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.
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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.
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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.
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英文
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The surface hydroxyl and oxygen vacancy dependent Cr(vi) adsorption performance of BiOCl
作者：
Zhan, Guangming;Li, Jie;Hu, Yue;Zhao, Shengxi;Cao, Shiyu;...
期刊：
Environmental Science: Nano ,2020年7(5):1454-1463 ISSN：2051-8153
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Cao, Shiyu; Li, Jie; Zhao, Shengxi; Zhan, Guangming; Hu, Yue; Jia, Falong] 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：
The migration and bioavailability of Cr(vi) are determined by its adsorption behavior, which is sensitive to the coordination environment and to the physicochemical properties of mineral surfaces, especially natural surface defects, such as surface hydroxyls (OHs) and oxygen vacancies (OVs). However, natural minerals with high percentages of surface OHs and OVs are not available, concealing the quantitative relationship between surface OHs and OVs and Cr(vi) adsorption on minerals. With regard to the easy tuning of OHs and OVs on the 001 surface of BiOCl (BiOCl-001), herein we systematically check how surface OHs and OVs influence Cr(vi) adsorption on BiOCl-001, using density functional theory calculations,in situattenuated total reflectance Fourier transform infrared spectroscopy, and synchrotron-based Cr K-edge extended X-ray absorption fine structure spectroscopy, aiming to elucidate the contribution of surface OHs and OVs to Cr(vi) adsorption on minerals at a molecular level. The results revealed that 3.90 OHs captured one Cr(vi) in a hydrogen bonded adsorption and outer-sphere model with subtly distortedTdsymmetry, and 1.33 OVs anchored one Cr(vi) by forming a Cr-O-Bi bond to produce a monodentate mononuclear inner-sphere surface complex withC3vsymmetry, along with the partial reduction of Cr(vi) by unpaired electrons located in the OVs on BiOCl-001. This difference would intensely affect the mobility and long-term fate of Cr(vi) species. This study clarifies the surface defect dependent adsorption behavior of Cr(vi), and sheds light on the environmental effects of surface OHs and OVs of minerals. © The Royal Society of Chemistry 2020.
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英文
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Photothermal reverse-water-gas-shift over Au/CeO2 with high yield and selectivity in CO2 conversion
作者：
Lu, Bowen;Quan, Fengjiao;Sun, Zheng;Jia, Falong* ;Zhang, Lizhi
期刊：
Catalysis Communications ,2019年129:105724 ISSN：1566-7367
通讯作者：
Jia, Falong
作者机构：
[Quan, Fengjiao; Zhang, Lizhi; Lu, Bowen; Sun, Zheng; Jia, Falong] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm Chem,Coll Chem, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Jia, Falong] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Inst Environm Chem,Coll Chem, Wuhan 430079, Hubei, Peoples R China.
关键词：
Carbon dioxide;Carbon monoxide;Hydrogenation;Photothermal process
摘要：
Photothermal reverse-water-gas-shift is realized with high conversion rate and selectivity of CO in the case of Au/CeO2 catalyst. Moreover, photothermal reaction rate is much higher (>10 times) than that performed under thermal condition. As indicated by the results of in-situ infrared spectroscopy and kinetic experiments, the special role of light is found to be related with the promotion of hydrogen-splitting step. The robust Au/CeO2 catalyst exhibits stable activity and CO selectivity under long-term light irradiation. It is expected that the combination of catalysts and light may afford new perspectives for the CO2 hydrogenation. © 2019 Elsevier B.V.
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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.
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英文
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Insights into the facet-dependent adsorption of phenylarsonic acid on hematite nanocrystals
作者：
Cao, Shiyu;Zhang, Xin;Huang, Xiaopeng;Wan, Shuhao;An, Xuezheng;...
期刊：
Environmental Science: Nano ,2019年6(11):3280-3291 ISSN：2051-8153
通讯作者：
Jia, Falong;Zhang, Lizhi
作者机构：
[Zhang, Xin; Zhang, Lizhi; Cao, Shiyu; Huang, Xiaopeng; An, Xuezheng; Jia, Falong; Zhang, LZ; Wan, Shuhao] 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：
[Jia, FL; Zhang, LZ] C;Cent China Normal Univ, Coll Chem, Inst Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
摘要：
Organic arsenics have been frequently detected in natural environments and regarded as a group of emerging contaminants. Elucidating the migration of organic arsenics requires a deep understanding of intrinsic adsorption mechanisms of organic arsenics on iron-bearing minerals, which are seldom investigated. In this study, we investigated the facet-dependent adsorption behavior of phenylarsonic acid (PhAs) on hematite nanocrystals with open circuit potential (OCP) analysis, batch adsorption experiments, adsorption isotherm curves, synchrotron-based As K-edge extended X-ray absorption fine structure (EXAFS) spectroscopy, attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy, and density functional theory (DFT) calculations. We found that organic arsenics adsorbed on two facets (e.g. {001} and {012}) of hematite through the same non-protonated inner-sphere coordination but in different molecular configurations. Surface complexation models were set up to analyze the preferred coordination geometries dependent on the facets, and the {012} facet was found to favor the PhAs adsorption more than the {001} facet. These findings clarified the dependence of organic arsenic adsorption on the hematite facets, and shed light on the environmental effects of hematite on the migration of PhAs. This journal is © 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.
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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.
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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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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.
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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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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：
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.
语种：
英文
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Durch Sauerstoff‐Leerstellen vermittelte Photokatalyse mit BiOCl: Reaktivität, Selektivität und Ausblick
作者：
Dr. Hao Li;Dr. Jie Li;Prof. Zhihui Ai;Prof. Falong Jia;Prof. Lizhi Zhang;...
期刊：
Angewandte Chemie ,2018年130(1):128-145 ISSN：0044-8249
通讯作者：
Prof. Lizhi Zhang<&wdkj&>Prof. Lizhi Zhang Prof. Lizhi Zhang Prof. Lizhi Zhang
作者机构：
[Dr. Hao Li; Dr. Jie Li; Prof. Zhihui Ai; Prof. Falong Jia; Prof. Lizhi Zhang; Dr. Hao Li Dr. Hao Li Dr. Hao Li; Dr. Jie Li Dr. Jie Li Dr. Jie Li; Prof. Zhihui Ai Prof. Zhihui Ai Prof. Zhihui Ai; Prof. Falong Jia Prof. Falong Jia Prof. Falong Jia; Prof. Lizhi Zhang Prof. Lizhi Zhang Prof. Lizhi Zhang] Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental Chemistry, College of Chemistry, Central China Normal University, Wuhan, 430079 Volksrepublik China
通讯机构：
[Prof. Lizhi Zhang; Prof. Lizhi Zhang Prof. Lizhi Zhang Prof. Lizhi Zhang] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental Chemistry, College of Chemistry, Central China Normal University, Wuhan, 430079 Volksrepublik China
关键词：
BiOCl;Photokatalyse;Sauerstoffaktivierung;Stickstoff-Fixierung;Wasserspaltung
摘要：
<jats:title>Abstract</jats:title><jats:p>Die Halbleiter‐Photokatalyse ist eine vielversprechende Methode für die Nutzung von Sonnenlicht für Energieumwandlungen. Ihre Effizienz ist derzeit jedoch aufgrund einer begrenzten Lichtreaktion und/oder der ausgeprägten Rekombination der Ladungsträger noch unbefriedigend. Moderne Charakterisierungstechniken sowie Berechnungen der elektronischen Struktur zeigen, dass selbst winzige Konzentrationen von Sauerstoff‐Leerstellen (“oxygen vacancies”, OVs) auf der Oberfläche realer Photokatalysatoren deren Kinetik und Energetik sowie die Mechanismen photokatalytischer Reaktionen entscheidend beeinflussen können. Dieser Aufsatz stellt die inhärente photokatalytische Funktionalität von OVs auf BiOCl‐Oberflächen auf molekularer Ebene dar. Die Korrelation zwischen der Struktur der OVs und Reaktivität sowie Selektivität photokatalytischer Reaktionen wird am Beispiel von OVs auf prototypischen BiOCl‐Flächen eingehend diskutiert.</jats:p>
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 Fe@Fe2O3 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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