赤铁矿的环境效应
作者:
黄小鹏;侯晓静;赵进才;张礼知
作者机构:
[黄小鹏; 侯晓静; 赵进才; 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:
中国化学会第30届学术年会-第二十六分会:环境化学
会议时间:
2016-07-01
会议地点:
中国辽宁大连
会议论文集名称:
中国化学会第30届学术年会摘要集-第二十六分会:环境化学
关键词:
赤铁矿;铁循环;环境效应;暴露晶面
摘要:
前人多采用不规则纳米颗粒来研究赤铁矿对环境污染物迁移转化的影响,且缺乏有效实验表征和理论计算手段,无法在原子层次上深入理解铁循环涉及的污染物吸附脱附、氧化还原及电子转移过程。我们提出可控合成出不同晶面暴露的赤铁矿纳米晶,利用扩展X射线吸收精细结构光谱、衰减全反射傅里叶红外光谱等现代表征技术,并结合密度泛函理论计算手段,系统地研究典型环境污染物在赤铁矿不同晶面上吸附/脱附和氧化还原以及电子转移过程,
语种:
中文
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Protocatechuic Acid Promoted Alachlor Degradation in Fe(III)/H2 O2 Fenton System
作者:
Qin, Yaxin;Song, Fahui;Ai, Zhihui;Zhang, Pingping;Zhang, Lizhi*
期刊:
Environmental Science & Technology ,2015年49(13):7948-7956 ISSN:0013-936X
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Qin, Yaxin; Song, Fahui; Ai, Zhihui; Zhang, Pingping] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Inst Environm Chem, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Inst Environm Chem, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.
摘要:
In this study, we demonstrate that protocatechuic acid (PCA) can significantly promote the alachlor degradation in the Fe(III)/H2O2 Fenton oxidation system. It was found that the addition of protocatechuic acid could increase the alachlor degradation rate by 10 000 times in this Fenton oxidation system at pH = 3.6. This dramatic enhancement of alachlor degradation was attributed to the complexing and reduction abilities of protocatechuic ligand, which could form stable complexes with ferric ions to prevent their precipitation and also accelerate the Fe(III)/Fe(II) cycle to enhance the ·OH generation. Meanwhile, the Fe(III)/PCA/H2O2 system could also work well at near natural pH even in the case of PCA concentration as low as 0.1 mmol/L. More importantly, both alachlor and PCA could be effectively mineralized in this Fenton system, suggesting the environmental benignity of PCA/Fe(III)/H2O2 Fenton system. We employed gas chromatography-mass spectrometry to identify the degradation intermediates of alachlor and then proposed a possible alachlor degradation mechanism in this novel Fenton oxidation system. This study provides an efficient way to remove chloroacetanilide herbicides, and also shed new insight into the possible roles of widely existed phenolic acids in the conversion and the mineralization of organic contaminants in natural aquatic environment. (Chemical Equation Presented). © 2015 American Chemical Society.
语种:
英文
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A highly sensitive photoelectrochemical detection of perfluorooctanic acid with molecularly imprined polymer-functionalized nanoarchitectured hybrid of AgI-BiOI composite
作者:
Gong, Jingming* ;Fang, Tian;Peng, Dinghua;Li, Aimin;Zhang, Lizhi
期刊:
Biosensors and Bioelectronics ,2015年73:256-263 ISSN:0956-5663
通讯作者:
Gong, Jingming
作者机构:
[Peng, Dinghua; Zhang, Lizhi; Gong, Jingming; Li, Aimin; Fang, Tian] Cent China Normal Univ, Coll Chem, Key Lab Pe Sticide & Chem Biol, Minist Educ,Inst Environm Chem, Wuhan 430079, Peoples R China.
通讯机构:
[Gong, Jingming] C;Cent China Normal Univ, Coll Chem, Key Lab Pe Sticide & Chem Biol, Minist Educ,Inst Environm Chem, Wuhan 430079, Peoples R China.
关键词:
Molecularly imprinted polymer;Nanohybrids;Perfluorooctanoic acid;Photoelectrochemical sensor
摘要:
A rapid and ultrasensitive signal-off photoelectrochemical sensor has been developed under visible-light irradiation, for the detection of perfluorooctanoic acid (PFOA), especially low level PFOA present in environment, whereby a novel nanostructured probe made of molecularly imprinted polymer (MIP) modified AgI nanoparticles-BiOI nanoflake arrays (AgI-BiOINFs) is designed as the photoactive electrode (denoted as MIP@AgI-BiOINFs). Here, the unique nanoarchitectured hybrid of AgI-BiOINFs was first in situ synthesized via a facile successive ionic layer adsorption and reaction (SILAR) approach and then employed as a matrix to graft the recognition element of MIP. Such a newly designed PEC sensor exhibits high sensitivity and selectivity for the determination of PFOA. The PEC analysis is highly linear over the PFOA concentration ranging from 0.02 to 1000.0. ppb with a detection limit of 0.01. ppb (S/. N=3). This value obtained by using the facile PEC sensor is comparable to the results obtained by using well-established liquid chromatography-tandem mass spectrometry (LC-MS/MS). Toward practical applications, this low-cost and sensitive assay was successfully applied to measure PFOA in real water samples. © 2015 Elsevier B.V..
语种:
英文
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A highly efficient zinc catalyst for selective electroreduction of carbon dioxide in aqueous NaCl solution
作者:
Quan, Fengjiao;Zhong, Dan;Song, Hancheng;Jia, Falong* ;Zhang, Lizhi
期刊:
Journal of Materials Chemistry A ,2015年3(32):16409-16413 ISSN:2050-7488
通讯作者:
Jia, Falong
作者机构:
[Quan, Fengjiao; Zhang, Lizhi; Song, Hancheng; Jia, Falong; Zhong, Dan] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构:
[Jia, Falong] C;Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
摘要:
A low-cost zinc catalyst, prepared by a facile electrochemical strategy, produces CO with up to 93% Faraday efficiency in aqueous NaCl solution. The catalytic activity of the Zn catalyst is demonstrated to be dependent on both the morphology of the catalyst and the catholyte anions. © 2015 The Royal Society of Chemistry.
语种:
英文
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Extraction of endocrine disrupting phenols with iron-ferric oxide core-shell nanowires on graphene oxide nanosheets, followed by their determination by HPLC
作者:
Li, Feng;Cai, Cuicui;Cheng, Jing* ;Zhou, Hongbin;Ding, Kerong;...
期刊:
Microchimica Acta ,2015年182(15-16):2503-2511 ISSN:0026-3672
通讯作者:
Cheng, Jing
作者机构:
[Zhang, Lizhi; Li, Feng; Zhou, Hongbin; Cheng, Jing; Ding, Kerong; Cai, Cuicui] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构:
[Cheng, Jing] C;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
关键词:
Iron-ferric oxide/graphene oxide composite;Magnetic solid-phase extraction;Magnetic sorbent;Scanning electron microscopy;Transmission electron microscopy;High performance liquid chromatography;Environmental analysis
摘要:
We describe a novel magnetic nanosorbent that consists of nanowires consisting of a core of metallic iron and an iron (III) oxide shell. These nanowires were then deposited on graphene oxide to form a composite of the type [email protected]2O3/GO. Specifically, the magnetic composite is formed via electrostatic interaction between negatively charged GO nanosheets and positively charged [email protected]2O3 nanowires in aqueous solution. The material was successfully applied to the extraction of the endocrine-disrupting phenols bisphenol A, triclosan and 2,4-dichlorophenol from water samples. Compared to neat graphene oxide, the composite material exhibits improved properties in terms of microextraction where both the hydrophilic graphene oxide and the [email protected]2O3 nanowires participate in the adsorption of the hydrophilic analytes. The amount of adsorbent, pH of water sample, extraction time and desorption time, type and volume of desorption solution were optimized. Following extraction for the absorbent, the phenols were quantified by HPLC. The three phenols can be determined in 0.5 to 100 ng∙mL−1 concentration range, with limits of detection (at an S/N ratio of 3) ranging from 0.08 to 0.10 ng∙mL−1. The repeatability was investigated by evaluating the intra- and inter-day precisions with relative standard deviations of lower than 7.5 % (n = 5). The recoveries from spiked real water samples were in the range from 84.8 to 92.0 %. The results indicate that the novel material can be successfully applied to the extraction and analysis of phenols from water samples. [Figure not available: see fulltext.] © 2015, Springer-Verlag Wien.
语种:
英文
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Insight into core-shell dependent anoxic Cr(VI) removal with Fe@Fe2O3 nanowires: Indispensable role of surface bound Fe(II)
作者:
Mu, Yi;Ai, Zhihui* ;Zhang, Lizhi;Song, Fahui
期刊:
ACS Applied Materials & Interfaces ,2015年7(3):1997-2005 ISSN:1944-8244
通讯作者:
Ai, Zhihui
作者机构:
[Zhang, Lizhi; Mu, Yi; Ai, Zhihui; Song, Fahui] Cent China Normal Univ, Inst Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构:
[Ai, Zhihui] C;Cent China Normal Univ, Inst Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
关键词:
Cr(VI) removal;adsorption;anoxic;core-shell [email protected]2O3 nanowires;surface bound Fe(II)
摘要:
In this study, we investigated the anoxic Cr(VI) removal with core-shell Fe@Fe2O3 nanowires. It was found the surface area normalized Cr(VI) removal rate constants of Fe@Fe2O3 nanowires first increased with increasing the iron oxide shell thickness and then decreased, suggesting that Fe@Fe2O3 nanowires possessed an interesting core-shell structure dependent Cr(VI) removal property. Meanwhile, the Cr(VI) removal efficiency was positively correlated to the amount of surface bound Fe(II). This result revealed that the core-shell structure dependent Cr(VI) removal property of Fe@Fe2O3 nanowires was mainly attributed to the reduction of Cr(VI) by the surface bound Fe(II) besides the reduction of Cr(VI) adsorbed on the iron oxide shell via the electrons transferred from the iron core. The indispensable role of surface bound Fe(II) was confirmed by Tafel polarization and high-resolution X-ray photoelectron spectroscopic depth profiles analyses. X-ray diffraction patterns and scanning electron microscope images of the fresh and used Fe@Fe2O3 nanowires revealed the formation of Fe(III)/Cr(III)/Cr(VI) composite oxides during the anoxic Cr(VI) removal process. This study sheds a deep insight into the anoxic Cr(VI) removal mechanism of core-shell Fe@Fe2O3 nanowires and also provides an efficient Cr(VI) removal method. © 2014 American Chemical Society.
语种:
英文
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Molecularly imprinted ultrathin graphitic carbon nitride nanosheets-Based electrochemiluminescence sensing probe for sensitive detection of perfluorooctanoic acid
作者:
Chen, Sihua;Li, Aimin;Zhang, Lizhi;Gong, Jingming*
期刊:
Analytica Chimica Acta ,2015年896:68-77 ISSN:0003-2670
通讯作者:
Gong, Jingming
作者机构:
[Zhang, Lizhi; Gong, Jingming; Li, Aimin; Chen, Sihua] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, 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, Peoples R China.
关键词:
Electrochemiluminescence sensor;Molecularly imprinted polymer;Perfluorooctanoic acid;Ultrathin graphitic carbon nitride nanosheet
摘要:
Driven by the urgent demand for the determination of low level perfluorooctanoic acid (PFOA) present in environment, a novel electrochemiluminescence (ECL) sensor has been first developed for the detection of PFOA using the molecularly imprinted polypyrrole modified two-dimensional ultrathin g-C<inf>3</inf>N<inf>4</inf>(utg-C<inf>3</inf>N<inf>4</inf>) nanosheets as a cathodic ECL emitter with S<inf>2</inf>O<inf>8</inf><sup>2-</sup>as coreactant. The prepared molecularly imprinted polymer (MIP) functionalized utg-C<inf>3</inf>N<inf>4</inf>nanosheets (MIP@utg-C<inf>3</inf>N<inf>4</inf>) exhibit a stable and significantly amplified ECL signal. It is found that the targets of PFOA could be efficiently oxidized by the electro-generated strong oxidants of SO<inf>4</inf><sup>-</sup>(from the reduction of coreactant S<inf>2</inf>O<inf>8</inf><sup>2-</sup>), thus leading to a low yield of the excited utg-C<inf>3</inf>N<inf>4</inf>(g-C<inf>3</inf>N<inf>4</inf>*) and finally a decrease in ECL signal. Based on this, a highly sensitive and selective MIP@utg-C<inf>3</inf>N<inf>4</inf>-based signal-off ECL sensor is developed for sensing PFOA. Such a newly designed ECL sensor exhibits highly linear over the PFOA concentration in two ranges, from 0.02 to 40.0 ng mL<sup>-1</sup>and 50.0-400.0 ng mL<sup>-1</sup>. The detection limit (S/N = 3) is estimated to be 0.01 ng mL<sup>-1</sup>(i.e. 0.01 ppb), comparable to the results obtained by using well-established liquid chromatography-tandem mass spectrometry (LC-MS/MS). Toward practical applications, this low-cost and sensitive assay was successfully applied to measure PFOA in real water samples, showing fine applicability for the detection of PFOA in real samples. ©2015 Elsevier B.V.
语种:
英文
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Facet-level mechanistic insights into general homogeneous carbon doping for enhanced solar-to-hydrogen conversion
作者:
Li, Jie* ;Zhao, Kun;Yu, Ying;Zhang, Lizhi
期刊:
Advanced Functional Materials ,2015年25(14):2189-2201 ISSN:1616-301X
通讯作者:
Li, Jie
作者机构:
[Zhang, Lizhi; Li, Jie; Zhao, Kun] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Li, Jie; Yu, Ying] Cent China Normal Univ, Coll Phys Sci & Technol, Inst Nanosci & Nanotechnol, Wuhan 430079, Peoples R China.
通讯机构:
[Li, Jie] C;Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词:
BiOCl;carbon doping;facet exposure;photocatalysis;solar-to-hydrogen conversion
摘要:
Homogeneous doping can boost solar-to-hydrogen conversion and therefore attracts great attention. Although a great deal of effort has been made to explore the doping-photoreactivity relationship, the doping mechanisms, especially from the perspective of crystal facets, are seldom explored. In this study, a general homogeneous carbon doping strategy is established and then serves as the doping model for a mechanistic investigation, as encouraged by its versatility in enabling homogeneous incorporation of carbon and improving solar-to-hydrogen conversion for typical oxides including TiO2, ZnO, and BiOCl. Using well-defined BiOCl nanosheets of high {001} or {010} facet exposure, we clarify the homogeneous carbon doping mechanism at the level of crystal facets for the first time. This mechanism involves the initial facet-dependent adsorption of the dopant precursor, regulated by the surface atomic structures, and the subsequent facet-dependent diffusion of carbon dopants associated with the facet-related arrangements of bulk atoms. This results in facet-dependent carbon doping behavior and a dopant-concentration-dependent solar-to-hydrogen conversion property of BiOCl nanosheets. These mechanistic insights also suggest that the implantation of the dopant precursor in the shallow lattice of host nanocrystal is vital for the effective homogeneous doping. This new doping model is different from the conventional counterpart based on the organic ligands or gas molecules adsorption onto the surface of host nanocrystals, where surface doping usually occurs. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
语种:
英文
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磷酸根促进Fe@Fe2O3纳米线生成活性氧物种的机理研究
作者:
穆毅;艾智慧;张礼知
作者机构:
[穆毅; 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:
2015-11-20
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>1.引言近年来,零价纳米铁的在环境治理领域的研究和应用引起了人们越来越多的关注,Fe@Fe2O3纳米线是一种常见的零价纳米铁,它具有比表面积大,活性高,还原能力强等优点(1-2)。但是Fe@Fe2O3纳米线产生具有氧化活性的活性氧物种(H2O2,·OH,·O2-)的效率太低,限制了它的应用前景(3)。本研究发现当磷酸根加入体系中以后,大大促进了Fe@Fe2O3纳米线
语种:
中文
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Construction of flexible photoelectrochemical solar cells based on ordered nanostructural BiOI/Bi2S3 heterojunction films
作者:
Fang, Mingqing;Jia, Huimin;He, Weiwei;Lei, Yan;Zhang, Lizhi* ;...
期刊:
PHYSICAL CHEMISTRY CHEMICAL PHYSICS ,2015年17(20):13531-13538 ISSN:1463-9076
通讯作者:
Zhang, Lizhi
作者机构:
[Fang, Mingqing; Lei, Yan; Zheng, Zhi; He, Weiwei; Jia, Huimin] Xuchang Univ, Key Lab Micronano Mat Energy Storage & Convers He, Henan 461000, Peoples R China.;[Fang, Mingqing; Lei, Yan; Zheng, Zhi; He, Weiwei; Jia, Huimin] Xuchang Univ, Inst Surface Micro & Nano Mat, Henan 461000, Peoples R China.;[Fang, Mingqing; Zhang, Lizhi] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要:
Ordered 2D nanostructural BiOI nanoflake arrays decorated with Bi2S3 nanospheres have been designed and in situ fabricated for the first time, to form BiOI/Bi2S3 bulk heterojunctions through a soft chemical route. A modified successive ionic layer adsorption and reaction (SILAR) method was developed to fabricate BiOI nanoflake arrays on flexible ITO/PET substrates at room temperature. The degree of transformation of BiOI to Bi2S3 was controlled through the adjustment of exposure time of the BiOI/ITO substrate to thioacetamide (TAA) aqueous solution. The morphologies of BiOI, BiOI/Bi2S3 heterojunctions and Bi2S3 films were examined by scanning electron microscopy (SEM), X-ray powder diffraction (XRD) patterns, and high resolution transmission electron microscopy (HRTEM). The presence of Bi2S3 was further validated through Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). Especially, photoelectrochemical measurements demonstrated that such a Bi2S3 decorated BiOI photoanode based cell exhibits significant augments of short-circuit current density (J(sc)) and incident photon-to-current conversion efficiency (IPCE, 3 times higher than the pure BiOI photoanode), attributable to the stronger photo-absorption and better photogenerated charge carrier separation and transport efficiency. The surface photovoltage (SPV) measurements further confirmed the importance of BiOI/Bi2S3 heterojunctions in such PEC cells. This solution-based process directly on flexible ITO offers the promise for low-cost, large-area, roll-to-roll application of the manufacturing of the third generation thin-film photovoltaic devices.
语种:
英文
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抗坏血酸/Fe@Fe2O3异相Fenton体系降解甲草胺的研究
作者:
侯晓静;黄小鹏;艾智慧;张礼知
作者机构:
[侯晓静; 黄小鹏; 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:
2015-11-20
会议地点:
中国湖南长沙
摘要:
<正>Fenton反应因其速率快、低毒性、操作简单易控而被广泛用于污染物的降解,但其大规模工业应用却受到很大限制。这主要是由于其工作范围窄(p H-23)和H2O2需求量大以及反应过程中Fe2+氧化沉积导致的铁泥。为了克服这些缺点,近年来很多科研研究者将Fenton反应与其它高级氧化过程耦合,如E-Fenton、UV-Fenton等,但这些耦合过程导致成本大幅
语种:
中文
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Substrate-dependent photoreactivities of BiOBr nanoplates prepared at different pH values
作者:
Ai, Zhihui;Wang, Jilin;Zhang, Lizhi*
期刊:
催化学报 ,2015年36(12):2145-2154 ISSN:0253-9837
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Wang, Jilin; Ai, Zhihui] Cent China Normal Univ, 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, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词:
Degradation;Visible light;Substrate dependent photoreactivity;Bismuth oxybromide nanoplate;Rhodamine B;Salicylic acid
摘要:
In this study, we showed that BiOBr nanoplates prepared at different pH values have substrate-dependent photocatalytic activities under visible-light irradiation. The BiOBr nanoplates synthesized at pH 1 (BOB-1) degraded salicylic acid more effectively than did those obtained at pH 3 (BOB-3), but the order of their photocatalytic activities in rhodamine B (RhB) degradation were reversed. Electrochemical Mott-Schottky and zeta-potential measurements showed that BOB-1 had a more positive valence band and lower surface charge, leading to superior photocatalytic activity in salicylic acid degradation under visible light. However, BOB-3 was more powerful in RhB degradation because larger numbers of superoxide radicals were generated via electron injection from the excited RhB to its more negative conduction band under visible-light irradiation; this was confirmed using active oxygen species measurements and electron spin resonance analysis. This study deepens our understanding of the origins of organic-pollutant-dependent photoreactivities of semiconductors, and will help in designing highly active photocatalysts for environmental remediation. © 2015, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
语种:
英文
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α-Fe2O3表面限域亚铁离子高效Fenton氧化降解污染物
作者:
黄小鹏;侯晓静;赵进才;张礼知
作者机构:
[黄小鹏; 侯晓静; 赵进才; 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:
2015-01-01
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>由于人类社会的高速发展,导致的环境污染问题越来越严重,其中水污染问题显得很突出。在众多有机废水治理的方法中,高级氧化技术因其高效的氧化难降解和彻底矿化有机物的能力而备受关注,而Fenton反应就是一种被广泛应用的高级氧化技术。Fenton反应一般是Fe2+和H2O2反应,产生具有极强氧化能力的羟基自由基,它能够无选择地氧化有毒有机污染物。Fenton反应效率强烈依赖于pH值。而Fe
语种:
中文
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Efficient remediation of pentachlorophenol contaminated soil with tetrapolyphosphate washing and subsequent ZVI/Air treatment
作者:
Cao, Menghua;Wang, Li;Ai, Zhihui* ;Zhang, Lizhi
期刊:
Journal of Hazardous Materials ,2015年292:27-33 ISSN:0304-3894
通讯作者:
Ai, Zhihui
作者机构:
[Cao, Menghua; Zhang, Lizhi; Wang, Li; Ai, Zhihui] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构:
[Ai, Zhihui] C;Cent China Normal Univ, Coll Chem, Inst Environm Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
关键词:
Molecular oxygen activation;Pentachlorophenol;Soil washing;Tetrapolyphosphate;Zerovalent iron
摘要:
In this study, we demonstrate that pentachlorophenol contaminated soil can be efficiently remediated with tetrapolyphosphate washing and subsequent zerovalent iron (ZVI)/Air treatment. 2mmolL(-1) of tetrapolyphosphate could wash away 52.8% of pentachlorophenol (PCP) at pH 7.0 and 84.2% of pentachlorophenol at pH 11.0 from contaminated soil owing to the promotion effect of tetrapolyphosphate on the soil matrix dispersion and the subsequent solubilization of pentachlorophenol. More importantly, tetrapolyphosphate ions remained in the washing effluent could greatly enhance the molecular oxygen activation by ZVI to oxidize the desorbed PCP without any pH adjustment, and also avoid the competitive consumption of reactive oxygen species, as caused by the common organic surfactants in the washing effluent. Therefore, 85.1% of pentachlorophenol could be aerobically removed from the washing effluent by merely using 5gL(-1) of ZVI. We also interestingly found that the dissolved iron ions released from the soil could enhance the oxidation of pentachlorophenol in the washing effluent, but the dissolved organic matter had the opposite effect. This study suggests the coupling tetrapolyphosphate washing and subsequent ZVI/Air treatment is an optional approach to remediate pentachlorophenol contaminated soil in view of its low cost and environmental benign. Copyright © 2015 Elsevier B.V. All rights reserved.
语种:
英文
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高选择性电还原二氧化碳的廉价锌催化体系
作者:
全凤娇;贾法龙;张礼知
作者机构:
[全凤娇; 贾法龙; 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:
2015-01-01
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>1.引言近几十年来,人类在利用化石燃料的同时排放了大量二氧化碳(CO2)气体,日益加剧了温室效应对地球生存环境的负面影响,如何将二氧化碳回收并利用成为了当前一个重要的研究课题。以CO2为碳源,通过还原途径转化为可利用资源为实现CO2的绿色转化提供了思路。而且利用可再生能源所产生的电能,催化CO2转化为CO、甲酸、醇类或碳氢化合物[1-2],特别是电还原过程与太阳能等再生能源系统耦合后
语种:
中文
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Facile synthesis of porous graphene-like carbon nitride (C6 N9 H3 ) with excellent photocatalytic activity for NO removal
作者:
Dong, Guohui;Ho, Wingkei* ;Li, Yuhan;Zhang, Lizhi
期刊:
Applied Catalysis B: Environmental ,2015年174-175:477-485 ISSN:0926-3373
通讯作者:
Ho, Wingkei
作者机构:
[Ho, Wingkei; Dong, Guohui; Li, Yuhan] Hong Kong Inst Educ, Dept Sci & Environm Studies, Tai Po, Hong Kong, Peoples R China.;[Ho, Wingkei; Dong, Guohui; Li, Yuhan] Hong Kong Inst Educ, Ctr Educ Environm Sustainabil, Tai Po, Hong Kong, Peoples R China.;[Zhang, Lizhi; Dong, Guohui] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;[Ho, Wingkei] Chinese Acad Sci, Inst Earth Environm, Key Lab Aerosol Chem & Phys, Xian 710075, Peoples R China.
通讯机构:
[Ho, Wingkei] H;Hong Kong Inst Educ, Dept Sci & Environm Studies, Tai Po, Hong Kong, Peoples R China.
关键词:
C6N9H3;NO removal;Photocatalytic;Porous;Visible light
摘要:
We reported the possible synthesis of a new porous graphene-like carbon nitride (C6N9H3) by simply adding hydrochloric acid in the precursor of block g-C3N4. The formation of the porous graphene-like C6N9H3 can be attributed to the change in the thermal condensation modal of the precursor and the acidic condition induced by Cl- and H+. The photocatalytic activity of the samples was evaluated by the removal of NO under visible light illumination. We found that the porous graphene-like C6N9H3 exhibited enhanced photocatalytic activity compared to the block g-C3N4. We also researched the removal mechanism and found that the removal of NO in our systems was due to the synergic effect of h+ and O2-. This study could shed light on the design of efficient photocatalysts and facilitate a deep understanding of the NO removal mechanism through photocatalytic technology. © 2015 Elsevier B.V.
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英文
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原儿茶酸促进Fe3+/H2O2体系降解甲草胺的研究
作者:
秦雅鑫;张礼知
作者机构:
[秦雅鑫; 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:
2015-11-20
会议地点:
中国湖南长沙
摘要:
<正>甲草胺是一种广泛使用的除草剂,在自然环境中大量残留。由于甲草胺结构稳定,它在土壤和水体中的可半衰期长达70和30天,而且它是一种内分泌干扰素,对环境中的生物及人类健康造成严重危害。[1]Fenton(Fe2+/H2O2和Fe3+/H2O2)体系因其反应速率快,简单易操作和环境友好等特点,受到了广泛关注。Fenton体系能产生具有极强氧化能力的羟基自由基,
语种:
中文
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Hydrothermal Synthesis of FeS2 as a High-Efficiency Fenton Reagent to Degrade Alachlor via Superoxide-Mediated Fe(II)/Fe(III) Cycle
作者:
Liu, Wei;Wang, Yueyao;Ai, Zhihui* ;Zhang, Lizhi
期刊:
ACS Applied Materials & Interfaces ,2015年7(51):28534-28544 ISSN:1944-8244
通讯作者:
Ai, Zhihui
作者机构:
[Zhang, Lizhi; Liu, Wei; Wang, Yueyao; Ai, Zhihui] Cent China Normal Univ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Ai, Zhihui] C;Cent China Normal Univ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
关键词:
FeS2;molecular oxygen activation;superoxide anions;Fe(II)/Fe(III) cycle;alachlor
摘要:
In this study, we demonstrate that hydrothermally synthesized FeS2 (syn-FeS2) is highly efficient at catalyzing the H2O2 decomposition for alachlor degradation at a wide range of initial pH (3.2-9.2). The alachlor degradation rate of syn-FeS2 heterogeneous Fenton system was almost 55 times that of its commercial pyrite (com-FeS2) counterpart at an initial pH of 6.2. Experimental results revealed that the alachlor oxidation enhancement in the syn-FeS2 Fenton system was attributed to the molecular oxygen activation induced by more surface-bound ferrous ions on syn-FeS2. The molecular oxygen activation process could generate superoxide anions to accelerate the Fe(II)/Fe(III) cycle on the syn-FeS2 surface, which favored the H2O2 decomposition to generate more hydroxyl radicals for the alachlor oxidation. It was found that the hydroxyl radicals generation rate constant of syn-FeS2 Fenton system was 71 times that of its com-FeS2 counterpart, and even 1-3 orders of magnitude larger than those of commonly used Fe-bearing heterogeneous catalysts. We detected the alachlor degradation intermediates with gas chromatography-mass spectrometry to propose tentatively a possible alachlor degradation pathway. These interesting findings could provide some new insights on the molecular oxygen activation induced by FeS2 minerals and the subsequent heterogeneous Fenton degradation of organic pollutants in the environment. © 2015 American Chemical Society.
语种:
英文
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Design of a highly efficient and wide ph electro-fenton oxidation system with molecular oxygen activated by ferrous-tetrapolyphosphate complex
作者:
Wang, Li;Cao, Menghua;Ai, Zhihui;Zhang, Lizhi*
期刊:
Environmental Science & Technology ,2015年49(5):3032-3039 ISSN:0013-936X
通讯作者:
Zhang, Lizhi
作者机构:
[Cao, Menghua; Zhang, Lizhi; Wang, Li; Ai, Zhihui] Cent China Normal Univ, Minist Educ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Minist Educ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要:
In this study, a novel electro-Fenton (EF) system was developed with iron wire, activated carbon fiber, and sodium tetrapolyphosphate (Na6TPP) as the anode, cathode, and electrolyte, respectively. This Na6TPP-EF system could efficiently degrade atrazine in a wide pH range of 4.0-10.2. The utilization of Na6TPP instead of Na2SO4 as the electrolyte enhanced the atrazine degradation rate by 130 times at an initial pH of 8.0. This dramatic enhancement was attributed to the formation of ferrous-tetrapolyphosphate (Fe(II)-TPP) complex from the electrochemical corrosion (ECC) and chemical corrosion (CC) of iron electrode in the presence of Na6TPP. The Fe(II)-TPP complex could provide an additional molecular oxygen activation pathway to produce more H2O2 and •OH via a series single-electron transfer processes, producing the Fe(III)-TPP complex. The cycle of Fe(II)/Fe(III) was easily realized through the electrochemical reduction (ECR) process on the cathode. More interestingly, we found that the presence of Na6TPP could prevent the iron electrode from excessive corrosion via phosphorization in the later stage of the Na6TPP-EF process, avoiding the generation of iron sludge. Gas chromatograph-mass spectrometry, liquid chromatography-mass spectrometry, and ion chromatography were used to investigate the degradation intermediates to propose a possible atrazine oxidation pathway in the Na6TPP-EF system. These interesting findings provide some new insight on the development of a low-cost and highly efficient EF system for wastewater treatment in a wide pH range. © 2015 American Chemical Society.
语种:
英文
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Reactive oxygen species dependent degradation pathway of 4-chlorophenol with Fe@Fe2O3 core–shell nanowires
作者:
Huang, Qi;Cao, Menghua;Ai, Zhihui;Zhang, Lizhi*
期刊:
Applied Catalysis B: Environmental ,2015年162:319-326 ISSN:0926-3373
通讯作者:
Zhang, Lizhi
作者机构:
[Cao, Menghua; Zhang, Lizhi; Huang, Qi; Ai, Zhihui] Cent China Normal Univ, Inst Environm Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Inst Environm Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词:
4-Chlorophenol;Degradation mechanism;Diethylenetriaminepentacetate acid;Molecular oxygen activation;Nanoscale zero-valent iron
摘要:
In this study, an environmentally benign polyaminocarboxylic ligand diethylenetriamine pentacetate (DTPA) was first used to promote the aerobic 4-chlorophenol (4-CP) degradation with Fe@Fe2O3 core-shell nanowires, and then compared with the most used counterpart ethylenediamine tetraacetate (EDTA) of poor biodegradability. Although the 4-CP removal rate in the Fe@Fe2O3/DTPA/Air system was slower owing to the preferential degradation of DTPA, the total organic carbon removal rate in the Fe@Fe2O3/DTPA/4-CP/Air system was much faster than that in the Fe@Fe2O3/EDTA/4-CP/Air system. We interestingly found that hydroxyl radicals could more easily react with DTPA to produce DTPA radicals than with EDTA to produce EDTA radicals. Ligands (DTPA or EDTA) could significantly accelerate the hydroxyl radicals production with Fe@Fe2O3, while more hydroxyl radicals were generated in the Fe@Fe2O3/DTPA/Air system. We also employed gas chromatography-mass spectrometry and ion chromatography to detect organic intermediates and chloride ions to probe the 4-chlorophenol degradation pathways, and found its degradation pathways were dependent on the reactive oxygen species generated in the different systems. This study can clarify the roles of polyaminocarboxylic ligands on the molecular oxygen activation with nanoscale zero-valent iron, and also provide a green chlorophenols removal method. © 2014 Elsevier B.V.
语种:
英文
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