-acceleration process. The Cr(VI) reduction rate constant during the late auto-acceleration process was about 10 times that of the initial induction period. Characterization results revealed that this interesting two-step Cr(VI) reduction phenomenon was attributed to the in-situ generated Mn(3+) by the oxidation of Mn(2+) with Cr(VI) in the presence of oxalic acid during the induction period. The in-situ generated Mn(3+) might complex with oxalate and Cr(VI) to produce a ternary complex, thus facilitating the electron transfer from oxalate to Cr(VI) to automatically accelerate the Cr(VI) reduction process. These findings shed insight into the possible roles of widely existed Mn ions (Mn(2+) and Mn(3+)) and oxalic acid in the transformation of Cr(VI) in natural aquatic environment, and also provided an efficient way to remediate Cr(VI)-containing acid wastewater.
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英文
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New opportunities for efficient N-2 fixation by nanosheet photocatalysts
作者：
Li, Hao;Mao, Chengliang;Shang, Huan;Yang, Zhiping;Ai, Zhihui;...
期刊：
Nanoscale ,2018年10(33):15429-15435 ISSN：2040-3364
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Yang, Zhiping; Mao, Chengliang; Shang, Huan; Li, Hao; 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：
Catalytic ammonia synthesis from dinitrogen (N2) under mild conditions has been considered to be the "holy grail" of N2 fixation, which is one of the most important chemical processes in the agriculture, biological and industrial fields. Given that current artificial N2 fixation is still dominated by the energy-intensive Haber-Bosch process, solar N2 fixation represents an encouraging and fascinating route for carbon-free and energy-saving N2 fixation. However, its practical application is seriously hampered by surface sluggish reaction kinetics. In this minireview, we share our perspectives on the use of two-dimensional (2D) nanosheets for the manipulation of photocatalytic N2 fixation. Nanosheet photocatalysts serve as the perfect platform for the engineering of surface active sites, including defects and iron, all of which can not only bolster photon-exciton interaction toward robust charge carriers generation upon light absorption, but also mimic the function schemes of MoFe-cofactor in nitrogenase toward sufficient N2 binding and activation. These merits endowed by nanosheets photocatalysts provide instructive information on exploring the rich nitrogen photochemistry on solid surfaces and offer new opportunities for the design of novel photocatalysts towards efficient N2 fixation. © 2018 The Royal Society of Chemistry.
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英文
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Disposable photoelectrochemical sensing strip for highly sensitive determination of perfluorooctane sulfonyl fluoride on functionalized screen-printed carbon electrode
作者：
Li, Xin;Wang, Xinlei;Fang, Tian;Zhang, Lizhi;Gong, Jingming*
期刊：
Talanta ,2018年181:147-153 ISSN：0039-9140
通讯作者：
Gong, Jingming
作者机构：
[Zhang, Lizhi; Gong, Jingming; Wang, Xinlei; Fang, Tian; Li, Xin] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Inst Appl & Environm Chem, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Gong, Jingming] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Inst Appl & Environm Chem, Wuhan 430079, Hubei, Peoples R China.
关键词：
Disposable sensing strip;In-situ electrodeposition;Molecularly imprinted polymer;Perfluorooctane sulfonyl fluoride;Photoelectrochemical sensor
摘要：
Owing to the lack of chromophores and ionizable functional groups, it is a significant challenge to determine perfluorooctane sulfonyl fluoride (PFOSF) by traditional high-performance liquid chromatography or liquid chromatography/mass spectrometry, especially at a low concentration. In this work a unique photoelectrochemical (PEC) sensing strip has been developed for the first time for the detection of PFOSF. The sensing strip is cost effective and disposable, whereby BiOI nanoflake arrays are fabricated on a home-made screen-printed electrode through a facile one-step in-situ electrodeposition process, and then the molecule tags (i.e., molecularly imprinted polymers) for PFOSF are subsequently grafted on the surface. Benefitting from a three-dimensional interconnected framework, the as-fabricated sensing strip has a rapid response to the interfacial steric hindrance effect between the sensing platform and the target analyte of PFOSF. The elaborated PEC sensor exhibits a outstanding linear response to a concentration of PFOSF ranging from 0.05 to 500.0 ppb and a detection limit down to 0.01 ppb (S/N = 3) Furthermore, our low-cost and highly sensitive sensor has been further explored to detect PFOSF in real water samples, showing satisfactory results. © 2018 Elsevier B.V.
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英文
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Persistent free radicals in carbon-based materials on transformation of refractory organic contaminants (ROCs) in water: A critical review
作者：
Qin, Yaxin;Li, Guiying;Gao, Yanpeng;Zhang, Lizhi;Ok, Yong Sik;...
期刊：
Water Research ,2018年137:130-143 ISSN：0043-1354
通讯作者：
An, Taicheng
作者机构：
[An, Taicheng; Qin, Yaxin; Gao, Yanpeng; Li, Guiying] Guangdong Univ Technol, Inst Environm Hlth & Pollut Control, Sch Environm Sci & Engn, Guangzhou Key Lab Environm Catalysis & Pollut Con, Guangzhou 510005, Guangdong, Peoples R China.;[Zhang, Lizhi] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Ok, Yong Sik] Korea Univ, O Jeong Ecoresilience Inst, Korea Blochar Res Ctr, Seoul 02841, South Korea.;[Ok, Yong Sik] Korea Univ, Div Environm Sci & Ecol Engn, Seoul 02841, South Korea.
通讯机构：
[An, Taicheng] G;Guangdong Univ Technol, Inst Environm Hlth & Pollut Control, Sch Environm Sci & Engn, Guangzhou Key Lab Environm Catalysis & Pollut Con, Guangzhou 510005, Guangdong, Peoples R China.
关键词：
*Black carbon;*Carbon-based materials;*Hydrochar;*Persistent free radicals;*Pollution control mechanism;*Refractory organic contaminants
摘要：
With the increased concentrations and kinds of refractory organic contaminants (ROCs) in aquatic environments, many previous reviews systematically summarized the applications of carbon-based materials in the adsorption and catalytic degradation of ROCs for their economically viable and environmentally friendly behavior. Interestingly, recent studies indicated that carbon-based materials in natural environment can also mediate the transformation of ROCs directly or indirectly due to their abundant persistent free radicals (PFRs). Understanding the formation mechanisms of PFRs in carbo-based materials and their interactions with ROCs is essential to develop their further applications in environment remediation. However, there is no comprehensive review so far about the direct and indirect removal of ROCs mediated by PFRs in amorphous, porous and crystalline carbon-based materials. The review aims to evaluate the formation mechanisms of PFRs in carbon-based materials synthesized through pyrolysis and hydrothermal carbonization processes. The influence of synthesis conditions (temperature and time) and carbon sources on the types as well as the concentrations of PFRs in carbon-based materials are also discussed. In particular, the effects of metals on the concentrations and types of PFRs in carbon-based materials are highlighted because they are considered as the catalysts for the formation of PFRs. The formation mechanisms of reactive species and the further transformation mechanisms of ROCs are briefly summarized, and the surface properties of carbon-based materials including surface area, types and number of functional groups, etc. are found to be the key parameters controlling their activities. However, due to diversity and complexity of carbon-based materials, the exact relationships between the activities of carbon-based materials and PFRs are still uncertain. Finally, the existing problems and current challenges for the ROCs transformation with carbon-based materials are also pointed out. © 2018 Elsevier Ltd
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英文
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Visible Light Driven Organic Pollutants Degradation with Hydrothermally Carbonized Sewage Sludge and Oxalate Via Molecular Oxygen Activation
作者：
Chen, Na;Shang, Huan;Tao, Shuangyi;Wang, Xiaobing;Zhan, Guangming;...
期刊：
Environmental Science & Technology ,2018年52(21):12656-12666 ISSN：0013-936X
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Shang, Huan; An, Zhihui; Chen, Na; Wang, Xiaobing; Li, Hao; Zhan, Guangming] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Yang, Jiakuan; Tao, Shuangyi] Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Hubei, Peoples R China.
通讯机构：
[Zhang, Lizhi] C;Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
摘要：
Converting sewage sludge into functional environmental materials has become an attractive sewage sludge disposal route. In this study, we synthesize a sewage sludge-based material via a facile one-pot hydrothermal carbonization method and construct a visible light molecular oxygen activation system with hydrothermally carbonized sewage sludge (HTC-S) and oxalate to degrade various organic pollutants. It was found that iron species of HTC-S could chelate with oxalate to generate H 2 O 2 via molecular oxygen activation under visible light, and also promote the H 2 O 2 decomposition to produce • OH for the fast organic pollutants degradation. Taking sulfadimidine as the example, the apparent degradation rate of HTC-S/oxalate system was almost 5-20 times that of iron oxides/oxalate system. This outstanding degradation performance was attributed to the presence of iron-containing clay minerals in HTC-S, as confirmed by X-ray diffraction measurements and Mössbauer spectrometry. In the oxalate solution, these iron-containing clay minerals could be excited more easily than common iron oxides under visible light, because the silicon species strongly interacted with iron species in HTC-S to form Fe-O-Si bond, which lowered the excitation energy of Fe-oxalate complex. This work provides an alternative sewage sludge conversion pathway and also sheds light on the environmental remediation applications of sewage sludge-based materials. Copyright © 2018 American Chemical Society.
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