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Revealing the role of electrode potential micro-environments in single Mn atoms for carbon dioxide and oxygen electrolysis

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Nano Research 2024年第9期17卷 7957-7966页

作者： Pengcheng Liu anyi Liu Kaili Wang Shuai Shi Mengmeng Jin Jingxiu Liu Tao Qin Qian Liu Xijun Liu Jia He Tianjin Key Laboratory of Organic Solar Cells and Photochemical Conversion School of Chemistry and Chemical EngineeringInstitute of New-Energy Materials and Low-Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China School of Chemistry and Chemical Engineering and Environmental Engineering Weifang UniversityWeifang 261061China Department of Electrical Engineering and Automation Luoyang Institute of Science and TechnologyLuoyang 471023China institute for advanced study Chengdu UniversityChengdu 610106China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured MaterialsSchool of ResourcesEnvironment and MaterialsGuangxi UniversityNanning 530004China

Elucidation the relationship between electrode potentials and heterogeneous electrocatalytic reactions has attracted widespread *** we construct the well-defined Mn single-atom(MnSA)catalyst with four N-coordination through a simple thermal pyrolysis preparation method to investigate the electrode potential micro-environments effect on carbon dioxide reduction reactions(CO_(2)RR)and oxygen reduction reactions(ORR).MnSA catalysts generate higher CO production Faradaic efficiency of exceeding 90%at-0.9 V for CO_(2)RR and higher H_(2)O_(2)yield from 0.1 to 0.6 V with excellent ORR *** functional theory(DFT)calculations based on constant potential models were performed to study the mechanism of MnSA on CO_(2)*** thermodynamic energy barrier of CO_(2)RR is lowest at-0.9 V *** hydrogen electrode(RHE).Similar DFT calculations on the H_(2)O_(2)yield of ORR showed that the H_(2)O_(2)yield at 0.2 V was *** study provides a reasonable explanation for the role of electrode potential micro-environments.

关键词： electrode potential micro-environments Mn single-atom catalyst carbon dioxide reduction reaction oxygen reduction reaction constant potential models

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Response of ocean acidification to atmospheric carbon dioxide removal

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Journal of Environmental Sciences 2024年第6期140卷 79-90页

作者： Jiu Jiang Long Cao Xiaoyu Jin Zechen Yu Han Zhang Jianjie Fu Guibin Jiang School of Environment Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Key Laboratory of Geoscience Big Data and Deep resources of Zhejiang Province School of Earth SciencesZhejiang UniversityHangzhou 310058China Zhejiang Climate Center Hangzhou 310052China

Artificial CO_(2)removal from the atmosphere(also referred to as negative CO_(2)emissions)has been proposed as a potential means to counteract anthropogenic climate *** we use an Earth system model to examine the response of ocean acidification to idealized atmospheric CO_(2)removal *** our simulations,atmospheric CO_(2)is assumed to increase at a rate of 1%per year to four times its pre-industrial value and then decreases to the pre-industrial level at a rate of 0.5%,1%,2%per year,*** results show that the annual mean state of surface ocean carbonate chemistry fields including hydrogen ion concentration([H^(+)]),pH and aragonite saturation state respond quickly to removal of atmospheric CO_(2).However,the change of seasonal cycle in carbonate chemistry lags behind the decline in atmospheric CO_(2).When CO_(2)returns to the pre-industrial level,over some parts of the ocean,relative to the pre-industrial state,the seasonal amplitude of carbonate chemistry fields is substantially *** results also show that changes in deep ocean carbonate chemistry substantially lag behind atmospheric CO_(2)*** CO_(2)returns to its pre-industrial value,the whole-ocean acidity measured by[H^(+)]is 15%-18%larger than the pre-industrial level,depending on the rate of CO_(2)*** study demonstrates that even if atmospheric CO_(2)can be lowered in the future as a result of net negative CO_(2)emissions,the recovery of some aspects of ocean acidification would take decades to centuries,which would have important implications for the resilience of marine ecosystems.

关键词： Carbon dioxide removal Net negative CO_(2)emission Ocean acidification Climate change Earth system modeling

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Ordered mesoporous materials for water pollution treatment: Adsorption and catalysis

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Green Energy & Environment 2024年第8期9卷 1239-1256页

作者： Peng Zhang Mingming He Wei Teng Fukuan Li Xinyuan Qiu Kexun Li Hao Wang College of Environmental Science and Engineering MOE Key Laboratory of Pollution Processes and Environmental CriteriaTianjin Key Laboratory of Environmental Remediation and Pollution TreatmentTianjin Key Laboratory of Environmental Technology for Complex Trans-Media PollutionNankai University Department of Chemistry and State Key Laboratory Marine Pollution Hong Kong institute for advanced study City University of Hong Kong State Key Laboratory for Pollution Treatment College of Environmental Science and EngineeringShanghai Institute of Pollution Treatment and Ecological SecurityTongji University State Key Laboratory of Simulation and Regulation of Water Cycles in River Basins China Institute of Water Resources and Hydropower Research

To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is *** mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore *** properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and *** this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals (Hg2+,Pb2+,Cd2+,Cr6+,etc.),toxic anions （nitrate,phosphate,fluoride,etc.）,and organic contaminants （organic dyes,antibiotics,etc.）.These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active ***,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are *** work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.

关键词： Water pollution treatment Ordered mesoporous materials Toxic contaminants Adsorption Catalysis

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Carbene-Catalyzed Asymmetric Ring-Opening Reaction of Biaryl Lactams to Access Axially Chiral Biaryls

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Chinese Journal of Chemistry 2024年第15期42卷 1734-1740页

作者： Guanjie Wang Guowei Yuan Chenlong Wei Ye Zhang Haibin Zhu Weiqi Yang Dongping Shi Xiaoxiang Zhang Zhenqian Fu institute of advanced Materials Nanjing Tech UniversityNanjingJiangsu 211816China Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest resources College of Chemical EngineeringNanjing Forestry UniversityNanjingJiangsu 210037China

Axially chiral biaryls represent the most important class of atropisomers,and they widely exist in natural products and biologically active *** also constitute a unique scaffold for chiral ligands and catalysts in organic *** development of synthetic methods to obtain such chiral compounds has received widespread attention,among which catalytically atroposelective ring-opening of configurationally labile compounds represents one of the most attractive *** substrates with strained cyclic structures,such as the renowned Bringmann's lactones,can undergo asymmetric transformation into stable *** advancement primarily relies on metal catalyst combined with well-designed chiral ligands,the approaches utilizing organocatalysis as a critical resolution strategy are notably *** this study,we disclosed a N-heterocyclic carbene(NHC)-catalyzed asymmetric ring-opening reaction of biaryl lactams via direct atroposelective nucleophilic *** optimized bulky carbene catalyst ensures that the reaction can proceed under mild conditions,affording the desired product with good to excellent yields and atroposelectivity.

关键词： N-Heterocyclic carbene Axially chiral biaryls Organocatalysis Ring-opening reactions Dibenzo cyclic lactams Axially chiral amino acids Amide C-N bond activation Atropisomerism Asymmetric catalysis Lactams

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Gravity Wave Activity and Stratosphere-Troposphere Exchange During Typhoon Molave(2020)

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Journal of Tropical Meteorology 2024年第3期30卷 306-326页

作者： HUANG Dong WAN Ling-feng WAN Yi-shun CHANG Shu-jie MA Xin ZHAO Kai-jing College of Ocean and Meteorology/South China Sea institute of Marine Meteorology/Laboratory for Coastal Ocean Variation and Disaster Prediction/Key Laboratory of Climate Resources and Environment in Continental Shelf Sea and Deep Sea(LCRE)/Key Laboratory of Space Ocean Remote Sensing and ApplicationMinistry of Natural ResourcesGuangdong Ocean UniversityZhanjiangGuangdong 524088 China Frontier Science Center for Deep Ocean Multispheres and Earth System(DOMES) Institute for Advanced Ocean Study(IAOS)Ocean University of ChinaQingdaoShandong 266100 China School of Earth and Environment University of LeedsLeeds LS29JT UK Shanghai Astronomical Observatory Chinese Academy of SciencesShanghai 200030 China

To investigate the stratosphere-troposphere exchange(STE)process induced by the gravity waves(GWs)caused by Typhoon Molave(2020)in the upper troposphere and lower stratosphere,we analyzed the ERA5 reanalysis data provided by the European Centre for Medium-Range Weather Forecasts and the CMA Tropical Cyclone Best Track *** also adopted the mesoscale forecast model Weather Research and Forecasting model V4.3 for numerical *** of the previous studies were about typhoon-induced STE and typhoon-induced GWs,while our research focused on the STE caused by typhoon-induced gravity *** analysis shows that most of the time,the gravity wave signal of Typhoon Molave appeared below the *** was stronger on the east side of the typhoon center(10°-20°N,110°-120°E)than on the west side,suggesting an eastward tilted structure with height *** the GWs in the upper troposphere and lower stratosphere region on the west side of the typhoon center broke up,it produced strong turbulence,resulting in stratosphere-troposphere *** this time,the average potential vorticity vertical flux increased with the average ozone mass mixing *** gravity wave events and STE process simulated by the WRF model were basically consistent with the results of ERA5 reanalysis data,but the time of gravity wave breaking was *** study indicates that after the breaking of the GWs induced by typhoons,turbulent mixing will also be generated,and thus the STE.

关键词： gravity wave typhoon stratosphere-troposphere exchange STE upper troposphere and lower stratosphere UTLS

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First-principles study on the heterogeneous formation of environmentally persistent free radicals(EPFRs)overα-Fe2O3(0001)surface:Effect of oxygen vacancy

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Journal of Environmental Sciences 2024年第8期142卷 279-289页

作者： Wenxiao Pan Shuming He Qiao Xue Xian Liu Jianjie Fu Kang Xiao Aiqian Zhang State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China School of Environment Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310012China College of resources and Environment University of Chinese Academy of SciencesBeijing 100049China Beijing Yanshan Earth Critical Zone National Research Station University of Chinese Academy of SciencesBeijing 101408China

Metal oxides with oxygen vacancies have a significant impact on catalytic activity for the transformation of organic pollutants in waste-to-energy(WtE)incineration *** study aims to investigate the influence of hematite surface oxygen point defects on the formation of environmentally persistent free radicals(EPFRs)from phenolic compounds based on the first-principles *** oxygen-deficient conditions were considered:oxygen vacancies at the top surface and on the *** simulations indicate that the adsorption strength of phenol on theα-Fe_(2)O_(3)(0001)surface is enhanced by the presence of oxygen ***,the presence of oxygen vacancies has a negative impact on the dissociation of the phenol molecule,particularly for the surface with a defective point at the top ***-kinetic parameters were established over a temperature range of300-1000 K,and lower reaction rate constants were observed for the scission of phenolic O-H bonds over the oxygen-deficient surfaces compared to the pristine *** negative effects caused by the oxygen-deficient conditions could be attributed to the local reduction of FeⅢto FeⅡ,which lower the oxidizing ability of surface reaction *** findings of this study provide us a promising approach to regulate the formation of EPFRs.

关键词： EPFR formation Phenol dissociation Oxygen-vacancy impact Hematite surface First-principles calculation

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Selective leaching of lithium from spent lithium-ion batteries using sulfuric acid and oxalic acid

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International Journal of Minerals,Metallurgy and Materials 2024年第4期31卷 688-696页

作者： Haijun Yu Dongxing Wang Shuai Rao Lijuan Duan Cairu Shao Xiaohui Tu Zhiyuan Ma Hongyang Cao Zhiqiang Liu institute of advanced Wear&Corrosion Resistant and Functional Materials Jinan UniversityGuangzhou 510632China institute of resources Utilization and Rare Earth Development Guangdong Academy of SciencesGuangzhou 510650China State Key Laboratory of Separation and Comprehensive Utilization of Rare Metals Guangzhou 510650China Guangdong Province Key Laboratory of Rare Earth Development and Application Guangzhou 510650China

Traditional hydrometallurgical methods for recovering spent lithium-ion batteries(LIBs)involve acid leaching to simultaneously extract all valuable metals into the *** methods usually are followed by a series of separation steps such as precipitation,extraction,and stripping to separate the individual valuable *** this study,we present a process for selectively leaching lithium through the synergistic effect of sulfuric and oxalic *** optimal leaching conditions(leaching time of 1.5 h,leaching temperature of 70°C,liquid-solid ratio of 4 mL/g,oxalic acid ratio of 1.3,and sulfuric acid ratio of 1.3),the lithium leaching efficiency reached89.6%,and the leaching efficiencies of Ni,Co,and Mn were 12.8%,6.5%,and 21.7%.X-ray diffraction(XRD)and inductively coupled plasma optical emission spectrometer(ICP-OES)analyses showed that most of the Ni,Co,and Mn in the raw material remained as solid residue oxides and *** study offers a new approach to enriching the relevant theory for selectively recovering lithium from spent LIBs.

关键词： selective leaching oxalic acid sulfuric acid spent lithium-ion batteries

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Assembly of a core–shell MOF with stability into polyacrylamide hydrogel for boosting extraction of uranium from seawater

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Nano Research 2024年第4期17卷 3398-3406页

作者： Yucheng Song Huanhuan Tan Shiliang Qin Zhong Liu Chuntai Liu Changyu Shen Peipei Yang Songwei Li National Engineering Research Center for advanced Polymer Processing Technology Key Laboratory of Materials Processing and Mold(Ministry of Education)Zhengzhou UniversityZhengzhou 450002China Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake resources Qinghai Provincial Key Laboratory of Resources and Chemistry of Salt LakesQinghai Institute of Salt LakesChinese Academy of SciencesXining 810008China

Efficient and selective extraction of uranium(U(VI))from seawater is essential for sustainable nuclear power *** study reports a novel adsorbent zeolitic imidazolate framework(ZIF)-67@SiO_(2)-A/polyacrylamide(PAM)which was synthesized by grafting the core–shell metal–organic frameworks(MOFs)-based nanostructures coated with the 3-aminopropyl triethoxysilane(APTES)functionalized SiO_(2)(SiO_(2)-A)onto PAM *** SiO_(2) shell was grown on the surface of MOF,which improved the acid-base resistance of *** introduction of ZIF-67@SiO_(2)-A enhances the specific surface area and adsorption efficiency of the *** ZIF-67@SiO_(2)-A/PAM shows remarkable adsorption capacity,fast adsorption kinetics,and good reusability for *** has excellent adsorption property(6.33 mg·g^(-1),30 d)in natural *** X-ray photoelectron spectroscopy(XPS),Fourier transform infrared(FTIR),energy dispersive spectroscopy(EDS)mappings,and density functional theory reveal that the coordination by N and O in ZIF-67@SiO_(2)-A/PAM with uranium is the main mechanism of uranium ***,ZIF-67@SiO_(2)-A/PAM has great potential to capture uranium from natural seawater.

关键词： hydrogel metal–organic frameworks core–shelled nanostructures uranium extraction from seawater

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Environmental Obesogens and Their Perturbations in Lipid Metabolism

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Environment & Health 2024年第5期2卷 253-268页

作者： Xiaoyun Wang Zhendong Sun Qian S.Liu Qunfang Zhou Guibin Jiang State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China College of resources and Environment University of Chinese Academy of SciencesBeijing 100049China School of Environment Hangzhou Institute for Advanced StudyUCASHangzhou 310024China

Epidemiological data show that obesity is now a *** homeostasis requires the coordination of multiple tissues and organs,including the liver,kidney,cardiovascular system,and adipose tissues,to maintain bodily *** increasing amounts of chemicals are being synthesized,applied,and released into the environment,their obesogenic effects have triggered serious ***,more than 50 types of chemicals with high human exposure levels have been identified as environmental obesogens that can interfere with lipid metabolism and induce *** studies have shown that the lipid metabolism interference effects of obesogens have multiple targets,including nuclear receptors,transcription factors,cytokines,and *** interfering factors of environmental obesogeninduced obesity include transgenerational effects,susceptibility windows,gender differences,structure−effect relationships,and diet *** research approaches have been established to conduct obesogenic effect *** comprehensive review summarizes the mechanisms underlying obesogen actions and the research progress on obesogen-disrupted lipid metabolism,along with the influencing factors and research approaches,aiming to provide a framework for understanding the effects of environmental obesogens on lipid metabolism.

关键词： environmental obesogens lipid metabolism risk assessment influencing factors research approaches

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Layer-by-layer fabrication of montmorillonite coating immobilizing Cu_(2)O nanoparticles for continuously catalyzing glycerol to dihydroxyacetone

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Chinese Journal of Chemical Engineering 2024年第4期68卷 263-275页

作者： Kejin Li Jiahui Liu Dajian Li Xiaolan Chen Chunhui Zhou Research Group for advanced Materials&Sustainable Catalysis(AMSC) State Key Laboratory Breeding Base of Green Chemistry-Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310032China Qing Yang institute for Industrial Minerals Qingyang 242804China Engineering Research Center of Non-metallic Minerals of Zhejiang Province Zhejiang Institute of Geology and Mineral ResourcesHangzhou 310007China

Microreactors are increasingly used for green and safe chemical processes owing to their benefits of superior mass and heat transfer,increased yield,safety,and simplicity of ***,immobilizing catalysts in microreactors remains *** this investigation,a technique for creating Cu_(2)O/montmorillonite catalyst coating,using electrostatic attraction for layer-by-layer self-assembly,was *** montmorillonite film's morphology and thickness could be efficiently regulated by adjusting the degree of exfoliation and surface charge of montmorillonite,alongside layer-by-layer coating *** Cu_(2)O nanoparticles were immobilized using the flow deposition *** resulting Cu_(2)O@montmorillonite-film-coated capillary microreactor successfully transformed glycerol into *** conversion of glycerol and product selectivity could be controlled by adjusting the molar ratio of reactants,temperature,residence time,and Cu_(2)O *** maximum glycerol conversion observed was 47.6%,with a 27%selectivity toward *** study presents a technique for immobilizing montmorillonite-based catalyst coatings in capillary tubing,which can serve as a foundation for the future application of microreactors in glycerol conversion.

关键词： Microreactor Coating Montmorillonite Glycerol Cu_(2)O

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