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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Efficient visible light nitrogen fixation with BiOBr nanosheets of oxygen vacancies on the exposed {001} Facets
作者:
Li, Hao;Shang, Jian;Ai, Zhihui;Zhang, Lizhi*
期刊:
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY ,2015年137(19):6393-6399 ISSN:0002-7863
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Li, Hao; Ai, Zhihui; Shang, Jian] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
摘要:
Even though the well-established Haber-Bosch process has been the major artificial way to 'fertilize' the earth, its energy-intensive nature has been motivating people to learn from nitrogenase, which can fix atmospheric N<inf>2</inf>to NH<inf>3</inf>in vivo under mild conditions with its precisely arranged proteins. Here we demonstrate that efficient fixation of N<inf>2</inf>to NH<inf>3</inf>can proceed under room temperature and atmospheric pressure in water using visible light illuminated BiOBr nanosheets of oxygen vacancies in the absence of any organic scavengers and precious-metal cocatalysts. The designed catalytic oxygen vacancies of BiOBr nanosheets on the exposed {001} facets, with the availability of localized electrons for-back-donation, have the ability to activate the adsorbed N<inf>2</inf>, which can thus be efficiently reduced to NH<inf>3</inf>by the interfacial electrons transferred from the excited BiOBr nanosheets. This study might open up a new vista to fix atmospheric N<inf>2</inf>to NH<inf>3</inf>through the less energy-demanding photochemical process. ©2015 American Chemical Society.
语种:
英文
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Photocatalytic NO removal on BiOI surface: The change from nonselective oxidation to selective oxidation
作者:
Dong, Guohui;Ho, Wingkei* ;Zhang, Lizhi
期刊:
Applied Catalysis B: Environmental ,2015年168-169:490-496 ISSN:0926-3373
通讯作者:
Ho, Wingkei
作者机构:
[Ho, Wingkei; Dong, Guohui] Hong Kong Inst Educ, Dept Sci & Environm Studies, Tai Po, Hong Kong, Peoples R China.;[Ho, Wingkei; Dong, Guohui] Hong Kong Inst Educ, Ctr Educ Environm Sustainabil, Tai Po, Hong Kong, Peoples R China.;[Ho, Wingkei] Chinese Acad Sci, Inst Earth Environm, Beijing 100864, Peoples R China.;[Zhang, Lizhi; Dong, Guohui] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, 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.
摘要:
Numerous publications have investigated nitric oxide (NO) removal through semiconductor photocatalytic technology. However, few reports are available on the products and mechanisms of the photocatalytic NO removal process. In this study, BiOI hollow microspheres are synthesized for the photocatalytic removal of NO under the visible light irradiation. Results show that NO removal product and NO removal mechanism could interfere with each other. NO removal process could be changed from nonselective oxidation to selective oxidation as the irradiation time increases. Meanwhile, the product of NO removal could be changed from nitrate (NO3-) to nitrogen dioxide (NO2). These interesting changes were attributed to the generated NO3-, which was produced from the reactions between NO and OH. The generated NO3- could inhibit OH generation, thus leading to a change in the NO removal products and NO removal mechanism. This study can improve our understanding of NO removal on the photocatalyst surface and serve as a guide in using photocatalysts for NO removal. © 2015 Elsevier B.V.
语种:
英文
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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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Oxygen vacancy induced selective silver deposition on the {001} facets of BiOCl single-crystalline nanosheets for enhanced Cr(vi) and sodium pentachlorophenate removal under visible light
作者:
Li, Hao;Zhang, Lizhi*
期刊:
Nanoscale ,2014年6(14):7805-7810 ISSN:2040-3364
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Li, Hao] Cent China Normal Univ, Inst Environm Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Inst Environm Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
摘要:
We demonstrate that the high oxygen density characteristic of BiOCl {001} facets ensures the fast generation of oxygen vacancies in ethylene glycol under microwave irradiation, resulting in in situ nucleation and growth of Ag on the {001} facets of BiOCl single-crystalline nanosheets. The resulting Ag selectively deposited BiOCl single-crystalline nanosheets exhibit much higher reactivity and stability on both Cr(VI) reduction and sodium pentachlorophenate oxidation than the randomly deposited counterparts under visible light because of the tight contact between Ag and the {001} facets of BiOCl arisen from oxygen vacancy induced selective silver deposition.
语种:
英文
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Novel visible-light-responsive photoelectrochemical sensor of 2,4-dichlorophenoxyacetic acid using molecularly imprinted polymer/BiOI nanoflake arrays
作者:
Peng, Dinghua;Li, Xue;Zhang, Lizhi;Gong, Jingming*
期刊:
Electrochemistry Communications ,2014年47:9-12 ISSN:1388-2481
通讯作者:
Gong, Jingming
作者机构:
[Peng, Dinghua; Zhang, Lizhi; Gong, Jingming; Li, Xue] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minis Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Gong, Jingming] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minis Educ, Wuhan 430079, Peoples R China.
关键词:
2,4-Dichlorophenoxyacetic acid;Photoelectrochemical sensor;BiOI nanoflake array;Molecularly imprinted polymer
摘要:
A novel and highly sensitive visible-light photoelectrochemical (PEC) sensor for the detection of 2,4-D has been developed using a nanocomposite of molecularly imprinted gold nanoparticles-polypyrrole polymer (MIP) modified BiOI nanoflake arrays (BiOINFs) as a photoactive electrode (labeled as MIP@BiOINFs). Our results demonstrate that the smart combination of BiOINFs with MIP offers a high-performance photoactive sensing platform. It features the intrinsically excellent visible-light responsive properties of BiOI and prominent recognition ability from MIP. The designed MIP@BiOINF composite dramatically facilitates the PEC determination of 2,4-D. The detection limit for 2,4-D is found to be as low as about 0.04 ng mL<sup>- 1</sup> (S/N = 3). Moreover, the resulting sensor could be used to detect 2,4-D in spiked soil samples. ©2014 Published by Elsevier B.V.
语种:
英文
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Synthesis and internal electric field dependent photoreactivity of Bi 3 O4 Cl single-crystalline nanosheets with high {001} facet exposure percentages
作者:
Li, Jie;Zhang, Lizhi* ;Li, Yujie;Yu, Ying
期刊:
Nanoscale ,2014年6(1):167-171 ISSN:2040-3364
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Li, Jie] 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; Li, Yujie] Cent China Normal Univ, Inst Nanosci & Nanotechnol, Coll Phys Sci & Technol, Wuhan 430079, 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, Peoples R China.
摘要:
We prepared Bi3O4Cl single-crystalline nanosheets with high {001} facet exposure percentages and demonstrated that their photoreactivity strongly depended on the magnitude of the internal electric field (IEF), which was correlated with the {001} facet exposure percentage. More {001} facet exposure could induce the generation of stronger IEF, which favored the photogenerated charge separation and transfer, and thus enhancing the photoreactivity.
语种:
英文
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A nonaqueous sol–gel route to highly water dispersible TiO2 nanocrystals with superior photocatalytic performance
作者:
Ai, Zhihui;Wu, Na;Zhang, Lizhi*
期刊:
Catalysis Today ,2014年224:180-187 ISSN:0920-5861
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Ai, Zhihui; Wu, Na] 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:
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Inst Environm Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
会议名称:
4th International Symposium on Environmental Science and Technology (ISEST)
会议时间:
JUN 04-07, 2013
会议地点:
Dalian, PEOPLES R CHINA
会议主办单位:
[Ai, Zhihui;Wu, Na;Zhang, Lizhi] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
关键词:
Photocatalysis;TiO2 nanocrystals;Visible-light;Water dispersible
摘要:
In this study, we report that highly water dispersible TiO2 nanocrystals could be synthesized via a facile nonaqueous sol-gel method using titanium tetrachloride and ethanol as the precursors. The resulting TiO 2 samples were 5-10 nm in diameter according to characterizations with X-ray diffraction, transmission electron microscopy, and high resolution transmission electron microscopy. X-ray photoelectron spectroscopy, thermal gravimetric analysis, and Fourier-transform infrared spectroscopy analysis revealed that carbonaceous species were formed and bound on the surface of TiO2 nanocrystals during the synthesis. These carbonaceous species could prevent the agglomeration of TiO2 nanocrystals and endow the TiO2 nanocrystals with highly water dispersible property and superior photocatalytic activity on the degradation of organic pollutant under visible light irradiation. We believe that the resulting TiO2 nanocrystals with highly water dispersibility and superior photocatalytic activity could find wide applications in many fields. © 2013 Elsevier B.V.
语种:
英文
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Microwave Catalytic Molecular Oxygen Activation to Degrade Dimethyl Phthalate over Fe@Fe2O3/AC
作者:
Yiling Chen;Zhihui Ai;Lizhi Zhang
作者机构:
Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079
会议名称:
第七届全国环境催化与环境材料学术会议
会议时间:
20110812
会议地点:
北京
会议论文集名称:
第七届全国环境催化与环境材料学术会议论文集
关键词:
dimethyl phthalate;molecular oxygen activation;microwave irradiation;Fe@Fe2O3;AC
摘要:
We demonstrate that dimethyl phthalate (DMP) could be rapidly decomposed by microwave irradiation (MW) over Fe@Fe2O3/activated carbon (Fe@Fe2O3/AC) catalyst within 2 min.Active species trapping experiments revealed that the catalytic microwave decomposition of dimethyl phthalate was attributed to an unique microwave induced molecular oxygen activation process.
语种:
英文
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厌氧条件下抗坏血酸降解阿特拉津的动力学与机理研究
作者:
侯晓静;艾智慧;张礼知
作者机构:
[侯晓静; 艾智慧; 张礼知] 华中师范大学化学学院环境化学研究所 武汉 430079
会议名称:
2014年第12届全国水处理化学大会
会议时间:
2014-01-01
会议地点:
中国广东广州
会议主办单位:
中国化学会
会议论文集名称:
2014年第12届全国水处理化学大会暨学术研讨会论文摘要集
摘要:
<正>阿特拉津(Atrazine),是一种人工合成的并在世界范围内广泛使用的三嗪类除草剂。它认为是一种环境雌激素并具有潜在的致癌性,会导致生物内分泌失衡,出现生殖器官畸形,癌症发病率上升等现象。使用阿特拉津所导致的主要环境问题是其使用范围广,残留时间长,难于降解,而且具有土壤淋溶性,易被雨水、灌溉水淋溶至较深层土,或是随地表径流进入河流、湖泊,对地下水和地表水造成污染。世界上具有多年阿特拉津使用历
语种:
中文
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Dramatically enhanced aerobic atrazine degradation with Fe@Fe 2 O3 core-shell nanowires by tetrapolyphosphate
作者:
Wang, Li;Cao, Menghua;Ai, Zhihui;Zhang, Lizhi*
期刊:
Environmental Science & Technology ,2014年48(6):3354-3362 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, Inst Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Inst Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要:
In this study, the effects of an inorganic ligand tetrapolyphosphate on the molecular oxygen activation and the subsequent aerobic atrazine degradation by Fe@Fe2O3 core-shell nanowires were investigated systematically at a circumneutral to alkaline pH range (pH 6.0-9.0). We interestingly found that the addition of tetrapolyphosphate could enhance the aerobic atrazine degradation rate 955 times, which was even 10 times that of the traditional organic ligand ethylenediamine tetraacetate. This tetrapolyphosphate induced dramatic aerobic atrazine degradation enhancement could be attributed to two factors. One was that the presence of tetrapolyphosphate strongly suppressed hydrogen evolution from the reduction of proton by Fe@Fe2O3 core-shell nanowires through proton confinement, leaving over more electrons for the reduction of Fe(III) to Fe(II) and the subsequent molecular oxygen activation. The other was that the complexation of tetrapolyphosphate with ferrous ions not only guaranteed enough soluble Fe(II) for Fenton reaction, but also provided another route to produce more •OH in the solution via the single-electron molecular oxygen reduction pathway. We employed gas chromatography-mass spectrometry and liquid chromatography-mass spectrometry to identify the atrazine degradation intermediates and proposed a possible aerobic atrazine degradation pathway. This study not only sheds light on the promotion effects of ligands on the molecular oxygen activation by nanoscale zerovalent iron, but also offers a facile and green iron-based method for the oxidative atrazine removal. © 2014 American Chemical Society.
语种:
英文
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Fe@Fe2O3 core-shell nanowires enhanced Fenton oxidation by accelerating the Fe(III)/Fe(II) cycles
作者:
Shi, Jingu;Ai, Zhihui* ;Zhang, Lizhi
期刊:
Water Research ,2014年59:145-153 ISSN:0043-1354
通讯作者:
Ai, Zhihui
作者机构:
[Zhang, Lizhi; Shi, Jingu; Ai, Zhihui] Cent China Normal Univ, Inst Environm Chem, Key Lab Pesticide & Chem Biol, Coll Chem,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, Coll Chem,Minist Educ, Wuhan 430079, Peoples R China.
关键词:
Fe@Fe(2)O(3) nanowires;Fenton oxidation;Iron cycling;Molecular oxygen activation;Rhodamine B
摘要:
In this study we demonstrate Fe@Fe<inf>2</inf>O<inf>3</inf> core-shell nanowires can improve Fenton oxidation efficiency by two times with rhodamine B as a model pollutant at pH>4. Active species trapping experiments revealed that the rhodamine B oxidation enhancement was attributed to molecular oxygen activation induced by Fe@Fe<inf>2</inf>O<inf>3</inf> core-shell nanowires. The molecular oxygen activation process could generate superoxide radicals to assist iron core for the reduction of ferric ions to accelerate the Fe(III)/Fe(II) cycles, which favored the H<inf>2</inf>O<inf>2</inf> decomposition to produce more hydroxyl radicals for the rhodamine B oxidation. The combination of Fe@Fe<inf>2</inf>O<inf>3</inf> core-shell nanowires and ferrous ions (Fe@Fe<inf>2</inf>O<inf>3</inf>/Fe<sup>2+</sup>) offered a superior Fenton catalyst to decompose H<inf>2</inf>O<inf>2</inf> for producing OH. We employed benzoic acid as a probe reagent to check the generation of OH and found the OH generation rate of Fe@Fe<inf>2</inf>O<inf>3</inf>/Fe<sup>2+</sup> was 2-4 orders of magnitude larger than those of commonly used iron based Fenton catalysts and 38 times that of Fe<sup>2+</sup>. The reusability and the stability of Fe@Fe<inf>2</inf>O<inf>3</inf> core-shell nanowires were studied. Total organic carbon and ion chromatography analyses revealed the mineralization of rhodamine B and the releasing of nitrate ions. Gas chromatograph-mass spectrometry was used to investigate the degradation intermediates to propose the possible rhodamine B Fenton oxidation pathway in the presence of Fe@Fe<inf>2</inf>O<inf>3</inf> nanowires. This study not only provides a new Fenton oxidation system for pollutant control, but also widenthe application of molecular oxygen activation induced by nanoscale zero valent iron. ©2014 Elsevier Ltd.
语种:
英文
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Anoxic and oxic removal of humic acids with Fe@Fe2O3 core–shell nanowires: A comparative study
作者:
Wu, Hao;Ai, Zhihui* ;Zhang, Lizhi
期刊:
Water Research ,2014年52:92-100 ISSN:0043-1354
通讯作者:
Ai, Zhihui
作者机构:
[Zhang, Lizhi; Wu, Hao; Ai, Zhihui] Cent China Normal Univ, Inst Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol,Coll Chem, 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,Coll Chem, Wuhan 430079, Peoples R China.
关键词:
Adsorption;Fe@Fe(2)O(3) core-shell nanowires;Humic acids;Molecular oxygen activation;Oxidation;Removal
摘要:
In this study we comparatively investigate the removal of humic acids with Fe@Fe2O3 core-shell nanowires under anoxic and oxic conditions. The products of humic acids after reacting with Fe@Fe2O3 core-shell nanowires under anoxic and oxic conditions were carefully examined with three-dimensional excitation emission matrix fluorescence spectroscopy and gas chromatography mass spectrometry. It was found that humic acids were removed by Fe@Fe2O3 core-shell nanowires via adsorption under anoxic condition. Langmuir adsorption isotherm was applicable to describe the adsorption processes. Kinetics of humic acids adsorption onto Fe@Fe2O3 core-shell nanowires was found to follow pseudo-second-order rate equation. By contrast, the oxic removal of humic acids with Fe@Fe2O3 core-shell nanowires involved adsorption and subsequent oxidation of humic acids because Fe@Fe2O3 core-shell nanowires could activate molecular oxygen to produce reactive oxygen species to oxidize humic acids. This subsequent oxidation of humic acids could improve the oxic removal rate to 2.5 times that of anoxic removal, accompanying with about 8.4% of mineralization. This study provides a new method for humic acids removal and also sheds light on the effects of humic acids on the pollutant removal by nano zero-valent iron.
语种:
英文
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Ferrous ions promoted aerobic simazine degradation with Fe@Fe2O3 core–shell nanowires
作者:
Liu, Wei;Ai, Zhihui;Cao, Menghua;Zhang, Lizhi*
期刊:
Applied Catalysis B: Environmental ,2014年150-151:1-11 ISSN:0926-3373
通讯作者:
Zhang, Lizhi
作者机构:
[Cao, Menghua; Zhang, Lizhi; Liu, Wei; Ai, Zhihui] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm Chem,Coll Chem, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm Chem,Coll Chem, Wuhan 430079, Peoples R China.
关键词:
Molecular oxygen activation;Simazine;Surface bound ferrous ions;Surface hydroxyl radicals;[email protected]2O3 nanowires
摘要:
In this study, we investigated the effect of extra ferrous ions on the aerobic simazine degradation with Fe@Fe<inf>2</inf>O<inf>3</inf> core-shell nanowires at circumneutral pH and interestingly found that ferrous ions could promote the aerobic simazine degradation efficiency of nanowires by about 5 times. The aerobic simazine degradation improvement was realized by maintaining enough dissolved ferrous ions and enhancing single-electron reduction molecular oxygen activation via providing more surface bound ferrous ions on the iron oxide shell. These increased surface bound ferrous ions could produce more surface hydroxyl radicals to enhance the simazine degradation. The 2,2'-bipytridine inhibition and reactive oxygen species detection results revealed that the contribution of sequential single-electron molecular oxygen activation by surface bound ferrous ions to reactive oxygen species production was more than 60%, higher than that of two-electron molecular oxygen activation pathway. We determined the degradation intermediates of simazine with high performance liquid chromatography-mass spectrometry and gas chromatography-mass spectrometry to tentatively propose a possible simazine degradation pathway. These interesting findings could provide new insight on nanoscale zero valent iron induced molecular oxygen activation and its aerobic removal of organic pollutants at circumneutral pH. ©2013 Elsevier B.V.
语种:
英文
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激光拉曼检测气体的新方法
作者:
王梦兰;贾法龙;张礼知
作者机构:
华中师范大学 化学学院,武汉 430079
会议名称:
2014年全国化学与光谱分析会议
会议时间:
2014-09-01
会议地点:
太原
会议论文集名称:
2014年全国化学与光谱分析会议论文集
关键词:
气体检测;激光拉曼技术;石英毛细管;镀金工艺;信号强度
摘要:
利用石英毛细管作为气体拉曼检测的样品室,为了增强气体的拉曼信号,尝试了镀金石英毛细管并开发出可行的镀金工艺.结果表明:在石英内壁沉积了200nm厚度的金膜后,氮气的拉曼信号增强了近5倍,为今后进一步实现气体在线拉曼监测奠定了基础.
语种:
中文
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Sustainable molecular oxygen activation with oxygen vacancies on the {001} facets of BiOCl nanosheets under solar light
作者:
Li, Hao;Shi, Jingu;Zhao, Kun;Zhang, Lizhi*
期刊:
Nanoscale ,2014年6(23):14168-14173 ISSN:2040-3364
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Li, Hao; Shi, Jingu; Zhao, Kun] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
摘要:
We demonstrate that oxygen vacancies on the {001} facets of BiOCl nanosheets can more sustainably activate molecular oxygen for organic pollutant removal under solar light than the TiO2 counterparts. The oxygen vacancies on the {001} facets of BiOCl nanosheets are effectively refreshed by UV light, and are also responsible for the efficient utilization of visible light to activate molecular oxygen, accounting for their long term stability and high efficiency.
语种:
英文
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Enhanced selectivity for the electrochemical reduction of CO2 to alcohols in aqueous solution with nanostructured Cu-Au alloy as catalyst
作者:
Jia, Falong* ;Yu, Xinxing;Zhang, Lizhi
期刊:
Journal of Power Sources ,2014年252(Apr.15):85-89 ISSN:0378-7753
通讯作者:
Jia, Falong
作者机构:
[Zhang, Lizhi; Yu, Xinxing; Jia, Falong] 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.
关键词:
Carbon dioxide;Electrochemical reduction;Copper-gold alloy;Nanostructure
摘要:
Electrochemical reduction of CO<inf>2</inf> in an aqueous 0.5 M KHCO <inf>3</inf> solution is studied by use of novel nanostructured Cu-Au alloys, which are prepared through electrochemical deposition with a nanoporous Cu film (NCF) as template. Linear voltammetry results show that the as-synthesized Cu-Au alloys exhibit obvious catalysis towards electrochemical reduction of CO <inf>2</inf>. Further analysis of products reveals that faradic efficiencies of alcohols (methanol and ethanol) are greatly dependent on the nanostructures and compositions of Cu-Au alloys. It is expected that this work could provide new insight into the development of powerful electrocatalysts for reduction of CO<inf>2</inf> to alcohols. ©2013 Elsevier B.V. All rights reserved.
语种:
英文
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Total aerobic destruction of azo contaminants with nanoscale zero-valent copper at neutral pH: Promotion effect of in-situ generated carbon center radicals
作者:
Dong, Guohui;Ai, Zhihui* ;Zhang, Lizhi
期刊:
Water Research ,2014年66:22-30 ISSN:0043-1354
通讯作者:
Ai, Zhihui
作者机构:
[Zhang, Lizhi; Dong, Guohui; Ai, Zhihui] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Ai, Zhihui] 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:
Azo contaminants;Carbon center radicals;Molecular oxygen activation;Nanoscale zero-valent copper
摘要:
In this study, nanoscale zero-valent copper (nZVC) was synthesized with a facile solvothermal method and used for the aerobic removal of azo contaminants at neutral pH for the first time. We found that both Cu(I) and OH generated during the nZVC induced molecular oxygen activation process accounted for the rapid total destruction of azo contaminants in the nZVC/Air system, where nZVC could activate molecular oxygen to produce H<inf>2</inf>O<inf>2</inf>, and also release Cu(I) to break the -NN- bond of azo contaminants via the sandmeyer reaction for the generation of carbon center radicals. The in-situ generated carbon center radicals would then react with OH produced by the Cu(I) catalyzed decomposition of H<inf>2</inf>O<inf>2</inf>, resulting in the generation of low molecular weight organic acids and their subsequent mineralization. The indispensible role of Cu(I) catalyzed sandmeyer reaction and the promotion effect of in-situ generated carbon center radicals on the rapid total destruction of azo contaminants in the nZVC/Air system were confirmed by gas chromatography-mass spectrometry analysis. This study can deepen our understanding on the degradation of organic pollutant with molecular oxygen activated by zero valent metal, and also provide a new method to remove azo contaminants at neutral pH. ©2014 Elsevier Ltd.
语种:
英文
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