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Highly selective and efficient photocatalytic NO removal:Charge carrier kinetics and interface molecular process

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Nano Research 2024年第3期17卷 1003-1026页

作者： Huan Shang Hongbao Jia Pengpeng Li Hao Li Wenbin Zhang Shuangjun Li Qing Wang Shuning Xiao Ding Wang Guisheng Li Dieqing Zhang School of Materials and chemistry University of Shanghai for Science and TechnologyShanghai 200093China the education ministry key lab of resource chemistry Joint International Research Laboratory of Resource Chemistry of Ministry of EducationShanghai Key Laboratory of Rare Earth Functional Materialsand Shanghai Frontiers Science Center of Biomimetic CatalysisShanghai Normal UniversityShanghai 200234China School of Environmental Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China

The widespread nitrogen oxides(NOx,mainly in NO)in the atmosphere have threatened human health and ecological environment.The dilute NO(ppb)is difficult to efficiently remove via the traditional process due to its characteristics of low concentration,wide range,large total amount,etc.Photocatalysis can utilize solar energy to purify NO pollutants under mild conditions,but its application is limited due to the low selectivity of nitrate and poor activity of NO removal.The underlying reason is that the interface mechanism of NO oxidation is not clearly understood,which leads to the inability to accurately regulate the NO oxidation process.Herein,the recent advances in the photocatalytic oxidation of NO are summarized.Firstly,the common strategies to effectively regulate carrier dynamics such as morphology control,facet engineering,defect engineering,plasma coupling,heterojunction and single-atom catalysts are discussed.Secondly,the progress of enhancing the adsorption and activation of reactants such as NO and O_(2) during NO oxidation is described in detail,and the corresponding NO oxidation mechanisms are enumerated.Finally,the challenges and prospects of photocatalytic NO oxidation are presented in term of nanotechnology for air pollution control.This review can shed light on the interface mechanism of NO oxidation and provide illuminating information on designing novel catalysts for efficient NOx control.

关键词： nitrogen oxide(NO)oxidation photocatalysis NO/O_(2)activation charge carrier kinetics interfacial mechanism

Hollow Ni Mo-based nitride heterojunction with super-hydrophilic/aerophobic surface for efficient urea-assisted hydrogen production

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Journal of Energy chemistry 2024年第8期95卷 428-439页

作者： Yuying Fan Ying Gu Dongxu Wang Yanqing Jiao Aiping Wu Chungui Tian key laboratory of Functional Inorganic Material chemistry Ministry of Education of the People's Republic of China Heilongjiang University College of chemistry Chemical Engineering and Resource Utilization Northeast Forestry University

Hydrogen evolution reaction（HER） and urea oxidation reaction（UOR） are key reactions of the watercycling associated catalytic process/device.The design of catalysts with a super-hydrophilic/aerophobic structure and optimized electron distribution holds great promise.Here,we have designed a threedimensional（3D） hollow Ni/NiMoN hierarchical structure with arrayed-sheet surface based on a onepot hydrothermal route for efficient urea-assisted HER based on a simple hydrothermal process.The Ni/NiMoN catalyst exhibits super-hydrophilic/aerophobic properties with a small droplet contact angle of 6.07° and an underwater bubble contact angle of 155.7°,thus facilitating an escape of bubbles from the electrodes.Density functional theory calculations and X-ray photoelectron spectroscopy results indicate the optimized electronic structure at the interface of Ni and NiMoN,which can promote the adsorption/desorption of reactants and intermediates.The virtues combining with a large specific surface area endow Ni/NiMoN with efficient catalytic activity of low potentials of 25 mV for HER and 1.33 V for UOR at10 mA cm-2.The coupled HER and UOR system demonstrates a low cell voltage of 1.42 V at 10 mA cm-2,which is approximately 209 mV lower than water electrolysis.

关键词： Hollow heterojunctions Hydrogen evolution Super hydrophilic/aerophobic Transition metal nitrides Urea electrooxidation

Visible Light-Induced Photocatalysis:Self-Fenton Degradation of p-CIPhOH Over Graphitic Carbon Nitride by a Polyethylenimine Bifunctional Catalyst

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Transactions of Tianjin University 2024年第2期30卷 130-139页

作者： Yuan Bai Shuangjun Li Bolin Yin Jinpeng Zhao Hexing Li key laboratory of resource chemistry of ministry of education Shanghai Key Laboratory of Rare Earth Functional MaterialsCollege of Chemistry and Materials ScienceShanghai Normal UniversityShanghai 200234China

Deep degradation of organic pollutants by sunlight-induced coupled photocatalytic and Fenton (photo-Fenton) reactions is of immense importance for water purification. In this work, we report a novel bifunctional catalyst (Fe-PEI-CN) by codoping graphitic carbon nitride (CN) with polyethyleneimine ethoxylated (PEI) and Fe species, which demonstrated high activity during p-chlorophenol (p-ClPhOH) degradation via H_(2)O_(2) from the photocatalytic process. The relationship between the catalytic efficiency and the structure was explored using diff erent characterization methods. The Fe modification of CN was achieved through Fe-N coordination, which ensured high dispersion of Fe species and strong stability against leaching during liquid- phase reactions. The Fe modification initiated the Fenton reaction by activating H_(2)O_(2) into ·OH radicals for deep degradation of p-ClPhOH. In addition, it eff ectively promoted light absorption and photoelectron-hole (e-h ^(+) ) separation, corresponding to improved photocatalytic activity. On the other hand, PEI could significantly improve the ability of CN to generate H_(2)O_(2) through visible light photocatalysis. The maximum H_(2)O_(2) yield reached up to 102.6 μmol/L, which was 22 times higher than that of primitive CN. The cooperation of photocatalysis and the self-Fenton reaction has led to high-activity mineralizing organic pollutants with strong durability, indicating good potential for practical application in wastewater treatment.

关键词： Fe-PEI-CN bifunctional catalyst Photo-Fenton p-chlorophenol(p-ClPhOH)degradation Synergetic effect

The response and anti-stress mechanisms of nitrifying sludge under long-term exposure to Cd Se quantum dots

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Journal of Environmental Sciences 2024年第1期135卷 174-184页

作者： Linkai Guo Lei Yang Yongxiang Ren Shen Cui Xiaotong Li Jia Wang Jun Lan Haoqi Lu Yuchao Wang Shaanxi key laboratory of Environmental Engineering Xi’an University of Architecture and TechnologyXi’an 710055China key lab of Northwest Water resource Environment and EcologyMinistry of EducationXi’an University of Architecture and TechnologyXi’an 710055China

The wide application of CdSe quantum dots(QDs)increases its stress risk to sewage treatment systems.This study evaluated the response of nitrification performance,floc characteristics and microbial community of nitrifying sludge under long-term exposure to CdSe QDs.Results showed CdSe QDs(≥1 mg/L)would decrease the activity of ammonia monooxygenase(AMO).Under the stress of 30 mg/L CdSe QDs,the activity of AMO was reduced by 66%,while the activities of hydroxylamine oxidase and nitrite oxidoreductase were enhanced by 19.1%and 26%,respectively.Thus,the final nitrification effects were not adversely affected,and the production rates of NO_(2)^(-)-N and NO_(3)^(-)-N were accelerated.Additionally,CdSe QDs improved biomass concentration in sludge and maintained the stability of sludge settleability.High throughput sequencing analysis showed that CdSe QDs evidently reduced the abundance and diversity of microbial community in nitrifying sludge.The abundances of amino acid metabolism and lipid metabolism were enriched.Moreover,CdSe QDs decreased the fluorescence intensity of tryptophan-like protein from 2,326 to 1,179 a.***.in loosely bound extracellular polymeric substances(EPSs)and from 3,792 to 3,117 a.***.in tightly bound EPSs.To relieve CdSe QD stress,the polysaccharide content increased from0.31 to 0.61 mg/g MLSS and intracellular antioxidant defense was activated.With CdSe QD level increasing to 30 mg/L,the total antioxygenic capacity and the activities of catalase were enhanced up to 411%and 143.2%,respectively.Thereby,CdSe QDs had little adverse effects on cell membrane integrity,microbial metabolism and the abundance of Nitrospirae.

关键词： Quantum dots Activated sludge Extracellular polymeric substances Microbial community Antioxidant effect

Soil inorganic amendments produce safe rice by reducing the transfer of Cd and increasing key amino acids in brown rice

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Journal of Environmental Sciences 2024年第2期136卷 121-132页

作者： Fanyi Kong Shenggao Lu Zhejiang Provincial key laboratory of Agricultural resources and Environment Key Laboratory of Environmental Remediation and Ecosystem HealthMinistry of EducationCollege of Environmental and Resource SciencesZhejiang UniversityHangzhou 310058China

The digestibility of cadmium(Cd)in brown rice is directly related to amino acid metabolism in rice and human health.In our field study,three kinds of alkaline calcium-rich soil inorganic amendments(SIAs)at three dosages were applied to produce safe rice and improve the quality of rice in Cd-contaminated paddy.With the increased application of SIA,Cd content in iron plaque on rice root significantly increased,the transfer of Cd from rice root to grain significantly decreased,and then Cd content in brown rice decreased synchronously.The vitro digestibility of Cd in brown rice was estimated by a physiologically based extraction test.Results showed that more than 70%of Cd in brown rice could be digested by simulated gastrointestinal juice.Based on the total and digestible Cd contents in brown rice to evaluate the health risk,the application of 2.25 ton SIA/ha could produce safe rice in acidic slightly Cd-contaminated paddy soils.The amino acids(AAs)in brown rice were determined by high-performance liquid chromatography.The contents of 5 key AAs(KAAs)that actively respond to environmental changes increased significantly with the increased application of SIA.The structural equation model indicated that KAAs could be affected by the Cd translocation capacity from rice root to grain,and consequently altered the ratio of indigestible Cd in brown rice.The formation of indigestible KAAs-Cd complexes by combining KAAs(phenylalanine,leucine,histidine,glutamine,and asparagine)with Cd in brown rice could be considered a potential mechanism for reducing the digestibility of Cd.

关键词： Cadmium digestibility Soil inorganic amendments Safe rice Amino acid Priming effect Health risk

Stable α-CsPbI3 with extremely red emission for expanding the color gamut

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Science China(Information Sciences) 2024年第5期67卷 311-317页

作者： Yong ZHANG Xin WEI Lei GAO Weijie ZHAO Changjiu SUN Junli WEI Mingjian YUAN Zhenhua NI Junpeng LU Hongwei LIU School of Physics and key laboratory of MEMS of the ministry of education Southeast University key laboratory of Advanced Energy Materials chemistry (ministry of education) Renewable Energy Conversion and Storage Center (RECAST) College of Chemistry Nankai University Jiangsu key lab on Opto-Electronic Technology School of Physics and TechnologyNanjing Normal University

The wider color gamut represents the better reproducibility of the real natural colors. Perovskite materials exhibit promising potential in full-color wide-gamut displays because of the wide tunability and high saturability of their photon emission. However, the full-color wide gamut(>100% Rec.2020) has not been constructed due to the lack of the extreme red primary color(～700 nm). Herein, the widest color gamut is realized, whereinα-CsPbI3 is used to generate the extreme red primary color. An in-situ encapsulation approach is advised to stabilizeα-CsPbI3 at room temperature by means of polyvinylpyrrolidone(PVP).Theα-CsPbI3 encapsulated by PVP(denoted as P-CPI) shows highly saturated(FWHM(full width at half maximum) ～28 nm) and extremely(～697 nm) red emission. The green emission is provided by P-CPBr(CsPbBr3 with PVP) which is also synthesized using the universal in-situ encapsulation approach. With the assistance of a commercial Ga N chip, the RGB gamut is extended to the widest(151% NTSC, 113%Rec.2020).

关键词： all-inorganic perovskite wide color gamut LED display carrier recombination

Phenylhydrazone anions excitation for the photochemical carbonylation of aryl iodides with aldehydes

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Chinese Chemical Letters 2024年第4期35卷 346-351页

作者： Lei Shen Yang Zhang Linlin Zhang Chuanwang Liu Zhixian Ma Kangjiang Liang Chengfeng Xia key laboratory of Medicinal chemistry for Natural resource Ministry of EducationYunnan Provincial Center for Research&Development of Natural ProductsSchool of PharmacyYunnan UniversityKunming 650500China

Spectroscopic investigations discovered that the in-situ generated phenylhydrazone anion was significantly bathochromically shifted to visible light region for photoactivation under irradiation. The photoexcited phenylhydrazone anion was potential to reduce aryl iodides via single electron transfer process for the subsequent radical chain reaction. A redox-neutral photochemical carbonylation of aryl iodides was developed on basis of the special spectroscopic features of phenylhydrazone anion. This protocol provided a convenient and efficient synthetic tool for accessing carbonylation products under redox neutral conditions without the need of transition-metals.

关键词： Organic anion Hydrazone Carbonylation Visible light Single electron transfer

Antimicrobial resistance characteristics and phylogenetic relationships of pleuromutilin-resistant Enterococcus isolates from different environmental samples along a laying hen production chain

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Journal of Environmental Sciences 2024年第3期137卷 195-205页

作者： Cong Lin Yuxuan Feng Xianjun Xie Haoyu Zhang Jie Wu Yixiao Zhu Jing Yu Jingyi Feng Wen Su Shanming Lai Anyun Zhang Animal Disease Prevention and Food Safety key laboratory of Sichuan Province Key Laboratory of Bio-Resource and Eco-Environment of Ministry of EducationCollege of Life SciencesSichuan UniversityChengdu 610065China

Antimicrobial resistance in the laying hen production industry has become a serious public health problem.The antimicrobial resistance and phylogenetic relationships of the common conditional pathogen Enterococcus along the laying hen production chain have not been systematically clarified.105 Enterococcus isolates were obtained from 115 environmental samples (air,dust,feces,fies,sewage,and soil) collected along the laying hen production chain (breeding chicken,chick,young chicken,and commercial laying hen).These Enterococcus isolates exhibited resistance to some clinically relevant antibiotics,such as tetracycline (92.4%),streptomycin (92.4%),and erythromycin (91.4%),and all strains had multidrug resistance phenotypes.Whole genome sequencing characterized 29 acquired antibiotic resistance genes (ARGs) that conferred resistance to 11 classes of antibiotics in 51pleuromutilin-resistant Enterococcus isolates,and lsa(E),which mediates resistance to pleuromutilins,always co-occurred with lnu(B).Alignments with the Mobile Genetic Elements database identified four transposons (Tn554,Tn558,Tn6261,and Tn6674) with several ARGs(erm(A),ant(9)-la,fex(A),and optrA) that mediated resistance to many clinically important antibiotics.Moreover,we identified two new transposons that carried ARGs in the Tn554 family designated as Tn7508 and Tn7492.A complementary approach based on conventional multi-locus sequence typing and whole genome single nucleotide polymorphism analysis showed that phylogenetically related pleuromutilin-resistant Enterococcus isolates were widely distributed in various environments on different production farms.Our results indicate that environmental contamination by antimicrobial-resistant Enterococcus requires greater attention,and they highlight the risk of pleuromutilin-resistant Enterococcus and ARGs disseminating along the laying hen production chain,thereby warranting effective disinfection.

关键词： Antimicrobial resistance Enterococcus Laying hen production chain Pleuromutilin

Facile synthesis of hierarchical NiO/NiFe2O4 microsphere composite as efficient visible photocatalyst for 2,4-DCP degradation

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Rare Metals 2024年第4期43卷 1580-1588页

作者： Shabana Shaheen Shuai Xu Ji Bian Amir Zada Zi-Qing Zhang Yang Qu Li-Qiang Jing key laboratory of Functional Inorganic Materials chemistry (ministry of education) International Joint Research Center and Lab for Catalytic TechnologySchool of Chemistry and Materials ScienceHeilongjiang University Department of chemistry Abdul Wali Khan University

It is highly desired to develop efficient photocatalysts with recycling property for practical application to degrade toxic pollutants.Herein,nanosheet-assembled NiFe2O4microspheres with commendable activity are successfully synthesized by a facile solvothermal reaction with NH4F as the modifier,and their photoactivities are further improved by coupling with NiO through an in situ growth process.The optimized nickel oxide（NiO）/nickel ferrite（NiFe2O4） microsphere composite（5NiO/NFO-4）exhibits a satisfactory photocatalytic activity for 2,4-dichlorophenol（2,4-DCP） degradation under visible-light irradiation,which is attributed to its wide visible-light response,well-designed hierarchical structure and enhanced charge transfer and separation by coupling NiO as a high-level energy platform to accept electrons.Moreover,it is found that the NiO/NiFe2O4microsphere photocatalysts can be easily collected and recycled owing to the distinctive magnetic properties.This work provides a feasible route to rational design visible-light-driven photocatalysts with high-activity for environmental remediation and purification with good recyclability.

关键词： NiFe 2 O 4 microspheres NiO/NiFe 2 O 4 composite Charge separation Visible-light photocatalysis 2,4-Dichlorophenol degradation