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.
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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.
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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.
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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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.
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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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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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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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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.
语种：
英文
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Oxygen Vacancies Mediated Complete Visible Light NO Oxidation via Side-On Bridging Superoxide Radicals
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.
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英文
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Molecular Insights into NO-Promoted Sulfate Formation on Model TiO2 Nanoparticles with Different Exposed Facets
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.
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英文
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Energy-confined solar thermal ammonia synthesis with K/Ru/TiO2-xHx
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
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Ni(II) induced aerobic ring opening degradation of atrazine with core-shell Fe@Fe2 O3 nanowires
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.
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Iron oxide shell mediated environmental remediation properties of nano zero-valent iron
作者：
Mu, Yi;Jia, Falong;Ai, Zhihui* ;Zhang, Lizhi*
期刊：
Environmental Science: Nano ,2017年4(1):27-45 ISSN：2051-8153
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Mu, Yi; Ai, ZH; Zhang, LZ; Jia, Falong; Ai, Zhihui] Cent China Normal Univ, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Ai, ZH; Zhang, LZ] C;Cent China Normal Univ, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
摘要：
Nano zero-valent iron (nZVI) has attracted much more attention for its potential applications in the fields of environmental contaminant remediation and detoxification. Generally, nZVI consists of a zero-valent iron (Fe0) core and an iron oxide shell structure. As the underlying Fe0 core and the surface oxide shell determine the physical and chemical properties of nZVI, the nature of the oxide shell inevitably affects the organic/inorganic pollutant removal performance of nZVI, which has not been reviewed previously. In this article, we first introduce the synthesis and the oxide shell formation mechanism of core-shell structured nZVI and then discuss various characterization techniques to reveal the structure and chemical composition of the oxide shell. Subsequently, we clarify the roles of the oxide shell in the organic contaminant degradation efficiency and the molecular oxygen activation performance of nZVI and also highlight the effect of the oxide shell on heavy metal removal (including As) with nZVI. In addition, we summarize some oxide shell modification strategies to enhance the capacity and longevity of nZVI. Finally, we discuss the impacts of typical natural groundwater constituents (e.g. cations, anions, organic ligands, and dissolved oxygen) on the reactivity of nZVI and point out some unresolved issues related to the oxide shell dependent contaminant removal properties of nZVI. © The Royal Society of Chemistry.
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磁性Fe3S4纳米片催化类Fenton反应降解洛克沙胂的研究
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
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Ascorbate Induced Facet Dependent Reductive Dissolution of Hematite Nanocrystals
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 ±0.16) ×10<sup>-4</sup>and (1.59 ±0.14) ×10<sup>-4</sup>min<sup>-1</sup>for 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. ©2017 American Chemical Society.
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英文
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Fe@Fe2O3 promoted electrochemical mineralization of atrazine via a triazinon ring opening mechanism
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
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Sulfite promoted photochemical cleavage of s-triazine ring: The case study of atrazine
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
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Adsorption and reduction of roxarsone on magnetic greigite (Fe3S4): Indispensable role of structural sulfide
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.
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英文
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Environmental Chemistry of Iron-A Frontier in Environmental Chemistry and Geochemistry
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
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