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Visible light-driven oxidation of non-native substrate by laccase attached on Ru-based metal-organic frameworks

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Journal of environmental sciences 2024年第3期137卷 741-753页

作者： Wenguang Huang Wentao Zhang Guantongyi Chen Yun Chen Jun Ma Dawei Huang Qinzheng Zhaoc Bingdang Wu State environmental Protection Key Laboratory of environmental Pollution Health Risk Assessment South China Institute of Environmental SciencesMinistry of Ecology and Environment of PRCGuangzhou 510655China Tsinghua Shenzhen International Graduate School Tsinghua UniversityShenzhen 518055China School of environmental science and Engineering Suzhou University of Science and TechnologySuzhou 215002China Key Laboratory of Suzhou Sponge City Technology Suzhou 215002China

Light-induced electron transfer can broaden the substrate range of ***,the efficiency of photo-enzyme coupling is limited by the poor combination of photosensitizer or photocatalyst with ***,we prepared the nano-photocatalyst MIL-125-NH_(2)@Ru(bpy)by in site embedding ruthenium pyridine-diimine complex[Ru(bpy)_(3)^(2+)into metal organic frameworks MIL-125-NH_(2)and associated it with multicopper oxidase(MCO)*** to[Ru(bpy)_(3)]^(2+),the coupling efficiency of MIL-125-NH_(2)@Ru(bpy)_(3)for enzymatic oxygen reduction increased by 35.7%.A series of characterizations confirmed that the amino group of laccase formed chemical bonds with the surface defects or hydrophobic groups of MIL-125-NH_(2)@Ru(bpy)_(3).Consequently,the tight binding accelerated the quenching process and electron transfer between laccase and the immobilized ruthenium pyridine-diimine *** work would open an avenue for the synthesis of MOFs photocatalyst towards photo-enzyme coupling.

关键词： Laccase Light-driven biocatalysis Ruthenium photocatalyst Metal-organic frameworks Enzyme immobilization

Multiple isotopes reveal the driving mechanism of high NO_(3)^(-) level and key processes of nitrogen cycling in the lower reaches of Yellow River

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Journal of environmental sciences 2024年第4期138卷 597-606页

作者： Qianqian Zhang Huiwei Wang Lu Liu Tianlun Zhai Xueqing Zhang Hebei and china Geological Survey Key Laboratory of Groundwater Remediation Institute of Hydrogeology and Environmental GeologyChinese Academy of Geological SciencesHebei 050061China Geo-environmental Monitoring institute of Hebei Province Hebei 050011China Hebei Provincial Laboratory of Water environmental science Hebei 050037China Hebei Provincial Academy of Ecological environmental science Hebei 050037China

The continuous increase of nitrate(NO_(3)^(-))level in rivers is a hot issue in the ***,the driving mechanism of high NO_(3)^(-)level in large rivers is still lacking,which has limited the use of river water and increased the cost of water *** this study,multiple isotopes and source resolution models are applied to identify the driving mechanism of high NO_(3)^(-)level and key processes of nitrogen cycling in the lower reaches of the Yellow River(LRYR).The major sources of NO_(3)^(-)were sewage and manure(SAM)in the low-flow season and soil nitrogen(SN)and chemical fertilizer(CF)in the high-flow *** was the most key process of nitrogen cycling in the ***,in the biological removal processes,denitrification may not occur *** temporal variation of contributions of NO_(3)^(-)sources were estimated by a source resolution model in the *** proportional contributions of SAM and CF to NO_(3)^(-)in the low-flow and high-flow season were 32.5%-52.3%,44.2%-46.2%and 36.0%-40.8%,54.9%-56.9%,*** driving mechanisms of high NO_(3)^(-)level were unreasonable sewage discharge,intensity rainfall runoff,nitrification and lack of nitrate removal *** control the NO_(3)^(-)concentration,targeted measures should be implemented to improve the capacity of sewage and wastewater treatment,increase the utilization efficiency of nitrogen fertilizer and construct ecological *** study deepens the understanding of the driving mechanism of high nitrate level and provides a vital reference for nitrogen pollution control in rivers to other area of the world.

关键词： Nitrate Driving mechanism Nitrogen cycle Source apportionment Transformation Yellow River

Prediction model on hydrolysis kinetics of phthalate monoester:A density functional theory study

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Journal of environmental sciences 2024年第1期135卷 51-58页

作者： Tong Xu Jingwen Chen Deming Xia Weihao Tang Jiansheng Cui Chun Liu Shuangjiang Li College of environmental science and Engineering Hebei University of Science and TechnologyShijiazhuang 050000China Key Laboratory of Industrial Ecology and environmental Engineering(Ministry of Education) School of Environmental Science and TechnologyDalian University of TechnologyDalian 116024China National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in south china Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and ManagementInstitute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China

As primary degradation products of phthalate esters,phthalate monoesters(MPEs)have been widely detected in various aquatic environments and drawn growing toxicological *** kinetics that is of importance for assessing environmental persistence of chemicals remain elusive for ***,kinetics of base-catalyzed and neutral hydrolysis for 18 MPEs with different leaving groups was investigated by density functional theory *** indicate that MPEs with leaving groups having p Kaof<10 prefer dissociative transition *** are more persistent than their parents,and their hydrolysis half-lives were calculated to vary from 3.4 min to 79.2 years(p H=7–9).A quantitative structure-activity relationship model was developed for predicting the hydrolysis kinetics *** was found that p Kaof the leaving groups and electronegativity of the MPEs are key factors determining the hydrolysis *** work may lay a theoretical foundation for better understanding the chemical process that governs MPE persistence in aquatic environments.

关键词： Phthalate monoesters Phthalate esters Hydrolysis Density functional theory Quantitative structure-activity relationship

Alternate disinfection approaches or raise disinfectant dosages for sewage treatment plants to address the COVID-19 pandemic?From disinfection efficiency,DBP formation,and toxicity perspectives

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Frontiers of environmental science & Engineering 2024年第9期18卷 115-128页

作者： Xiaobin Liao Xinyue Liu Yueyun He Xueping Tang Ruanjunjie Xia Yongjun Huang Wenhua Li Jing Zou Zhenming Zhou Mazhan Zhuang institute of Municipal and environmental Engineering College of Civil EngineeringHuaqiao UniversityXiamen 361021China Xiamen institute of environmental science Xiamen 361021China College of Biomedical sciences Huaqiao UniversityXiamen 361021China

During the COVID-19 pandemic,most sewage treatment plants increased disinfectant dosages to inactivate pathogenic viruses and microorganisms more ***,this approach also led to the production of more disinfection by-products(DBPs).To ensure both disinfection efficiency and a reduction in DBP formation,new disinfection protocols are *** this study,the disinfection efficiency,DBP amounts,and toxicity changes resulting from ozone(O_(3)),ultraviolet(UV),chlorine(Cl_(2)),and their combined processes were *** results demonstrated that the O_(3)/UV/Cl_(2)combination achieved the highest disinfection *** produced the most DBPs,whereas UV treatment reduced the formation of trihalomethane(THM),halogenated ketones(HKs),haloacetic acids(HAA),dichloroacetonitrile(DCAN)and N-nitrosodimethylamine(NDMA)by 45.9%,52.6%,82.0%,67.95%,and 47%,respectively.O_(3)also significantly reduced their production by 99.1%,91.1%,99.5%,100%,and 35%.Intracellular organic matter(IOM)was identified as the primary DBP precursors,producing 2.94 times more DBPs than extracellular organic matter(EOM).The increased DBP formation during chlorination was attributed to IOM leakage and cell membrane damage,which was verified using scanning electron microscopy(SEM).The toxicities of DBPs were evaluated for six disinfection methods,revealing inconsistent *** overall toxicities were assessed using zebrafish embryo *** evaluations indicated that chlorination alone was the least favorable *** addition,the toxicities followed a sequence:Cl_(2)≈O_(3)/Cl_(2)>O_(3)>O_(3)/UV/Cl_(2)>UV>UV/Cl_(2).These findings can serve as a reference for sewage treatment plants in selecting appropriate disinfection methods to manage the COVID-19 epidemic from comprehensive perspective.

关键词： Sewage bacteria Disinfection by-products Toxicity Ozonation UV Chlorination

Eliminating H_(2)O/HF and regulating interphase with bifunctional tolylene-2,4-diisocyanate(TDI)additive for long life Li-ion battery

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Journal of Energy Chemistry 2024年第8期95卷 519-528,I0011页

作者： Xueyi Zeng Xiang Gao Peiqi Zhou Haijia Li Xin He Weizhen Fan Chaojun Fan Tianxiang Yang Zhen Ma Xiaoyang Zhao Junmin Nan School of Chemistry South China Normal UniversityGuangzhou 510006GuangdongChina Guangzhou Tinci Materials Technology Co.Ltd. Guangzhou 510760GuangdongChina School of environmental Engineering and Chemistry Luoyang Institute of Science and TechnologyLuoyang 471023HenanChina School of Geomatic and environmental Engineering Henan Polytechnic InstituteNanyang 473000HenanChina

Lithium-ion batteries(LIBs)featuring a Ni-rich cathode exhibit increased specific capacity,but the establishment of a stable interphase through the implementation of a functional electrolyte strategy remains *** when the battery is operated under high temperature,the trace water present in the electrolyte will accelerate the hydrolysis of the electrolyte and the resulting HF will further erode the *** order to enhance the long-term cycling performance of graphite/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)LIBs,herein,Tolylene-2,4-diisocyanate(TDI)additive containing lone-pair electrons is employed to formulate a novel bifunctional electrolyte aimed at eliminating H_(2)O/HF generated at elevated *** 1000 cycles at 25℃,the battery incorporating the TDI-containing electrolyte exhibits an impressive capacity retention of 94%at 1 *** contrast,the battery utilizing the blank electrolyte has a lower capacity retention of only 78%.Furthermore,after undergoing 550 cycles at 1 C under45℃,the inclusion of TDI results in a notable enhancement of capacity,increasing it from 68%to 80%.This indicates TDI has a favorable influence on the cycling performance of LIBs,especially at elevated *** analysis of the film formation mechanism suggests that the lone pair of electrons of the isocyanate group in TDI play a crucial role in inhibiting the generation of H_(2)O and HF,which leads to the formation of a thin and dense *** existence of this interphase is thought to substantially enhance the cycling performance of the *** work not only improves the performance of graphite/NCM811 batteries at room temperature and high temperature by eliminating H_(2)O/HF but also presents a novel strategy for advancing functional electrolyte development.

关键词： Graphite/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)battery Tolylene-2 4-diisocyanate Long-cycling performance H_(2)O/HF eliminated additive

Advancements in S-scheme heterojunction materials for photocatalytic environmental remediation

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Journal of Materials science & Technology 2024年第2期169卷 182-198页

作者： Changliang Nie Xiaohan Wang Ping Lu Yukun Zhu Xin Li Hua Tang School of environmental science and Engineering State Key Laboratory of Bio-fibers and Eco-textilesQingdao UniversityQingdao266071China institute of Biomass Engineering Key Laboratory of Energy Plants Resource and UtilizationMinistry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou510642China School of environmental science and Engineering Shandong UniversityQingdao266237China

Recently,S-scheme heterojunctions have gained considerable attention in the field of photocatalytic environmental remediation as their potential to achieve efficient spatial charge separation coupled with strong redox ***,this review provides an overview of the current state-of-the-art in the development of S-scheme-based photocatalysts for the purification of environmental *** review first covers the fundamentals of heterogeneous photocatalysis for environmental ***,an introduction to the background,mechanism,design principles,and characterization techniques of S-scheme heterojunctions is ***,the review presents a comparison and summary of using various S-scheme photocatalysts for the removal of several target pollutants,such as bacteria,heavy metals,nitrogen oxides,antibiotics,and ***,the modification strategies of S-scheme heterojunction photocatalysts are also ***,a brief discussion of the challenges and prospects associated with S-scheme photocatalytic systems is demonstrated.

关键词： S-scheme heterojunctions Photocatalyst Pollutant environmental remediation

Unraveling the role of NiSnPH@OOH/CC perovskite hydroxide for efficient electrocatalytic oxidation of methanol to formate

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Nano Research 2024年第4期17卷 2388-2399页

作者： Jing Shao Yusheng Fang Xiaobing Wu Muhammad Imran Abdullah Youkun Tao College of Chemistry and environmental Engineering Shenzhen UniversityShenzhen 518060China School of science Harbin Institute of TechnologyShenzhen 518055China

The sluggish kinetics of oxygen evolution reaction(OER)is the key tailback for hydrogen production from the water *** OER with thermodynamically auspicious methanol oxidation reaction(MOR)can significantly boost the H_(2) and value-added products ***,it is currently challenging to achieve a synergistic manipulation of product selectivity and performance for MOR ***,we report NiSnPH@OOH/CC(CC=carbon cloth)perovskite hydroxide nanosphere as an efficient MOR electrocatalyst with high activity,stability,and selectivity towards methanol oxidation to formate.A surface amorphous layer of defect rich NiOOH was generated in operando by selective Sn leaching with stable perovskite hydroxide bulk structure,which mitigates the oxidative power and optimizes the local coordination environment of the active NiOOH *** situ Raman combined with electrochemical studies further confirm the key active species,NiOOH,generated in operando enhance the MOR and blocking the over oxidation of methanol to CO_(2).As a result,NiSnPH@OOH/CC effectively masks the OER and attains>99%selectivity with 100%Faradic efficiency for *** results of this study show the advances of NiSnPH@OOH/CC as an efficient electrocatalyst for MOR and also suggest its potential applications for various small organic molecules oxidation.

关键词： perovskite hydroxide small organic molecules nickel oxy(hydroxide) value-added products methanol oxidation reaction

Efficient reduction and adsorption of Cr(Ⅵ)using FeCl_(3)-modified biochar:Synergistic roles of persistent free radicals and Fe(Ⅱ)

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Journal of environmental sciences 2024年第3期137卷 626-638页

作者： Shujie Hu Chengshuai Liu Hongling Bu Manjia Chen Ying-heng Fei National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in south china Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and ManagementInstitute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China State Key Laboratory of environmental Geochemistry Institute of GeochemistryChinese Academy of ScienceGuiyang 550081China School of Environment science and Engineering Guangzhou UniversityGuangzhou 510006China College of Resources and Environment Chongqing SchoolUniversity of Chinese Academy of SciencesChongqing 400714China School of environmental science and Engineering Guangdong University of TechnologyGuangzhou 510006China

Transition metal iron and persistent free radicals(PFRs)both affect the redox properties of biochar,but the electron transfer relationship between them and the coupling reduction mechanism of Cr(Ⅵ)requires further *** untangle the interplay between iron and PFRs in biochar and the infuences on redox properties,FeCl_(3)-modified rice husk biochar(FBCs)was prepared and its reduction mechanism for Cr(Ⅵ)without light was *** FBCs had higher surface positive charges,oxygen-containing functional groups,and PFRs compared with pristine rice husk biochar(BC).Phenoxyl PFRs with high electrondonating capability formed in *** pronounced electron paramagnetic resonance signals showed that the PFRs preferred to form at lower Fe(Ⅲ)*** a high concentration of Fe(Ⅲ)would be reduced to Fe(Ⅱ)and consumed the formed *** kinetics and X-ray photoelectron spectroscopy analysis indicated that the FBCs effectively enhanced the Cr(Ⅵ)removal efficiency by 1.54-8.20 fold and the Cr(Ⅵ)reduction efficiency by 1.88-9.29 fold compared to those of *** quenching and competitive reductant addition experiments revealed that the higher Cr(Ⅵ)reduction performance of FBCs was mainly attributed to the formed PFRs,which could contribute to~74.0%of Cr(Ⅵ)reduction by direct or indirect electron *** PFRs on FBCs surfaces could promote the Fe(Ⅲ)/Fe(Ⅱ)cycle through single electron transfer and synergistically accelerate~52.3%of Cr(Ⅵ)*** study provides an improved understanding of the reduction mechanism of iron-modified biochar PFRs on Cr(Ⅵ)in environments.

关键词： Biochar Iron-modification Cr(Ⅵ) Electron transfer Reduction mechanism

Performance and mechanism of CO_(2) absorption during the simultaneous removal of SO_(2) and NO_(x) by wet scrubbing process

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Journal of environmental sciences 2024年第1期135卷 534-545页

作者： Peng Lu Xianhui Yan Lyumeng Ye Dingsheng Chen Dongyao Chen Jianhang Huang Chaoping Cen Guangdong Province Engineering Laboratory for Air Pollution Control South China Institute of Environmental SciencesMinistry of Ecology and EnvironmentGuangzhou 510655China Guangdong Provincial Key Laboratory of Water and Air Pollution Control Guangzhou 510655China School of environmental science and Engineering Sun Yat-sen UniversityGuangzhou 510275China

The co-removal of CO_(2)while removing SO_(2)and NOxfrom industrial flue gas has great potential of carbon emission reduction but related research is *** this study,a wet scrubbing process with various urea solutions for desulfurization and denitrification was explored for the possibility of CO_(2)*** results showed that the urea-additive solutions were efficient for NOxand SO_(2)abatement,but delivered<10%CO_(2)absorption *** addition of Ca(OH)_(2)dramatically enhanced the CO_(2)absorption,remained the desulfurization efficiency,unfortunately restricted the denitrification *** various operating parameters,pH of solution played a determining role during the *** contradictory pH demands of CO_(2)absorption and denitrification were observed and discussed in detail.A higher pH of solution than 10 was favorable for CO_(2)absorption,while the oxidizing of NO to NO_(2),NO_(2)^(-)or NO_(3)^(-)by NaClO_(2)was inhibited in this ***7

关键词： CO_(2)absorption Synergistic desulfurization and denitrification Wet scrubbing process Urea-NaClO_(2)-Ca(OH)_(2)absorbent Carbonation reaction