Electrochemically self-doped WO3/TiO2 nanotubes for photocatalytic degradation of volatile organic compounds
作者：
Wang, Xiaoguang;Sun, Minghui;Murugananthan, Muthu;Zhang, Yanrong* ;Zhang, Lizhi*
期刊：
Applied Catalysis B: Environmental ,2020年260:118205 ISSN：0926-3373
通讯作者：
Zhang, Yanrong;Zhang, Lizhi
作者机构：
[Wang, Xiaoguang; Sun, Minghui; Zhang, Yanrong] Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China.;[Murugananthan, Muthu] PSG Coll Technol, Dept Chem, Coimbatore 641004, Tamil Nadu, India.;[Zhang, Lizhi] Cent China Normal Univ, Inst Environm Chem, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Zhang, Yanrong] H;[Zhang, Lizhi] C;Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China.;Cent China Normal Univ, Inst Environm Chem, Wuhan 430079, Hubei, Peoples R China.
关键词：
Electrochemical self-doping;Oxygen vacancy;Photocatalysis;VOC degradation;WO3/TiO2 nanotubes
摘要：
In this study, an electrochemically self-doped WO3/TiO2 nanotubes (R-WO3/TNTs) composite film was developed for the photocatalytic degradation of waste gas. The doping of oxygen vacancies (OVs) into the heterojunction of WO3/TNTs was conducted by a simple electrochemical approach, by which the quantity and distribution of OVs on surface as well as bulk were tailored with respect to the applied cathodic potential and the duration of the treatment. With an increase of applied cathodic potential as well as the duration, the quantity of OVs on WO3/TNTs was observed to be consistently raised, while those presented in the surface were raised initially and further showed a plateau trend as the duration extended at a fixed potential. The incorporation of OVs into WO3/TNTs enhanced the charge-transport resistance and reduced the electron-hole recombination, thereby showed an enhanced photocatalytic performance. The R-WO3/TNTs prepared by the electrochemical polarization process at −1.4 V (vs SCE) exhibited a 12 times higher photo-current density and obviously, an enhanced efficiency in the photocatalytic degradation of VOCs with a prolonging photostability compared to that of the pristine WO3/TNTs, under a simulated solar light irradiation. The single-time purification trial demonstrated the effectiveness of the R-WO3/TNTs composite in treating the VOCs for the practical application. © 2019 Elsevier B.V.
语种：
英文
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Enhanced adsorption and photocatalytic degradation of perfluorooctanoic acid in water using iron (hydr)oxides/carbon sphere composite
作者：
Xu, Tianyuan;Ji, Haodong;Gu, Yu;Tong, Tianyi;Xia, Yabei;...
期刊：
Chemical Engineering Journal ,2020年388:124230 ISSN：1385-8947
通讯作者：
Zhao, Dongye
作者机构：
[Zhao, Dongye; Ji, Haodong; Gu, Yu; Xu, Tianyuan] Auburn Univ, Dept Civil Engn, Environm Engn Program, Auburn, AL 36849 USA.;[Zhang, Lizhi; Tong, Tianyi; Xia, Yabei; Xu, Tianyuan] Cent China Normal Univ, Minist Educ, Key Lab Pesticide & Chem Biol, Inst Environm & Appl Chem,Coll Chem, Wuhan 430079, Peoples R China.
通讯机构：
[Zhao, Dongye] A;Auburn Univ, Dept Civil Engn, Environm Engn Program, Auburn, AL 36849 USA.
关键词：
Adsorption;Concentrate and destroy;Persistent organic pollutant;PFAS;PFOA;Photocatalysis
摘要：
Perfluorooctanoic acid (PFOA) has been widely detected in aquatic systems. Yet, cost-effective technologies for degrading PFAS have been lacking. We prepared and tested an adsorptive photocatalyst consisting of iron (hydr)oxides and carbon spheres (FeO/CS) through a one-step hydrothermal process. Characterization results revealed that the presence of carbon spheres affected the crystal formation of iron (hydr)oxides, and resulted in mutually modified mixed phases ferrihydrite and carbon spheres. FeO/CS was able to effectively adsorb and then degrade the pre-sorbed PFOA under simulated solar light. FeO/CS(1:1), prepared at an Fe:Glucose molar ratio of 1:1, showed the highest PFOA adsorption capacity and photoactivity. At a dosage of 1.0 g/L, FeO/CS(1:1) adsorbed nearly all 200 µg/L of PFOA within 1 h, and when the PFOA-laden FeO/CS(1:1) was subjected to simulated solar light at neutral pH, 95.2% of pre-concentrated PFOA was photodegraded and 57.2% defluorinated in 4 h. The efficient degradation also regenerated the material, allowing for repeated uses of the material without chemical regeneration. The much enhanced adsorption and photocatalytic activity of FeO/CS was attributed to: 1) CS facilitated formation of ferrihydrite, leading to adsorption of PFOA via binuclear and bidentate complexation, and 2) a hybrid ferrihydrite-CS structure, enabling multi-point, corporative adsorption of PFOA, and increasing direct electron extraction from PFOA under solar light irradiation. Moreover, [rad]OH radicals played an important role in PFOA degradation. Lastly, a photodegradation mechanism is proposed based on experimental findings and density functional theory calculations. © 2020 Elsevier B.V.
语种：
英文
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Insight into the effect of bromine on facet-dependent surface oxygen vacancies construction and stabilization of Bi2MoO6 for efficient photocatalytic NO removal
作者：
Wang, Shengyao* ;Ding, Xing;Yang, Nan;Zhan, Guangming;Zhang, Xuehao;...
期刊：
Applied Catalysis B: Environmental ,2020年265:118585 ISSN：0926-3373
通讯作者：
Wang, Shengyao;Chen, Hao
作者机构：
[Ding, Xing; Wang, Shengyao; Wang, SY; Chen, Hao; Yang, Nan; Zhang, Xuehao] Huazhong Agr Univ, Coll Sci, Wuhan 430070, Peoples R China.;[Zhang, Lizhi; Zhan, Guangming] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Inst Environm Chem, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.;[Dong, Guohui] Shaanxi Univ Sci & Technol, Sch Environm Sci & Engn, Xian 710021, Peoples R China.
通讯机构：
[Wang, SY; Chen, H] H;Huazhong Agr Univ, Coll Sci, Wuhan 430070, Peoples R China.
关键词：
Bi2MoO6;Bromine;Facet;NO removal;Oxygen vacancy
摘要：
Surface oxygen vacancies (OVs) are believed as active sites for photocatalytic NO removal. The construction and stabilization of OVs on materials, especially from the point of view of exogenous ions towards different facets is vital for OVs-mediated photocatalysis. Herein, the impact of bromide ions (Br−) on OVs construction on different facets of Bi2MoO6 was systematically investigated. Theoretical calculations and characterizations demonstrated that Br− can boost and stabilize the OVs on {001} facets of Bi2MoO6, while hardly affect that on {010} facets. The Br- induced OVs on Bi2MoO6 caused a light-absorption until near-infrared region and enhanced the molecular oxygen activation, thus endowing the OVs concentration optimized Bi2MoO6 (BMO-001-Br) with superior activity on NO removal (62.9%) and selectivity of NO complete oxidation (93.61%) in a flow reaction. This work provides new insight into understanding the exogenous ions on construction and stabilization of OVs and the roles of OVs in photocatalytic NO removal. © 2019
语种：
英文
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A one-step acidification strategy for sewage sludge dewatering with oxalic acid
作者：
Chen, Na;Tao, Shuangyi;Xiao, Keke;Liang, Sha;Yang, Jiakuan;...
期刊：
Chemosphere ,2020年238(Jan.):124598 ISSN：0045-6535
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Chen, Na] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Xiao, Keke; Liang, Sha; Yang, Jiakuan; Tao, Shuangyi] Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Hubei, Peoples R China.
通讯机构：
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词：
Extracellular polymeric substances;Hydrolysis;Oxalic acid;Pectins;Sewage sludge dewatering
摘要：
Sewage sludge dewatering is an efficient approach to reduce the volume of sludge for the subsequent disposal. In this study, a novel one-step acidification sludge dewatering method was developed with using oxalic acid as a conditioner. In laboratory-scale experiments with the dosage of 200 mg/g dry solid (DS), the normalized capillary suction time and the specific resistance to filtration were respectively decreased by 78.7% and 60.0% after 30 min of oxalic acid conditioning, much more efficient than those conditioned with sulfuric acid and hydrochloric acid at the same pH value. This superior dewatering performance was attributed to two factors. One was that oxalic acid could more efficiently promote the hydrolysis of polysaccharide, especially pectins, to release bound water. The other was that OA could dissolve more Fe3+ and Al3+, as well as form precipitate with Ca2+ in sludge, which may act as flocculants or co-precipitator for the subsequent sludge particles coagulation. In pilot-scale experiments, the water content of oxalic acid conditioned sludge cake was reduced to 60% under the optimum conditions, while the reagent cost was as low as 110.0 USD/t DS. This work provides a cost-effective and easy-operated sewage sludge disposal technique, and also sheds light on the potential of oxalic acid in environmental waste treatment. (C) 2019 Elsevier Ltd. All rights reserved.
语种：
英文
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Visible light promoted Fe3S4 Fenton oxidation of atrazine
作者：
Shi, Yanbiao;Wang, Xiaobing;Liu, Xiufan;Ling, Cancan;Shen, Wenjuan;...
期刊：
Applied Catalysis B: Environmental ,2020年277:119229 ISSN：0926-3373
通讯作者：
Zhang, Lizhi
作者机构：
[Ling, Cancan; Zhang, Lizhi; Liu, Xiufan; Shi, Yanbiao; Wang, Xiaobing; Shen, Wenjuan] Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol Minist Educ, Wuhan 430079, Peoples R China.;[Shen, Wenjuan] Wuhan Polytech Univ, Coll Chem & Environm Engn, Wuhan 430023, Peoples R China.
通讯机构：
[Zhang, Lizhi] C;Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol Minist Educ, Wuhan 430079, Peoples R China.
关键词：
Atrazine degradation;Heterogeneous Fenton reaction;Reusability;Surface iron redox cycle;Visible light irradiation
摘要：
We demonstrate that visible light irradiation can promote Fe3S4 Fenton oxidation of atrazine. The visible light irradiation could increase the atrazine Fenton degradation rate by 4.9 times. The enhanced atrazine degradation activity under visible light was attributed to the higher surficial Fe(II)/Fe(III) ratio of Fe3S4 and the efficient surface iron redox cycle triggered by visible light. Experimental results revealed that the operando formation of FeOOH on the Fe3S4 surface blocked the iron redox cycle and inhibited the H2O2 decomposition, accounting for the largely decreased Fenton activity of Fe3S4 in dark, while these problems were successfully solved by the introduction of visible light irradiation, which excite Fe3S4 to produce abundant photo-generated electrons and [rad]O2− for efficient regeneration of active Fe(II) species of Fe3S4 and in-situ formed FeOOH. © 2020 Elsevier B.V.
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
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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Pyrite enables persulfate activation for efficient atrazine degradation
作者：
Wang, Xiaobing;Wang, Yueyao;Chen, Na;Shi, Yanbiao;Zhang, Lizhi*
期刊：
Chemosphere ,2020年244:125568 ISSN：0045-6535
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Shi, Yanbiao; Wang, Xiaobing; Chen, Na; Wang, Yueyao] Cent China Normal Univ, Coll Chem, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构：
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
关键词：
Atrazine degradation;Fe(III)/Fe(II) cycle;Iron-contained minerals;Persulfate activation;Pyrite
摘要：
Persulfate (PS) is widely used for environmental remediation, but its organic contaminant removal performance strongly depends on its activation. In this study, we demonstrate that pyrite (FeS2) can more effectively activate PS than the commonly used FeSO4 for atrazine degradation. When 3.0 mM of PS and 4.2 mM of iron salts were used, the atrazine degradation efficiency of FeS2/PS was 1.4 times that of FeSO4/PS, while the amount of consumed PS in case of FeS2 was only 53% of that by FeSO4. The better PS activation performance of FeS2 could be attributed to its slow and sustainable release of dissolved Fe(II), inhibiting the quenching reaction between •SO4−/•OH and Fe(II) ions, and thus producing more reactive oxygen species for the atrazine degradation. More importantly, the surface bound Fe(II) of FeS2 could activate molecular oxygen to generate superoxide radical (•O2−), which could further promote the effective decomposition of PS by accelerating the Fe(III)/Fe(II) redox cycle. This study unravels the roles of dissolved Fe(II) and surface bound Fe(II) on the persulfate activation, and provides a promising heterogeneous persulfate activator for pollutant control and environmental remediation. © 2019 Elsevier Ltd
语种：
英文
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Simulated solar light driven roxarsone degradation and arsenic immobilization with hematite and oxalate
作者：
Chen, Na;Wan, Yichao;Zhan, Guangming;Wang, Xiaobing;Li, Meiqi;...
期刊：
Chemical Engineering Journal ,2020年384:123254 ISSN：1385-8947
通讯作者：
Zhang, Lizhi
作者机构：
[Zhang, Lizhi; Chen, Na; Wang, Xiaobing; Zhan, Guangming; Li, Meiqi; Wan, Yichao] 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：
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词：
Arsenic immobilization;Iron oxides;Oxalate;Roxarsone degradation;Solar light
摘要：
Solar light driven organoarsenicals degradation and simultaneous inorganic arsenic immobilization with naturally abundant hematite is very promising for organoarsenicals remediation, but suffers from the fast electron-hole charge recombination of hematite. Herein, we report that oxalate, widely existed in soil and water environments, can greatly enhance the photocatalytic molecular oxygen activation of hematite to degrade a typical organoarsenical roxarsone and immobilize the resulted inorganic arsenic. It was found that oxalate could chelate with surface Fe(III) of hematite to generate plenty of •OH via a surface Fe(III)/Fe(II) cycle mediated oxygen molecular activation process under a simulated solar light, and thus induced 85.1% of roxarsone transformation into inorganic arsenic species, mainly As(V), within 6 h. The generated As(V) could be further adsorbed on hematite surface with prolonging the reaction time to 24 h in dark, avoiding secondary pollution. More importantly, hematite was reusable for the simulated solar light driven roxarsone degradation and As(V) immobilization in the presence of oxalate. This study offers a green and effective strategy for organoarsenicals remediation, and also sheds light on the environmental effects of iron oxides and oxalate. © 2019 Elsevier B.V.
语种：
英文
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Atomic-Scale Tuning of Graphene/Cubic SiC Schottky Junction for Stable Low-Bias Photoelectrochemical Solar-to-Fuel Conversion
作者：
Li, Hao;Shi, Yuchen;Shang, Huan;Wang, Weimin;Lu, Jun;...
期刊：
ACS Nano ,2020年14(4):4905-4915 ISSN：1936-0851
通讯作者：
Sun, Jianwu
作者机构：
[Wang, Weimin; Hultman, Lars; Uhrberg, Roger I. G.; Shi, Yuchen; Li, Hao; Lu, Jun; Syvaejaervi, Mikael; Yakimova, Rositsa; Sun, Jianwu] Linkoping Univ, Dept Phys Chem & Biol IFM, Linkoping 58183, Sweden.;[Zhang, Lizhi; Shang, Huan] Cent China Normal Univ, Coll Chem, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Wang, Weimin; Zakharov, Alexei A.] Max IV Lab, SE-22484 Lund, Sweden.
通讯机构：
[Sun, Jianwu] L;Linkoping Univ, Dept Phys Chem & Biol IFM, Linkoping 58183, Sweden.
关键词：
CO2 reduction;Schottky junction;SiC;graphene;photoelectrochemistry
摘要：
Engineering tunable graphene-semiconductor interfaces while simultaneously preserving the superior properties of graphene is critical to graphene-based devices for electronic, optoelectronic, biomedical, and photoelectrochemical applications. Here, we demonstrate this challenge can be surmounted by constructing an interesting atomic Schottky junction via epitaxial growth of high-quality and uniform graphene on cubic SiC (3C-SiC). By tailoring the graphene layers, the junction structure described herein exhibits an atomic-scale tunable Schottky junction with an inherent built-in electric field, making it a perfect prototype to systematically comprehend interfacial electronic properties and transport mechanisms. As a proof-of-concept study, the atomic-scale-tuned Schottky junction is demonstrated to promote both the separation and transport of charge carriers in a typical photoelectrochemical system for solar-to-fuel conversion under low bias. Simultaneously, the as-grown monolayer graphene with an extremely high conductivity protects the surface of 3C-SiC from photocorrosion and energetically delivers charge carriers to the loaded cocatalyst, achieving a synergetic enhancement of the catalytic stability and efficiency.
语种：
英文
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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.
语种：
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.
语种：
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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Smart pH-Regulated Switchable Nanoprobes for Photoelectrochemical Multiplex Detection of Antibiotic Resistance Genes
作者：
Li, Xin;Lu, Junmiao;Feng, Lizhen;Zhang, Lizhi;Gong, Jingming*
期刊：
Analytical Chemistry ,2020年92(16):11476-11483 ISSN：0003-2700
通讯作者：
Gong, Jingming
作者机构：
[Feng, Lizhen; Zhang, Lizhi; Lu, Junmiao; Gong, Jingming; Li, Xin] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ,Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Wuhan 430079, Peoples R China.
通讯机构：
[Gong, Jingming] C;Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ,Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Wuhan 430079, Peoples R China.
摘要：
Antibiotic resistance, encoded via particular genes, has become a major global health threat and substantial burden on healthcare. Hence, the facile, low-cost, and precise detection of antibiotic resistance genes (ARGs) is crucial in the realm of human health and safety, especially multiplex sensing assays. Here, a smart pH-regulated switchable photoelectrochemical (PEC) bioassay has been created for ultrasensitive detection of two typical subtypes of penicillin resistance genes bla-CTX-M-1 (target 1, labeled as TDNA1) and bla-TEM (target 2, labeled as TDNA2), whereby pH-responsive antimony tartrate (SbT) complex-grafted silica nanospheres are ingeniously adopted as signal DNA1 tags (labeled as SDNA1-SbT@SiO2NSs). The operations of the PEC bioassay depend on the switchable dissociation of the pH-responsive SDNA1-SbT@SiO2NSs complex under the external pH stimuli, thus initiating the pH-regulated release of ions pre-embedded in sandwich-type DNA nanoassemblies. At acidic conditions, the dissociation of SDNA1 tags (ON state) triggers the release of the embedded SbO+. Under alkaline conditions, the dissociation of SDNA1 tags is inhibited (OFF state). The detection of TDNA2 was achieved via DNA hybridization-triggered metal ion release. The unwinding of the introduced hairpin T-Hg2+-T fragment, hybridized with the second anchored signal DNA (SDNA2), ignites the release of Hg2+. The released SbO+ or Hg2+ ions would trigger the formation of Sb2S3/ZnS or HgS/ZnS heterostructure through ion-exchange with the photosensitive ZnS layer, giving rise to the amplified photocurrents and eventually realizing the ultrasensitive detection of penicillin resistance genes subtypes, bla-CTX-M-1 and bla-TEM. The as-fabricated pH-regulated PEC bioassay, smartly integrating the pH-responsive intelligent unit as SDNA tags, pH-regulated release of embedded ions, and the subsequent ion-exchange-based signal amplification strategy, exhibits high sensitivity, specificity, low-cost, and ease of use for multiplex detection of ARGs. It can be successfully used for measuring bla-CTX-M-1 and bla-TEM in real E. coli plasmids, demonstrating great promise for developing a new class of genetic point-of-care devices. © 2020 American Chemical Society.
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Elucidating the Nature of the Cu(I) Active Site in CuO/TiO2 for Excellent Lowerature CO Oxidation
作者：
Fang, Yarong;Chi, Xiao;Li, Li;Yang, Ji;Liu, Shoujie;...
期刊：
ACS Applied Materials & Interfaces ,2020年12(6):7091-7101 ISSN：1944-8244
通讯作者：
Luo, Zhu;Guo, Yanbing;Gao, Puxian
作者机构：
[Luo, Zhu; Guo, YB; Zhang, Lizhi; Li, Li; Yang, Weiwei; Guo, Yanbing; Liu, Shoujie; Yang, Ji; Deng, Hongtao; Xiong, Juxia; Hoang, Son; Hu, Siyu; Fang, Yarong] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Lu, Xingxu; Gao, Puxian] Univ Connecticut, Dept Chem Mat & Biomol Engn, Inst Mat Sci, Storrs, CT 06269 USA.;[Chi, Xiao] Natl Univ Singapore, Singapore Synchrotron Light Source, Singapore 117603, Singapore.;[Ding, Jun; Xiao, Wen] Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore.;[Wang, Liming] Chinese Acad Sci, CAS Key Lab Biomed Effects Nanomat & Nanosafety, Inst High Energy Phys, Dept Mat Sci & Engn, Beijing 100049, Peoples R China.
通讯机构：
[Luo, Z; Guo, YB] C;[Gao, Puxian] U;Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;Univ Connecticut, Dept Chem Mat & Biomol Engn, Inst Mat Sci, Storrs, CT 06269 USA.
关键词：
CO adsorption;Ti-doped CuO;Ti-O-Cu hybridization;activated O;stabilized Cu+
摘要：
Stabilized Cu+ species have been widely considered as catalytic active sites in composite copper catalysts for catalytic reactions with industrial importance. However, few examples comprehensively explicated the origin of stabilized Cu+ in a low-cost and widely investigated CuO/TiO2 system. In this study, mass producible CuO/TiO2 catalysts with interface-stabilized Cu+ were prepared, which showed excellent lowerature CO oxidation activity. A thorough characterization and theoretical calculations proved that the strong charge-transfer effect and Ti-O-Cu hybridization in Ti-doped CuO(111) at the CuO/TiO2 interface contributed to the formation and stabilization of Cu+ species. The CO molecule adsorbed on Cu+ and reacted directly with Ti doping-promoted active lattice oxygen via a Mars-van Krevelen mechanism, leading to the enhanced lowerature activity. © 2020 American Chemical Society.
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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.
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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. © 2019 The Royal Society of Chemistry.
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英文
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Bifunctional S, N-Codoped carbon dots-based novel electrochemiluminescent bioassay for ultrasensitive detection of atrazine using activated mesoporous biocarbon as enzyme nanocarriers
作者：
Wu, Yunqing;Chen, Yuxin;Zhang, Shiqin;Zhang, Lizhi;Gong, Jingming*
期刊：
Analytica Chimica Acta ,2019年1073:45-53 ISSN：0003-2670
通讯作者：
Gong, Jingming
作者机构：
[Zhang, Shiqin; Zhang, Lizhi; Chen, Yuxin; Gong, Jingming; Wu, Yunqing] Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Gong, Jingming] C;Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
关键词：
Atrazine;Bifunctional S;Dissolved oxygen;Electrochemiluminescent bioassay;Mesoporous bicarbons;N-codoped carbon dots
摘要：
A novel and ultrasensitive electrochemiluminescent (ECL) bioassay has been developed for the detection of atrazine (ATZ), whereby bifunctional S, N-codoped carbon dots (S, N-CDs) and activated mesoporous bicarbons (BCs) have been innovatively integrated to synergistically amplify the ECL signal. When endogenous dissolved O2 is used as a coreactant, its sluggish reduction hinders the enhancement of ECL intensity of the luminophore, thus restricting its further application in bioanalysis. Here, bifunctional S, N-CDs severe as not only the ECL luminophore but the coreaction accelerator of dissolved O2 to generate more intermediates to boost the coreaction without using any other coreactant and coreaction accelerator. The as-formed nanoarchitectures of BCs possess enlarged surface area as the nanocarriers. They could provide adequate active sites for immobilization of tyrosinase (Tyr), which greatly prompts the ECL bioassay applications. Such a smart integration of bifunctional S, N-CDs, activated mesoporous BCs and the enzyme inhibition reaction achieves a unique and attractive high-performance signal-on ECL bioassay, realizing ultrasensitive detection of ATZ. Under the optimal condition, this bioassay exhibits two linear ranges, from 0.0001 to 0.01 μg L−1 and 0.01–20 μg L−1 with a detection limit of 0.08 ng L−1 at signal to noise ratio of 3. The as-fabricated assay is sensitive and economical, opening a new way for the enhancement of ECL signal output and a versatile strategy for ultrasensitive ECL bioanalysis. © 2019 Elsevier B.V.
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英文
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Protocatechuic acid promoted catalytic degradation of rhodamine B with Fe@Fe2O3 core-shell nanowires by molecular oxygen activation mechanism
作者：
Qin, Yaxin;Li, Guiying;Zhang, Lizhi* ;An, Taicheng*
期刊：
Catalysis Today ,2019年335:144-150 ISSN：0920-5861
通讯作者：
An, Taicheng;Zhang, Lizhi
作者机构：
[An, Taicheng; Qin, Yaxin; Li, Guiying] Guangdong Univ Technol, Sch Environm Sci & Engn, Inst Environm Hlth & Pollut Control, Guangzhou Key Lab Environm Catalysis & Pollut Con, Guangzhou 510006, Guangdong, Peoples R China.;[Zhang, Lizhi] 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：
[An, Taicheng] G;[Zhang, Lizhi] C;Guangdong Univ Technol, Sch Environm Sci & Engn, Inst Environm Hlth & Pollut Control, Guangzhou Key Lab Environm Catalysis & Pollut Con, Guangzhou 510006, Guangdong, Peoples R China.;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：
Complexing and reduction abilities;Fe(III)/Fe(II) cycle;[email protected]2O3 core-shell nanowires;Molecular oxygen activation;Protocatechuic acid addition
摘要：
The addition of ligands into the system of zero valent iron is an effective method to promote the yields of pollutants oxidant but may lead to the unfavorable environmental consequences. In this study, the addition effects of protocatechuic acid (PCA), a kind of complexing and reducing agent widely existed in many plants, on the molecular oxygen activation and the subsequent aerobic rhodamine B degradation by Fe@Fe2O3 core-shell nanowires were investigated. Results indicated that the degradation efficiency of rhodamine B increased from less than 6% to 92.4% within 120 min with the PCA addition in the system of Fe@Fe2O3 core-shell nanowires. This addition of PCA not only promote the molecular oxygen activation efficiencies induced by Fe@Fe2O3 core-shell nanowires, but also accelerate the Fe(III)/Fe(II) cycle to guarantee enough soluble Fe(II) for subsequent efficient Fenton reaction. Moreover, PCA can also defer the oxidation of Fe@Fe2O3 core-shell nanowires for its reduction ability. X-ray photoelectron spectroscopy and X-ray diffraction characterization revealed that there were no significant changes of the compositions of Fe@Fe2O3 core-shell nanowires before and after reactions in the system with PCA addition. Meanwhile, only slightly decrease of the rhodamine B degradation efficiency was observed after 4 cycles in the system of Fe@Fe2O3 core-shell nanowires and PCA. This study not only clarify the effects of PCA on the molecular oxygen activation by nanoscale zero-valent iron, but also sheds new insight into the possible roles of widely existed phenolic acids in the transformation of organic contaminants with nanoscale zero-valent iron in natural aquatic environment. © 2018 Elsevier B.V.
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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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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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