Surface structure-dependent photocatalytic O-2 activation for pollutant removal with bismuth oxyhalides
作者：
Li, Hao;Ai, Zhihui* ;Zhang, Lizhi*
期刊：
Chemical Communications ,2020年56(97):15282-15296 ISSN：1359-7345
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Li, Hao; Ai, ZH; Zhang, LZ; Ai, Zhihui] Cent China Normal Univ, Coll Chem, Inst Environm & Appl 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, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
摘要：
The purification of water and air by semiconductor photocatalysis is a rapidly growing area for academic research and industrial innovation, featured with ambient removal of organic or inorganic pollutants by using solar light as the energy source and atmospheric O2 as the green oxidant. Both charge transfer and energy transfer from excited photocatalysts can overcome the spin-forbidden nature of O2. Layered bismuth oxyhalides are a new group of two-dimensional photocatalysts with an appealing geometric and surface structure that allows the dynamic and selective tuning of O2 activation at the surface molecular level. In this Feature Article, we specifically summarize our recent progress in selective O2 activation by engineering surface structures of bismuth oxyhalides. Then, we demonstrate selective photocatalytic O2 activation of bismuth oxyhalides for environmental control, including water decontamination, volatile organic compound oxidation and nitrogen oxide removal, as well as selective catalytic oxidations. Challenges and opportunities regarding the design of photocatalysts with satisfactory performance for potential environmental control applications are also presented. This journal is © The Royal Society of Chemistry.
语种：
英文
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Enhanced Cr(VI) removal of zero-valent iron with high proton conductive FeC2O4·2H2O shell
作者：
Hu, Yue;Zhan, Guangming;Peng, Xing* ;Liu, Xiufan;Ai, Zhihui;...
期刊：
Chemical Engineering Journal ,2020年389:124414 ISSN：1385-8947
通讯作者：
Peng, Xing;Zhang, Lizhi
作者机构：
[Quan, Fengjiao; Zhang, Lizhi; Cao, Shiyu; Peng, Xing; Liu, Xiufan; Shen, Wenjuan; Hu, Yue; Zhan, Guangming; Ai, Zhihui; Jia, Falong; Peng, X; Zhang, LZ] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Peng, X; Zhang, LZ] C;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词：
Zero-valent iron;FeC2O4 center dot 2H(2)O shell;Cr(VI) removal;Proton transfer;Surface-bound Fe2+
摘要：
In this study, we coated a high proton conducive shell on the zero-valent iron (ZVI) surface by mechanically ball-milling ZVI with oxalic acid dihydrate (OX-ZVI), and demonstrated that the generated FeC2O4 center dot 2H(2)O shell dramatically improved the Cr(VI) removal rate of ZVI by about 15-80 times. Owing to a higher proton conductivity of FeC2O4 center dot 2H(2)O shell than that of Fe2O3 shell, proton could easily transfer through FeC2O4 center dot 2H(2)O shell into iron core and be reduced to center dot H, accompanying with fast surface-bound Fe2+ generation, resulting in high efficiency of Cr(VI) removal in a wide pH range. Meanwhile, the removed Cr(VI) was deposited on OX-ZVI surface in the formation of FexCr1-x(OH)(3) composites, accompanied by the appearance of typical hollow structure derived from iron core dissolution. This study clarifies the significance of proton transfer on the reactivity of zero-valent iron, and also provides a new strategy to prepare highly active zero-valent iron for Cr(VI) removal.
语种：
英文
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Surface hydrogen bond network spatially confined BiOCl oxygen vacancy for photocatalysis
作者：
Li, Hao;Chen, Shang;Shang, Huan;Wang, Xiaobing;Yang, Zhiping;...
期刊：
科学通报(英文版) ,2020年65(22):1916-1923 ISSN：2095-9273
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Chen, Shang; Yang, Zhiping; Shang, Huan; Li, Hao; Wang, Xiaobing; Ai, ZH; Zhang, LZ; Ai, Zhihui] Cent China Normal Univ, Coll Chem, Inst Environm & Appl 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, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词：
Oxygen vacancy;Hydrogen bond;Photocatalysis;NO oxidation;Selectivity
摘要：
Rational engineering of oxygen vacancy (V-O) at atomic precision is the key to comprehensively understanding the oxygen chemistry of oxide materials for catalytic oxidations. Here, we demonstrate that V-O can be spatially confined on the surface through a sophisticated surface hydrogen bond (HB) network. The HB network is constructed between a hydroxyl-rich BiOCl surface and polyprotic phosphoric acid, which remarkably decreases the formation energy of surface V-O by selectively weakening the metal-oxygen bonds in a short range. Thus, surface-confined V-O enables us to unambiguously distinguish the intrafacial and suprafacial oxygen species associated with NO oxidation in two classical catalytic systems. Unlike randomly distributed bulk V-O that benefits the thermocatalytic NO oxidation and lattice O diffusion by the dominant intrafacial mechanism, surface V-O is demonstrated to favor the photocatalytic NO oxidation through a suprafacial scheme by energetically activating surface O-2, which should be attributed to the spatial confinement nature of surface V-O. (C) 2020 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.
语种：
英文
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Amorphization enables highly efficient anaerobic thiamphenicol reduction by zero-valent iron
作者：
Shen, Wenjuan;Wang, Xiaoming;Jia, Falong* ;Tong, Zhe;Sun, Hongwei;...
期刊：
Applied Catalysis B: Environmental ,2020年264:118550 ISSN：0926-3373
通讯作者：
Jia, Falong;Ai, Zhihui;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Jia, FL; Ai, ZH; Zhang, LZ; Sun, Hongwei; Wang, Xiaobing; Shen, Wenjuan; Jia, Falong; Tong, Zhe; Song, Fahui; Ai, Zhihui] Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Wang, Xiaoming] Huazhong Agr Univ, Minist Agr, Coll Resources & Environm, Key Lab Arable Land Conservat Middle & Lower Reac, Wuhan 430070, Peoples R China.;[Chai, Bo; Shen, Wenjuan] Wuhan Polytech Univ, Sch Chem & Environm Engn, Wuhan 430023, Peoples R China.
通讯机构：
[Jia, FL; Ai, ZH; Zhang, LZ] C;Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
关键词：
Amorphous zero-valent iron;Anaerobic reduction;Ethylenediamine;Formation mechanism;Thiamphenicol
摘要：
As a new member of zero-valent iron (ZVI) family, amorphous zero-valent iron microspheres (A-mZVI) were very promising for the aerobic disinfection of Escherichia coli. However, their formation and anaerobic reduction performance are still unknown. In this study, we investigated A-mZVI's formation mechanism and checked its anaerobic reduction ability with using thiamphenicol as a model contaminant, and found that the presence of ethylenediamine decreased the reducing capacity of NaBH4, the Fe(II) reduction rate, and the energy for crystal growth, and thus favored the formation of metastable amorphous structure. Moreover, this amorphous structural nature of A-mZVI endowed it with an apparent thiamphenicol reduction rate constant as high as 4.8 × 10−2 min−1, 7.9 times that (6.1 × 10−3 min−1) of crystalline zero-valent iron microspheres (C-mZVI). Further investigation revealed that the enhanced anaerobic thiamphenicol reduction of A-mZVI was strongly ascribed to its promoted electron donating ability arisen from the amorphization process. © 2019 Elsevier B.V.
语种：
英文
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Hydrogen Spillover to Oxygen Vacancy of TiO2-xHy/Fe: Breaking the Scaling Relationship of Ammonia Synthesis
作者：
Mao, Chengliang;Wang, Jiaxian;Zou, Yunjie;Qi, Guodong;Loh, Joel Yi Yang;...
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY ,2020年142(41):17403-17412 ISSN：0002-7863
通讯作者：
Zhang, Lizhi;Ozin, Geoffrey A.
作者机构：
[Zhang, Lizhi; Zou, Yunjie; Liu, Xiao; Ai, Zhihui; Wang, Jiaxian; Mao, Chengliang; Shang, Huan; Zhao, Jincai; Li, Jie; Li, Meiqi] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Ghoussoub, Mireille; Mao, Chengliang; Wang, Lu; Xia, Meikun; Ozin, Geoffrey A.] Univ Toronto, Dept Chem, Solar Fuels Cluster, Mat Chem & Nanochem Res Grp, Toronto, ON M5S 3H6, Canada.;[Qi, Guodong; Xu, Jun; Deng, Feng] Chinese Acad Sci, State Key Lab Magnet Resonance & Atom & Mol Phys, Natl Ctr Magnet Resonance Wuhan, Wuhan Inst Phys & Math,Innovat Acad Precis Measur, Wuhan 430071, Peoples R China.;[Loh, Joel Yi Yang; Kherani, Nazir P.] Univ Toronto, Dept Mat Sci & Engn, Toronto, ON M5S 3E4, Canada.;[Zhang, Tianhua] Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst NERC C, Sch Chem Engn, Fuzhou 350002, Fujian, Peoples R China.
通讯机构：
[Zhang, Lizhi] C;[Ozin, Geoffrey A.] U;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;Univ Toronto, Dept Chem, Solar Fuels Cluster, Mat Chem & Nanochem Res Grp, Toronto, ON M5S 3H6, Canada.
摘要：
Optimizing kinetic barriers of ammonia synthesis to reduce the energy intensity has recently attracted significant research interest. The motivation for the research is to discover means by which activation barriers of N-2 dissociation and NHz (z = 1-2, surface intermediates) destabilization can be reduced simultaneously, that is, breaking the "scaling relationship". However, by far only a single success has been reported in 2016 based on the discovery of a strong-weak N-bonding pair: transition metals (nitrides)-LiH. Described herein is a second example that is counterintuitively founded upon a strong-strong N-bonding pair unveiled in a bifunctional nanoscale catalyst TiO2-xHy/Fe (where 0.02 <= x <= 0.03 and 0 < y < 0.03), in which hydrogen spillover (H) from Fe to cascade oxygen vacancies (O-V-O-V) results in the trapped form of O-V-H on the TiO2-xHy component. The Fe component thus enables facile activation of N-2, while the O-V-H in TiO2-xHy hydrogenates the N or NHz to NH3 easily.
语种：
英文
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Dual-site activation enhanced photocatalytic removal of no with Au/CeO2
作者：
Shang, Huan;Huang, Shun;Li, Hao;Li, Meiqi;Zhao, Shengxi;...
期刊：
Chemical Engineering Journal ,2020年386:124047 ISSN：1385-8947
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Wang, Jiaxian; Zhang, Lizhi; Shang, Huan; Li, Hao; Ai, ZH; Zhang, LZ; Zhao, Shengxi; Huang, Shun; Ai, Zhihui; Li, Meiqi] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm & Appl Chem, Wuhan 430079, 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, Wuhan 430079, Peoples R China.
关键词：
Air purification;Dual-site activation;Oxygen vacancy;Photocatalytic NO removal
摘要：
Photocatalytic technology provides an effective strategy for aerobic purification of dilute gaseous NO pollutant, but suffers from its low efficiency. In this study, we demonstrate that the bicomponent Au/CeO2 photocatalyst possesses an enhanced photocatalytic NO removal performance under visible light irradiation, with a higher NO conversion efficiency (65%) and triple rate constant (0.1451 min−1) versus CeO2 (50%, 0.0448 min−1). Density function theory calculations and experimental results revealed that oxygen vacancies on the CeO2 component could favorably initiate the adsorption and activation of O2 to generate [rad]O2−, simultaneously, Au nanoparticles loaded on the CeO2 surface were active centers for adsorption and activation of NO to produce NO+ by plasmonic holes of the Au under visible light irradiation. Subsequently, these [rad]O2− and NO+ species generated via dual-site activation pathway on Au/CeO2 photocatalyst reacted spontaneously to generate the final NO3−, leading to enhanced photocatalytic removal of NO. This study sheds light on a dual-site induced photocatalytic NO oxidation and advances the design of effective air purification photocatalyst. © 2020 Elsevier B.V.
语种：
英文
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Persulfate activation induced by ascorbic acid for efficient organic pollutants oxidation
作者：
Hou, Xiaojing;Zhan, Guangming;Huang, Xiaopeng;Wang, Nan;Ai, Zhihui* ;...
期刊：
Chemical Engineering Journal ,2020年382:122355 ISSN：1385-8947
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Hou, Xiaojing; Wang, Nan; Huang, Xiaopeng; Ai, ZH; Zhang, LZ; Zhan, Guangming; Ai, Zhihui] Cent China Normal Univ, Inst Environm & Appl Chem, Coll 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, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词：
Ascorbic acid;In situ chemical oxidation;Organic pollutants;Persulfate activation
摘要：
In this study, we demonstrate that ascorbic acid (AA) exhibited extremely high activity on persulfate (PS) activation (AA/PS) to produce SO4[rad]− and [rad]OH for the degradation of various organic pollutants, including atrazine, pentachlorophenol, alachlor, tetracycline, and chloramphenicol. Taken atrazine as a model natural organic micropollutants, we surprisingly found that the degradation rate constant of atrazine during PS activation in presence of AA was about 29 times larger than that in the absence of AA. The underlying mechanism of persulfate activation induced by AA was then systematically investigated by electron spin resonance (ESR) analysis, theoretical density functional theory (DFT) calculations, and kinetic experiments. The combination of ESR and DFT results confirmed that the persulfate activation induced by ascorbic acid was attributed to the electron transfer from AA to PS. In this process, AA undergoes a two-step oxidation by PS to generate SO4[rad]− and dehydroascorbic acid with the formation of an intermediate ascorbate free radical. More interestingly, atrazine in the real aquifer sediment system could be totally oxidized in the presence of PS and AA. These findings offer a new economically feasible persulfate activation strategy for the in situ chemical oxidation of organic compounds in contaminated water and sediment systems. © 2019
语种：
英文
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SO_2在矿质颗粒物表面非均相反应研究进展
作者：
尚欢;刘修凡;陈娜;李美琪;陈子越;...
期刊：
华中农业大学学报 ,2020年39(5):9-16 ISSN：1000-2421
作者机构：
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;[刘修凡; 李美琪; 陈子越; 张礼知; 艾智慧; 陈娜; 尚欢] 华中师范大学
关键词：
矿质颗粒物;硫酸盐;非均相反应;光化学;雾霾
摘要：
我国秋冬季雾霾频发,对人类健康造成巨大威胁。大气中SO_2经系列物理化学反应产生的硫酸盐气溶胶是雾霾产生的元凶,其中矿质颗粒物参与的SO_2表面非均相反应尤为重要,因此,厘清矿质颗粒物表面硫酸盐的形成机制是解析大气雾霾形成的关键科学问题。本文综述了SO_2在不同类型氧化型矿质颗粒物表面非均相反应的研究进展,讨论了多污染物共存体系、湿度和光照对SO_2非均相反应的影响,并对目前矿质颗粒物表面非均相反应研究中存在的问题进行了评述,旨在加深对矿质颗粒物促进硫酸盐形成机制的认识,助力揭示我国雾霾的成因,进而为雾霾治理提供理论指导。
语种：
中文
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Phosphate modification enables high efficiency and electron selectivity of nZVI toward Cr(VI) removal
作者：
Li, Meiqi;Mu, Yi;Shang, Huan;Mao, Chengliang;Cao, Shiyu;...
期刊：
Applied Catalysis B: Environmental ,2020年263:118364 ISSN：0926-3373
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Cao, Shiyu; Shang, Huan; Mao, Chengliang; Mu, Yi; Ai, ZH; Zhang, LZ; Ai, Zhihui; Li, Meiqi] Cent China Normal Univ, Inst Environm & Appl 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 Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
关键词：
Cr(VI) removal;Efficiency;Electron selectivity;Nanoscale zerovalent iron;Phosphate modification
摘要：
In this study, we demonstrate that surface phosphate modification of nZVI (p-nZVI) could enhance the electron selectivity of Cr(VI) reduction from 6.1% to 31.3%, as estimated by XANES and XPS, and thus promote the Cr(VI) removal efficiency by 4 folds. DFT calculation and experimental results revealed that phosphate groups were adsorbed on the surface of p-nZVI via a monodentate mononuclear model to inhibit the reaction with oxygen and/or water via the pendant protons of phosphate, accounting for high electron selectivity of p-nZVI. More importantly, surface phosphate modification shifted the binding configuration of Cr(VI) from a monodentate mononuclear model on nZVI to bidentate binuclear one on the p-nZVI surface, thus strengthening the Cr(VI) adsorption ability and favoring the subsequent Cr(VI) reduction. This study provides a facile strategy to enhance the electron selectivity towards metal remediation, and highlights the vital influence of surface structure on nZVI reactivity at the molecular level. © 2019 Elsevier B.V.
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英文
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Accelerated Dinitrogen Electroreduction to Ammonia via Interfacial Polarization Triggered by Single-Atom Protrusions
作者：
Li, Jie;Chen, Shang;Quan, Fengjiao;Zhan, Guangming;Jia, Falong;...
期刊：
Chem ,2020年6(4):885-901 ISSN：2451-9294
通讯作者：
Zhang, Lizhi
作者机构：
[Quan, Fengjiao; Zhang, Lizhi; Chen, Shang; Li, Jie; Zhan, Guangming; Jia, Falong; Ai, Zhihui] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Inst Environm & Appl Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
通讯机构：
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Inst Environm & Appl Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
关键词：
electric field;electrocatalytic ammonia synthesis;interfacial polarization;SDG7: Affordable and clean energy;single atom catalysis
摘要：
Electrocatalytic N2 reduction reaction (NRR) offers a promising low-energy, sustainable ammonia-synthesizing alternative to Haber-Bosch reaction. One roadblock lying in access to high-performance ammonia electrosynthesis emanates from the unsatisfied ability of electrocatalysts to wreck N≡N bond. Here, we report that interfacial polarization is an efficient scenario to enhance N≡N fracture to boost electrocatalytic ammonia synthesis. As a proof-of-concept demonstration, protrusion-shaped Fe single-atom catalysts immobilized onto MoS2 nanosheets engender electric fields to polarize N2. The resultant interfacial polarization fields between Fe-MoS2 and N2 drive the injection of more electrons into N2 antibonding orbitals in a fast manner, leading to a superior ammonia-evolving rate (36.1 ± 3.6 mmol g−1 h−1 or 97.5 ± 6 μg h−1 cm−2) at low applied potential. Similar phenomena are applicable in Co-MoS2, Cu-MoS2, Rh-MoS2, or Ru-MoS2, suggesting the potential universality of our interfacial polarization concept in upgrading wide-scope catalysis. Seeking a green, low-cost, sustainable approach to synthesize ammonia is crucial to society development and human living. A promising candidate is electrocatalytic nitrogen reduction. The insufficient ability of electrocatalysts to split the N≡N bond, however, limits the activity and selectivity. Using interfacial polarization as a conceptually novel strategy to promote N≡N disintegration, high-rate ammonia electrosynthesis up to 36.1 ± 3.6 mmol g−1 h−1 (97.5 ± 6 μg h−1 cm−2) is realized at a low applied potential (−0.2 V versus RHE). This work paves a new way toward replacing Haber-Bosch reaction with ambient ammonia electrosynthesis. Interfacial polarization is reported as a brand new, efficient, and generalizable strategy to accelerate electrocatalytic reduction of N2 to ammonia. The polarization is established by using an electric field to polarize N2. The electric field is triggered by protrusion-like single atoms anchored on MoS2. The interfacial polarization accelerates electron transfer from single atoms to N2 and thus promotes N2 reduction. As a result, ammonia synthesis in an electrochemical flow cell proceeds at a high rate of 36.1 ± 3.6 mmol g−1 h−1. © 2020 Elsevier Inc.
语种：
英文
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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.
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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Dechlorination-Hydroxylation of Atrazine to Hydroxyatrazine with Thiosulfate: A Detoxification Strategy in Seconds
作者：
Mu, Yi;Zhan, Guangming;Huang, Cuimei;Wang, Xiaobing;Ai, Zhihui* ;...
期刊：
Environmental Science & Technology ,2019年53(6):3208-3216 ISSN：0013-936X
通讯作者：
Ai, Zhihui;Zhang, Lizhi;Zou, Jianping
作者机构：
[Huang, Cuimei; Zhang, Lizhi; Mu, Yi; Wang, Xiaobing; Ai, ZH; Zhang, LZ; Zhan, Guangming; Ai, Zhihui] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm Chem, Wuhan 430079, Hubei, Peoples R China.;[Zou, Jianping; Mu, Yi; Luo, Shenglian] Nanchang Hangkong Univ, Key Lab Jiangxi Prov Persistent Pollutants Contro, Nanchang 330063, Jiangxi, Peoples R China.
通讯机构：
[Ai, ZH; Zhang, LZ] C;[Zou, Jianping] N;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm Chem, Wuhan 430079, Hubei, Peoples R China.;Nanchang Hangkong Univ, Key Lab Jiangxi Prov Persistent Pollutants Contro, Nanchang 330063, Jiangxi, Peoples R China.
摘要：
Hydroxylation of atrazine to nontoxic hydroxyatrazine is generally considered an efficient detoxification method to remediate atrazine-contaminated soil and water. However, previous studies suggested that hydroxylation was not the dominant pathway for atrazine degradation in the hydroxyl radical-generating systems such as Fenton reaction, ozonation and UV/H2O2. Herein we report that the addition of sodium thiosulfate can realize rapid hydroxylation of atrazine to hydroxyatrazine at pH ≤ 4 under room temperature. High resolution mass spectra and isotope experiments results revealed that the hydroxylation of atrazine was involved with nucleophilic substitution and subsequent hydrolysis reaction as follows. HS2O3-, as a species of thiosulfate only at pH ≤ 4, first attacked C atom connecting to chlorine of atrazine to dechlorinate atrazine and produce C8H14N5S2O3-. Subsequently, the S-S bond of C8H14N5S2O3- was cleaved easily to form SO3 and C8H14N5S-. Next, C8H14N5S- was hydrolyzed to generate hydroxyatrazine and H2S. Finally, the comproportionation of SO3 and H2S in situ produced S0 during hydroxylation of atrazine with thiosulfate. This study clarifies the importance of degradation pathway on the removal of pollutants, and also provides a nonoxidative strategy for atrazine detoxification in seconds. Copyright © 2019 American Chemical Society.
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Hexavalent chromium removal by a new composite system of dissimilatory iron reduction bacteria Aeromonas hydrophila and nanoscale zero-valent iron
作者：
Shi, Zunji;Shen, Wenjuan;Yang, Kai;Zheng, Ningning;Jiang, Xiaofang;...
期刊：
Chemical Engineering Journal ,2019年362:63-70 ISSN：1385-8947
通讯作者：
Xie, Bo;Ai, Zhihui
作者机构：
[Xie, Bo; Yang, Dandan; Yang, Kai; Shi, Zunji; Jiang, Xiaofang; Zheng, Ningning; Liu, Limin] Cent China Normal Univ, Hubei Key Lab Genet Regulat & Integrat Biol, Sch Life Sci, Wuhan 430079, Hubei, Peoples R China.;[Zhang, Lizhi; Shen, Wenjuan; Ai, Zhihui] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.;[Shi, Zunji] Chinese Acad Sci, Key Lab Magnet Resonance Biol Syst, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan Ctr Magnet Resonance,Wuhan Inst Phys & Math, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Xie, Bo; Ai, Zhihui] C;Cent China Normal Univ, Hubei Key Lab Genet Regulat & Integrat Biol, Sch Life Sci, Wuhan 430079, Hubei, Peoples R China.;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Hubei, Peoples R China.
关键词：
Aeromonas hydrophila;Anoxic reduction;Hexavalent chromium;Nanoscale zero-valent iron
摘要：
Core-shell Fe@Fe2O3 nanowire is one special nanoscale zero-valent iron (NZVI) with an iron core and an outside shell of iron oxide containing the surface bound ferrous ions, which has been used to remove various pollutants including Cr(VI). However, it can be easily oxidized to accumulate iron oxides on the shell, resulting in the loss of reactive activity during its long-term application. Therefore, the dissolution of iron oxides by reduction is required to maintain NZVI reactivity. In this study, we combine NZVI and a dissimilatory iron reduction bacteria (DIRB), Aeromonas hydrophila HS01, to establish a composite system for a sustainable anoxic reduction of Cr(VI). HS01 can stably coexist with NZVI, reduce the oxidized Fe on NZVI and generate more dissolved Fe(II) under anoxic conditions. This presence of HS01 can maintain the core-shell structured morphology and relatively more Fe0 and Fe(II) on NZVI surface, and enhance the reactivity in Cr(VI) removal. Our results indicated that a suitable DIRB can be used to prolong the reactivity of NZVI, and their combination is an efficient method for anoxic Cr(VI) removal. © 2019 Elsevier B.V.
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Interfacial Charging-Decharging Strategy for Efficient and Selective Aerobic NO Oxidation on Oxygen Vacancy
作者：
Li, Hao;Shang, Huan;Li, Yuhan;Cao, Xuemei;Yang, Zhiping;...
期刊：
Environmental Science & Technology ,2019年53(12):6964-6971 ISSN：0013-936X
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Yang, Zhiping; Shang, Huan; Li, Hao; Ai, ZH; Zhang, LZ; Ai, Zhihui; Cao, Xuemei] Cent China Normal Univ, Inst Appl & Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol,Coll Chem, Wuhan 430079, Hubei, Peoples R China.;[Li, Yuhan] Chongqing Technol & Business Univ, Chongqing Key Lab Catalysis & New Environm Mat, Engn Res Ctr Waste Oil Recovery Technol & Equipme, Minist Educ,Coll Environm & Resources, Chongqing 400067, 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,Coll Chem, Wuhan 430079, Hubei, Peoples R China.
摘要：
Intelligent defect engineering to harness surface molecular processes is at the core of selective oxidation catalysis. Here, we demonstrate that the two-electron-trapped oxygen vacancy (V-O) of BiOCL, a prototypical F center (V-O('')) is a superb site to confine O-2 toward efficient and selective NO oxidation to nitrate. Stimulated by solar light, V-O('')" accomplishes NO oxidation through a two-electron charging (V-O('') + O-2 -> V-O('') -O-2(2-)) and subsequent one-electron decharging process (V-O('')-O-2(2)- + NO -> V-O-NO3- + e(-)). The back-donated electron is retrapped by V-O to produce a new single-electron-trapped V-O (V-O(')), simultaneously triggering a second round of NO oxidation (V-O' -O-2 + NO -> VO-NO3-). This unprecedented interfacial charging-decharging scheme alters the peroxide-associated NO oxidation selectivity from NO2 to NO3- with a high efficiency and thus hold great promise for the treatment of risky NOx species in indoor air.
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Oxygen Vacancies Promoted the Selective Photocatalytic Removal of NO with Blue TiO2 via Simultaneous Molecular Oxygen Activation and Photogenerated Hole Annihilation
作者：
Shang, Huan;Li, Meiqi;Li, Hao;Huang, Shun;Mao, Chengliang;...
期刊：
Environmental Science & Technology ,2019年53(11):6444-6453 ISSN：0013-936X
通讯作者：
Ai, Zhihui;Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Shang, Huan; Mao, Chengliang; Li, Hao; Ai, ZH; Zhang, LZ; Huang, Shun; Ai, Zhihui; Li, Meiqi] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Ai, ZH; Zhang, LZ] C;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
摘要：
Semiconductor photocatalytic technology has great potential for the removal of dilute gaseous NO in indoor and outdoor atmospheres but suffers from unsatisfactory NO-removal selectivity due to undesirable NO2 byproduct generation. In this study, we demonstrate that the 99% selectivity of photocatalytic NO oxidation toward nitrate can be achieved over blue TiO2 bearing oxygen vacancies (OVs) under visible-light irradiation. First-principles density functional theory calculation and experimental results suggested that the OVs of blue TiO2 with localized electrons could facilitate the molecular oxygen activation through single-electron pathways to generate ·O2- and simultaneously promote the photogenerated hole annihilation. The generated ·O2- directly converted NO to nitrate, while the hole annihilation inhibited the side-reaction between holes and NO to avoid toxic NO2 byproduct formation, resulting in the highly selective removal of NO. This study reveals the dual functions of OVs in defective photocatalysts and also provides fundamental guidance for the selective purification of NO with photocatalytic technology. © 2019 American Chemical Society.
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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.
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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.
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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
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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：
In situ processing;Manganese;Manganese removal (water treatment);Organic acids;Oxalic acid;Rate constants;Acceleration process;Acid wastewater;Cr reductions;Electron transfer;Induction periods;Initial induction;Natural aquatic environments;Ternary complex;Chromium compounds;chromium;manganese;oxalic acid;aquatic environment;cation;chromium;electron;in situ measurement;oxalic acid;oxidation;pH;reduction;transformation;wastewater;wastewater treatment;acceleration;aquatic environment;Article;automation;bioremediation;biotransformation;chemical analysis;comparative study;concentration (parameters);controlled study;electron transport;metal recovery;oxidation;oxidation reduction reaction;proton transport;rate constant;reaction time;waste water management
摘要：
In this study, we demonstrate that Mn(2+) can greatly promote the Cr(VI) reduction by oxalic acid at pH<5 via an induction period and a subsequent auto-acceleration process. The Cr(VI) reduction rate constant during the late auto-acceleration process was about 10 times that of the initial induction period. Characterization results revealed that this interesting two-step Cr(VI) reduction phenomenon was attributed to the in-situ generated Mn(3+) by the oxidation of Mn(2+) with Cr(VI) in the presence of oxalic acid during the induction period. The in-situ generated Mn(3+) might complex with oxalate and Cr(VI) to produce a ternary complex, thus facilitating the electron transfer from oxalate to Cr(VI) to automatically accelerate the Cr(VI) reduction process. These findings shed insight into the possible roles of widely existed Mn ions (Mn(2+) and Mn(3+)) and oxalic acid in the transformation of Cr(VI) in natural aquatic environment, and also provided an efficient way to remediate Cr(VI)-containing acid wastewater.
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