Highly efficient electrochemical conversion of CO2 and NaCl to CO and NaClO
作者:
Quan, Fengjiao;Zhan, Guangming;Shang, Huan;Huang, Yahui;Jia, Falong* ;...
期刊:
Green Chemistry ,2019年21(12):3256-3262 ISSN:1463-9262
通讯作者:
Jia, Falong;Ai, Zhihui
作者机构:
[Quan, Fengjiao; Zhang, Lizhi; Huang, Yahui; Shang, Huan; Jia, Falong; Ai, ZH; Zhan, Guangming; Ai, Zhihui] 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:
[Jia, FL; Ai, ZH] 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:
A robust electrocatalyst based on single iron atoms was developed for CO2 reduction with a high faradaic efficiency over 99.6%. The cathodic CO2 reduction was then coupled with anodic production of hypochlorite, and high energy efficiency (82%) with nearly 100% atom economy could be achieved in this model electrolysis system. © 2019 The Royal Society of Chemistry.
语种:
英文
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Fast transformation of roxarsone into toxic arsenic species with ferrous iron and tetrapolyphosphate
作者:
Chen, Na;Wan, Yichao;Ai, Zhihui;Jia, Falong* ;Zhang, Lizhi
期刊:
Environmental Chemistry Letters ,2019年17(2):1077-1084 ISSN:1610-3653
通讯作者:
Jia, Falong
作者机构:
[Zhang, Lizhi; Chen, Na; Ai, Zhihui; Jia, Falong; Wan, Yichao] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Inst Environm Chem, Minist Educ,Coll Chem, Wuhan 430079, Hubei, Peoples R China.
通讯机构:
[Jia, Falong] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Inst Environm Chem, Minist Educ,Coll Chem, Wuhan 430079, Hubei, Peoples R China.
关键词:
Roxarsone;Transformation;Molecule oxygen activation;Ferrous-tetrapolyphosphate complex
摘要:
Organoarsenic compounds have been widely used as feed additives in livestock and poultry breeding. They are excreted in manure and thus cause environmental pollution. Moreover, organoarsenic compounds can be transformed into other arsenic species with higher toxicity. There is little knowledge on the transformation of organoarsenic compounds in the presence of iron species. Here, we studied the transformation of roxarsone (4-hydroxy-3-nitrophenylarsonic acid) in the presence of ferrous ion (Fe(II)) and tetrapolyphosphate. Various generated arsenic species were monitored. Results show that 94.8% of roxarsone was degraded within 30min in 10mmolL(-1) Fe(II) and 50mmolL(-1) tetrapolyphosphate under air atmosphere. 70%of roxarsone arsenic was converted to As(V) species by hydroxyl radicals generated in the air system. Moreover, roxarsone is reductively transformed into other organoarsenic compounds, for example 4-hydroxy-3-aminophenylarsonic acid, by accepting electrons from the Fe(II)-tetrapolyphosphate complex. The toxicity and mobility of the generated inorganic or organic arsenic species are higher than those of roxarsone, which may induce serious environment and human health problems.
语种:
英文
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Rapid Aerobic Inactivation and Facile Removal of Escherichia coli with Amorphous Zero-Valent Iron Microspheres: Indispensable Roles of Reactive Oxygen Species and Iron Corrosion Products.
作者:
Sun, Hongwei;Wang, Jian;Jiang, Yao;Shen, Wenjuan;Jia, Falong* ;...
期刊:
Environmental Science & Technology ,2019年53(7):3707-3717 ISSN:0013-936X
通讯作者:
Jia, Falong;Zhang, Lizhi;Liao, Xiaomei
作者机构:
[Zhang, Lizhi; Sun, Hongwei; Shen, Wenjuan; Jia, Falong; Zhang, LZ] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Wang, Jian; Jiang, Yao; Liao, Xiaomei; Wang, Shaohui] Cent China Normal Univ, Sch Life Sci, Hubei Key Lab Genet Regulat & Integrat Biol, Wuhan 430079, Hubei, Peoples R China.
通讯机构:
[Jia, FL; Zhang, LZ; Liao, Xiaomei] C;Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;Cent China Normal Univ, Sch Life Sci, Hubei Key Lab Genet Regulat & Integrat Biol, Wuhan 430079, Hubei, Peoples R China.
摘要:
Zero valent iron (ZVI) is recently regarded as a promising alternative for water disinfection, but still suffers from low efficiency. Herein we demonstrate that amorphous zerovalent iron microspheres (A-mZVI) exhibit both higher inactivation rate and physical removal efficiency for the disinfection of Escherichia coli than conventional crystalline nanoscale ZVI (C-nZVI) under aerobic condition. The enhanced E. coli inactivation performance of A-mZVI was mainly attributed to more reactive oxygen species (ROSs), especially free •OH, generated by the accelerated iron dissolution and molecular oxygen activation in bulk solution. In contrast, C-nZVI preferred to produce surface bound •OH, and its bactericidal ability was thus hampered by the limited physical contact between C-nZVI and E. coli. More importantly, hydrolysis of dissolved iron released from A-mZVI produced plenty of loose FeOOH to wrap E. coli, increasing the dysfunction of E. coli membrane. Meanwhile, this hydrolysis process lowered the stability of E. coli colloid and caused its rapid coagulation and sedimentation, favoring its physical removal. These findings clarify the indispensable roles of ROSs and iron corrosion products during the ZVI disinfection, and also provide a promising disinfection material for water treatment. Copyright © 2019 American Chemical Society.
语种:
英文
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基于表面铁循环调控的高效表面Fenton反应体系构建
作者:
侯晓静;黄小鹏;贾法龙;艾智慧;赵进才;...
作者机构:
华中师范大学化学学院 武汉430079
会议名称:
第九届全国环境化学大会
会议时间:
20171019
会议地点:
杭州
会议论文集名称:
第九届全国环境化学大会论文集
摘要:
实现高效铁循环是提高 Fenton 氧化技术效率的关键所在.在传统 Fenton(Fe2+/H2O2)体系中,亚铁离子和双氧水(H2O2)反应(76 M-1s-1)产生强氧化性羟基自由基(·OH)和三价铁离子,而三价铁离子与 H2O2 反应(0.02 M-1s-1)再生成亚铁的过程是非常缓慢的,使得体系中铁循环效率较低,导致 H2O2 不能持续分解利用率低.
语种:
中文
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Liquid Nitrogen Activation of Zero-Valent Iron and Its Enhanced Cr(VI) Removal Performance
作者:
Hu, Yue;Peng, Xing;Ai, Zhihui;Jia, Falong* ;Zhang, Lizhi*
期刊:
Environmental Science & Technology ,2019年53(14):8333-8341 ISSN:0013-936X
通讯作者:
Jia, Falong;Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Peng, Xing; Hu, Yue; Ai, Zhihui; Jia, Falong; Zhang, LZ] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构:
[Jia, FL; Zhang, LZ] C;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
摘要:
In this study, we report that liquid nitrogen treatment is a promising zero-valent iron activation method that does not remove the iron oxide shell; this can improve the apparent Cr(VI) removal rate constant of zero-valent iron by about 4-120 times, depending on the particle sizes and the suppliers of zero-valent iron. It was found that liquid nitrogen, with its low temperature of 77 K, could crack the iron oxide shell of zero-valent iron to produce abundant fractures because of the different thermal expansion coefficients of iron oxide and iron. These fractures provided suitable mass transfer channels for the inward transfer of water/oxygen molecules to the iron core and the subsequent in situ generation of Fe(II) for the reduction of Cr(VI) to Cr(III). More importantly, systematic characterizations confirmed the generation of an Fe(III)/Cr(III)/Cr(VI) composite on the surface of zero-valent iron during the removal, suggesting its environmental benignancy. This study provides a novel physical zero-valent iron activation method, sheds light on the importance of the iron oxide shell of zero-valent iron on Cr(VI) removal, and clarifies the intrinsic Cr(VI) removal mechanism of zero-valent iron. © 2019 American Chemical Society.
语种:
英文
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Oxygen Vacancy-Mediated Photocatalysis of BiOCl: Reactivity, Selectivity, and Perspectives
作者:
Li, Hao;Li, Jie;Ai, Zhihui;Jia, Falong;Zhang, Lizhi*
期刊:
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION ,2018年57(1):122-138 ISSN:1433-7851
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Li, Hao; Li, Jie; Ai, Zhihui; Jia, Falong] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词:
BiOCl;nitrogen fixation;oxygen activation;photocatalysis;water splitting
摘要:
Semiconductor photocatalysis is a trustworthy approach to harvest clean solar light for energy conversions, while state-of-the-art catalytic efficiencies are unsatisfactory because of the finite light response and/or recombination of robust charge carriers. Along with the development of modern material characterization techniques and electronic-structure computations, oxygen vacancies (OVs) on the surface of real photocatalysts, even in infinitesimal concentration, are found to play a more decisive role in determining the kinetics, energetics, and mechanisms of photocatalytic reactions. This Review endeavors to clarify the inherent functionality of OVs in photocatalysis at the surface molecular level using 2D BiOCl as the platform. Structure sensitivity of OVs on reactivity and selectivity of photocatalytic reactions is intensely discussed via confining OVs onto prototypical BiOCl surfaces of different structures. The critical understanding of OVs chemistry can help consolidate and advance the fundamental theories of photocatalysis, and also offer new perspectives and guidelines for the rational design of catalysts with satisfactory performance. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
语种:
英文
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Efficient light-driven CO2 hydrogenation on Ru/CeO2 catalysts
作者:
Quan, Fengjiao;Zhan, Guangming;Mao, Chengliang;Ai, Zhihui;Jia, Falong* ;...
期刊:
Catalysis Science & Technology ,2018年8(24):6503-6510 ISSN:2044-4753
通讯作者:
Jia, Falong
作者机构:
[Quan, Fengjiao; Zhang, Lizhi; Mao, Chengliang; Zhan, Guangming; Ai, Zhihui; Jia, Falong] Cent China Normal Univ, Coll Chem, Inst Environm Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.;[Liu, Shiyuan; Gu, Honggang] Huazhong Univ Sci & Technol, State Key Lab Digital Mfg Equipment & Technol, Wuhan 430074, Hubei, Peoples R China.
通讯机构:
[Jia, Falong] C;Cent China Normal Univ, Coll Chem, Inst Environm Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
摘要:
Light-driven heterogeneous catalysis provides a promising way to accomplish chemical reactions by the use of light energy, which reduces the consumption of chemical energy sources. Here, we show that Ru/CeO2 catalysts exhibit high activity for the hydrogenation of CO2 to methane under illumination only, reaching high CO2 conversion (over 99.9%) and selectivity of methane (∼100%) at low temperature. In sharp contrast, less CO2 is converted at the same temperature when a traditional heating model is used. As revealed by the results, the enhanced conversion rate under illumination should not only be attributed to the light-induced thermo-heating. Further investigations by in situ IR analysis and theoretical calculation provide comprehensive understanding of the reaction mechanism, and the important role of light is revealed. It is expected that the combination of catalysts and light may afford new perspectives for CO2 hydrogenation. © 2018 The Royal Society of Chemistry.
语种:
英文
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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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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.
语种:
英文
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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.
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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Ascorbate-Promoted Surface Iron Cycle for Efficient Heterogeneous Fenton Alachlor Degradation with Hematite Nanocrystals
作者:
Huang, Xiaopeng;Hou, Xiaojing;Jia, Falong;Song, Fahui;Zhao, Jincai;...
期刊:
ACS Applied Materials & Interfaces ,2017年9(10):8751-8758 ISSN:1944-8244
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Hou, Xiaojing; Huang, Xiaopeng; Zhao, Jincai; Jia, Falong; Song, Fahui] Cent China Normal Univ, Minist Educ, Coll Chem, Inst Environm Chem,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Minist Educ, Coll Chem, Inst Environm Chem,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
关键词:
surface iron cycle;heterogeneous Fenton oxidation;alachlor degradation;ascorbate ions;hematite nanocrystals
摘要:
This study reports the H2O2 activation with different hematite nanocrystals and ascorbate ions for the herbicide alachlor degradation at pH 5. We found that hematite nanoplates (HNPs) exposed with {001} facets exhibited better catalytic performance than hematite nanocubes (HNCs) exposed with {012} facets, which was attributed to the formation of inner-sphere iron-ascorbate complexes on the hematite facets. The 3-fold undercoordination Fe cations of {001} facet favors the formation of inner-sphere iron-ascorbate complexes, while the 5-fold undercoordination Fe cations of {012} facet has stereo-hindrance effect, disfavoring the complex formation. The surface area normalized alachlor degradation rate constant (23.3 × 10-4 min-1 L m-2) of HNPs-ascorbate Fenton system was about 2.6 times that (9.1 × 10-4 min-1 L m-2) of HNCs-ascorbate counterpart. Meanwhile, the 89.0% of dechlorination and 30.0% of denitrification in the HNPs-ascorbate Fenton system were also significantly higher than those (60.9% and 13.1%) of the HNCs-ascorbate one. More importantly, the reductive dissolution of hematite by ascorbate was strongly coupled with the subsequent H2O2 decomposition by surface bound ferrous ions through surface iron cycle on the hematite facets in the hematite-ascorbate Fenton systems. This coupling could significantly inhibit the conversion of surface bound ferrous ions to dissolved ones, and thus account for the stability of hematite nanocrystals. This work sheds light on the internal relationship between iron geochemical cycling and contaminants degradation, and also inspires us to utilize surface iron cycle of widely existent hematite for environmental remediation. © 2017 American Chemical Society.
语种:
英文
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铜离子促进Fe@Fe_2O_3纳米线活化分子氧降解阿特拉津的研究
作者:
Jia Falong;Liu Juan;Zhang Lizhi*
期刊:
化学学报 ,2017年75(6):602-607 ISSN:0567-7351
通讯作者:
Zhang Lizhi
作者机构:
[Zhang Lizhi; Liu Juan; Jia Falong] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, 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, Hubei, Peoples R China.
关键词:
阿特拉津;降解;Fe@Fe_2O_3纳米线;分子氧活化;铜离子
摘要:
阿特拉津是一种持久性含氯有机污染物,难以生物降解,因此有必要开发高效技术清除环境中残留的阿特拉津.近来纳米铁材料的发展为降解阿特拉津提供了一种可供选择的新方法,但降解过程中纳米铁活性逐渐减弱的问题仍需改进.本论文研究了铜离子(Cu~(2+))存在条件下Fe@Fe_2O_3纳米线活化分子氧降解阿特拉津的过程,并探讨了Cu~(2+)的作用机理.研究结果表明,少量Cu~(2+)的存在就可以显著促使Fe@Fe_2O_3生成溶解态Fe(II),从而有助于分子氧活化并产生更多·OH等活性氧物种.在降解过程中,阿特拉津首先被氧化,进而发生脱氯上羟基反应、侧链氧化以及脱侧链反应.
语种:
中文
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纳米零价铁活化分子氧原理及降解有机污染物性能增强策略
作者:
Mu Yi;Jia Falong;Ai Zhihui* ;Zhang Lizhi*
期刊:
化学学报 ,2017年75(6):538-543 ISSN:0567-7351
通讯作者:
Ai Zhihui;Zhang Lizhi
作者机构:
[Zhang Lizhi; Jia Falong; Ai, ZH; Zhang, LZ; Mu Yi; Ai Zhihui] Cent China Normal Univ, Inst Appl & Environm 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 Appl & Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
关键词:
纳米零价铁;分子氧活化;活性氧物种;高级氧化技术
摘要:
纳米零价铁直接还原降解有机污染物运行长效性差,且不能矿化有机污染物.利用纳米零价铁还原活化分子氧生成活性氧物种可以氧化甚至矿化有机污染物.在最近的研究中,作者提出了纳米零价铁活化分子氧的双途径机理,即铁核电子转移到氧化铁壳表面的双电子还原活化分子氧途径和氧化铁表面结合态亚铁离子的单电子还原活化分子氧途径,阐释了纳米零价铁核壳结构依赖的分子氧活化降解有机污染物性能机制及性能增强策略.证实在纳米零价铁活化分子氧体系添加少量亚铁离子能在零价铁表面形成更多的结合态亚铁,显著增强纳米铁表界面活性氧物种生成量;同时,在纳米零价铁活化分子氧体系中引入少量有机或无机配体亦可提高活性氧物种产生效率,从而增强有机污染物降解性能.最后讨论了典型环境因素如pH值、共存离子、天然有机物等影响纳米零价铁活化分子氧降解有机污染物性能的规律.
语种:
中文
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Efficient electroreduction of CO2 on bulk silver electrode in aqueous solution via the inhibition of hydrogen evolution
作者:
Quan, Fengjiao;Xiong, Mubing;Jia, Falong* ;Zhang, Lizhi
期刊:
Applied Surface Science ,2017年399:48-54 ISSN:0169-4332
通讯作者:
Jia, Falong
作者机构:
[Quan, Fengjiao; Zhang, Lizhi; Xiong, Mubing; Jia, Falong] Cent China Normal Univ, Inst Environm Chem, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构:
[Jia, Falong] C;Cent China Normal Univ, Inst Environm Chem, Coll Chem, Wuhan 430079, Peoples R China.
关键词:
Carbon dioxide;Electrocatalytic reduction;Hydrogen evolution;Silver electrode
摘要:
Electrochemical CO 2 reduction provides a desirable pathway to convert greenhouse gas into useful chemicals. It is a great challenge to reduce CO 2 efficiently in aqueous solution, especially on commercial bulk metal electrodes. Here, we report substantial improvement in CO 2 reduction on bulk silver electrode through the introduction of ionic surfactant in aqueous electrolyte. The hydrogen evolution on the electrode surface is greatly suppressed by the surfactant, while the catalytic ability of silver towards CO 2 reduction is maintained. The Faradaic efficiency for CO is greatly enhanced from 50% to 95% after the addition of this low-cost surfactant. This study may provide new pathways towards efficient CO 2 reduction through the inhibition of proton reduction. © 2016
语种:
英文
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Hydroxylamine Promoted Goethite Surface Fenton Degradation of Organic Pollutants
作者:
Hou, Xiaojing;Huang, Xiaopeng;Jia, Falong;Ai, Zhihui;Zhao, Jincai;...
期刊:
Environmental Science & Technology ,2017年51(9):5118-5126 ISSN:0013-936X
通讯作者:
Zhang, Lizhi
作者机构:
[Zhang, Lizhi; Hou, Xiaojing; Huang, Xiaopeng; Zhao, Jincai; Jia, Falong; Ai, Zhihui] Cent China Normal Univ, Inst Environm & Appl Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C;Cent China Normal Univ, Inst Environm & Appl Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要:
In this study, we construct a surface Fenton system with hydroxylamine (NH2OH), goethite (α-FeOOH), and H2O2 (α-FeOOH-HA/H2O2) to degrade various organic pollutants including dyes (methyl orange, methylene blue, and rhodamine B), pesticides (pentachlorophenol, alachlor, and atrazine), and antibiotics (tetracycline, chloramphenicol, and lincomycin) at pH 5.0. In this surface Fenton system, the presence of NH2OH could greatly promote the H2O2 decomposition on the α-FeOOH surface to produce ·OH without releasing any detectable iron ions during the alachlor degradation, which was different from some previously reported heterogeneous Fenton counterparts. Moreover, the ·OH generation rate constant of this surface Fenton system was 102-104 times those of previous heterogeneous Fenton processes. The interaction between α-FeOOH and NH2OH was investigated with using attenuated total reflectance Fourier transform infrared spectroscopy and density functional theory calculations. The effective degradation of organic pollutants in this surface Fenton system was ascribed to the efficient Fe(III)/Fe(II) cycle on the α-FeOOH surface promoted by NH2OH, which was confirmed by X-ray photoelectron spectroscopy analysis. The degradation intermediates and mineralization of alachlor in this surface Fenton system were then systematically investigated using total organic carbon and ion chromatography, liquid chromatography-mass spectrometry, and gas chromatography-mass spectrometry. This study offers a new strategy to degrade organic pollutants and also sheds light on the environmental effects of goethite. © 2017 American Chemical Society.
语种:
英文
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常温常压纳米零价铁活化分子氧矿化三嗪类除草剂新策略
作者:
艾智慧;贾法龙;张礼知
期刊:
环境化学 ,2016年35(10):1977-1984 ISSN:0254-6108
作者机构:
[艾智慧; 贾法龙; 张礼知] 华中师范大学化学学院, 农药与化学生物学教育部重点实验室, 武汉, 430079
关键词:
农药;三嗪环;纳米零价铁;分子氧活化;氢自由基
摘要:
三嗪环的开环及矿化是三嗪类除草剂农药在环境中彻底消除的必要步骤.温和条件下高级氧化技术氧化三嗪类除草剂的最终产物是三聚氰酸,无法实现其开环矿化.本课题组拟通过在纳米零价铁活化分子氧氧化体系引入镍离子,促进氢自由基产生,调控体系中活性物种种类,诱导三嗪类除草剂加氢脱氯,避免羟基自由基加羟基脱氯生成极其稳定的三聚氰酸中间产物,优化三嗪类除草剂的降解途径,实现常温常压下纳米零价铁活化分子氧矿化三嗪类除草剂.本文计划系统考察体系中界面电子转移途径、分子氧活化机理、溶剂水的作用、活性物种的种类,深入分析活性物种生成和消亡途径;研究除草剂污染物的降解特性以及各种活性物种在三嗪类除草剂C—Cl和C—N键断裂过程中的作用,揭示不同活性物种与典型三嗪类除草剂的相互作用规律,阐明三嗪类除草剂降解和三嗪环开环等机理,为发展绿色高效农药污染控制技术提供理论支持.
语种:
中文
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Conversion of commercial Pt/C to "clean" Pt-Cu/C catalyst with high activity toward methanol oxidation
作者:
Liu, Hongmei* ;Wang, Shengqing;Jia, Falong
期刊:
Electrochimica Acta ,2015年184:331-337 ISSN:0013-4686
通讯作者:
Liu, Hongmei
作者机构:
[Wang, Shengqing; Liu, Hongmei] Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Wuhan 430074, Peoples R China.;[Jia, Falong] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
通讯机构:
[Liu, Hongmei] H;Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Wuhan 430074, Peoples R China.
关键词:
Platinum alloy;Surfactant-free synthesis;Electrocatalyst;Methanol oxidation
摘要:
A green synthetic strategy is developed to prepare PtxCuy/C catalyst in the absence of any capping ligands. Commercial Pt/C catalyst is used as the platinum precursor, and the Pt nanoparticles on the carbon act as a catalyst for the reduction of copper (II) precursors by hydrazine, which leads to the confined deposition of Cu on the Pt nanoparticles. The newly deposited Cu diffuses into the Pt nanoparticles to form PtxCuy alloy nanoparticles under hydrothermal conditions. The as-synthesized PtxCuy/C exhibits superior activity compared with commercial Pt/C towards the electro-oxidation of methanol. The results highlight the significance of alloy formation as an approach to improve the activity of commercial Pt/C catalyst. (C) 2015 Elsevier Ltd. All rights reserved.
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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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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