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Chinese Chemical Letters 2024年第5期35卷 428-433页

作者： Chaozheng he Jia Wang Ling Fu wei wei henan Engineering Center of New Energy Battery Materials College of Chemistry and Chemical EngineeringShangqiu Normal UniversityShangqiu 476000China school of Chemistry and Chemical Engineering Shandong Provincial Key Laboratory/Collaborative Innovation Center of Chemical Energy Storage&Novel Cell TechnologyLiaocheng UniversityLiaocheng 252059China Institute of environment and Energy Catalysis Shaanxi Key Laboratory of Optoelectronic Functional Materials and DevicesSchool of Materials Science and Chemical EngineeringXi’an Technological UniversityXi’an 710021China College of Resources and environmental Engineering Tianshui Normal UniversityTianshui 741001China

Electrocatalytic synthesis of ammonia as an environment-friendly and sustainable development method has received widespread attention in recent ***-dimensional(2D)materials are a promising catalyst for ammonia synthesis due to their large surface *** this work,we have constructed a series of 2D metal borides(MBenes)with transition metal(TM)defects(TMd-MBenes)and comprehensively calculated the reactivity of electrocatalytic synthesis of ammonia-based on density functional *** results have demonstrated that the TMd-MBenes can effectively activate nitrogen oxide(NO)and nitrogen(N2)molecules *** interesting,the co-chemisorption of O atoms,dissociated from NO,can facilitate the spilled of the inert N2 molecules into single N atoms,which can further hydrogenate into ammonia easily with an ultralow limiting potential of 0.59 V on *** research has not only provided clues for catalyst design for experimental study but also paved the way for the industrial application of electrocatalytic ammonia synthesis.

关键词： 2D mbenes Nitrogen electro-reduction DFT N_(2)activation Ammonia synthesis

Comparison of antimony and arsenic behaviour at the river-lake junction in the middle of the Yangtze River Basin

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Journal of environmental Sciences 2024年第2期136卷 189-200页

作者： Huiji Liu wei Zeng Ziyang Lai Mengchang he Chunye Lin wei Ouyang Xitao Liu State Key Laboratory of Water environment Simulation School of EnvironmentBeijing Normal UniversityBeijing 100875China Advanced Interdisciplinary Institute of environment and Ecology Beijing Normal UniversityZhuhai 519087China

As typical metalloid toxic elements widely distributed in environmental media,the geochemical behaviour of antimony(Sb)and arsenic(As)affects environmental *** selected the surface waters and sediments at the river-lake junction of Dongting Lake as the research objects,analysed the concentration and chemical partitioning of Sb and As,assessed its contamination and ecological risk levels,and discussed its sources and potential influencing *** concentrations of dissolved Sb and As in surface waters were low(he concentrations of Sb and As in surface sediments were 2.49-22.65mg/kg and 11.10-136.34 mg/kg,*** and As in sediments were mainly enriched in the fraction of residues,but the proportion of As in bioavailability was significantly higher than that of *** the contamination level of Sb was higher than that of As,the risk assessment code(RAC)showed that the ecological risk level of As was higher than that of *** erosion and mining activities(in the midstream of Zijiang River)were the main contaminated sources of Sb,while As was affect mainly by rainwater *** contamination and ecological risk of Sb in the inlet of the Zijiang River should receive considerable attention,while those of As in the inlet of the Xiangjiang River should also be seriously *** study highlights the need for multi-index-based assessments of contamination and ecological risk and the importance of further studies on the environmental behaviour of metalloids in specific hydrological conditions,such as river-lake junctions.

关键词： Contamination Ecological risks Antimony(Sb) Arsenic(As) River-lake junction Dongting Lake

Scalable graphene foam with ultrahigh conductivity for stabilizing Pt towards efficient hydrogen evolution

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Nano Research 2024年第8期17卷 6968-6976页

作者： Ming Zhao Meng Huang Huihui Jin Dayin he wei Qian Zixin Zhang Daping he State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Hubei Engineering Research Center of RF-Microwave Technology and Application Wuhan University of TechnologyWuhan 430070China school of Information Engineering Wuhan University of TechnologyWuhan 430070China school of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya 572000China

For the carbon-based catalyst to be active and stable,especially in harsh electrochemical environments,the key is to decrease the concentration of defects and raise the degree of graphitization of the carbon ***,we develop a highly graphitized graphene foam with multiplicated structure to fabricate self-supporting Pt-based catalysts for efficient and stable hydrogen evolution reaction(heR)*** foam(GO-2850)is obtained through an ultra-high temperature treatment at 2850℃,with perfect graphene structure and extremely low defect,ensuring high electrical conductivity and corrosion ***,its multiplicated structure provides an inherently favorable environment for the dispersion of Pt nanoparticles(Pt NPs)and offers abundant channels for electrolyte infiltration during the catalytic *** a result,the as-prepared Pt/GO-2850 is far active and stable than the Pt NPs supported on commercial carbon paper(Pt/CP)counterpart toward catalyzing heR,exhibiting an outstanding activity and long-term durability(300 h@10 mA·cm^(−2))in acidic/alkaline/seawater *** can be attributed to the stronger interaction between the lower-defect GO-2850 substrate and Pt,as evidenced by characterization and theoretical *** work extends further insight into the design self-supporting catalysts of high activity and stability with promising prominent application toward green energy devices.

关键词： graphene foam high graphitization Pt nanoparticles hydrogen evolution reaction long-term stability

Photoinduced bismuth vanadate-catalyzed C(sp^(2))-H functionalization

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Chinese Chemical Letters 2024年第3期35卷 1-2页

作者： Rong-Nan Yi wei-Min he Key Laboratory of Food&environment&Drug Monitoring and Testing of Universities in Hunan Province Hunan Police AcademyChangsha 410138China school of Chemistry and Chemical Engineering University of South ChinaHengyang 421001China

Visible light-induced organic reactions have gained much attention in recent years due to their mild conditions and high efficiency[1,2].In this context,many efficient photocatalysts including transition metal complex... 详细信息

关键词： bismuth catalyzed gained

Photocatalytic Minisci-type multicomponent reaction for the synthesis of 1-(halo)alkyl-3-heteroaryl bicyclo[1.1.1]pentanes

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Chinese Chemical Letters 2024年第10期35卷 32-34页

作者： Rong-Nan Yi wei-Min he Key Laboratory of Food & environment & Drug Monitoring and Testing of Universities in Hunan Province Hunan Police Academy school of Chemistry and Chemical Engineering University of South China

Bioisosteres play an important role in pharmaceutical and agri cultural compound design that has been developed to enhance the properties of *** a sp3-rich small ring cage hydro carbons,bicyclo[1.1.1]pentanes （BCPs） were commonly considered as a bioisostere of the para-substituted arenes,internal alkynes and tert–butyl groups,and its introduction can significantly im prove pharmacokinetic properties,including passive permeability aqueous solubility,metabolic stability[1].Over the past decades numerous pharmaceutically relevant molecules with biaryl frame works were improved by the approach of bioisosteric replacement Conventional strategies for the synthesis of such BCP-aryls deriva tives mostly depend on the stepwise C–C formation via the di rect addition to bridgehead C–C bond of[1.1.1]propellane to pro vide active BCP-intermediates and followed by a second transition metal cross-coupling ***,these pioneer works were limited by the low step economy,the use of unstable reagents and harsh conditions in industrial ***,radical mediated one-step,multi-component reactions[2-6]for synthe sizing various BCP-aryl derivatives have made progress,although these strategies were limited to the prefunctionalized （het）arene and tertiary alkyl radicals[7].Therefore,it is of great significance to develop a method for diverse BCP-aryls that can be compatible with primary,secondary,tertiary radicals and direct C–H function alization of （het）arenes.

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Manipulating the Phase Transition Behavior of Dual Temperature-Responsive Block Copolymers by Adjusting Composition and Sequence

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Chinese Journal of Polymer Science 2024年第2期42卷 176-187,I0006页

作者： Zhi Zou Xiang Xu Hai-Tao Zhao Jian-Nan Cheng wei-wei he Li-Fen Zhang Zhen-Ping Cheng Suzhou key Laboratory of Macromolecular Design and Precision Synthesis Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationState and Local Joint Engineering Laboratory for Novel Functional Polymeric MaterialsCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of JiangsuSoochow UniversitySuzhou215123China

Temperature-responsive polymers have garnered significant attention due to their ability to respond to external *** this work,dual temperature-responsive block copolymers are synthesized via reversible addition-fragmentation chain transfer polymerization(RAFT)polymerization utilizing zwitterionic monomer methacryloyl ethyl sulfobetaine(SBMA) and N-isopropyl acrylamide(NIPAAm) as *** thermal responsive behaviors can be easily modulated by incorporating additional hydrophobic monomer benzyl acrylate(BN) or hydrophilic monomer acrylic acid(AA),adjusting concentration or pH,or varying the degree of polymerization of the block chain *** cloud points of the copolymers are determined by UV-Vis spectrophotometry,and these copolymers exhibit both controlled upper and lower critical solu bility temperatures(LCST and UCST) in aqueous *** study analyzes and summarizes the influencing factors of dual temperature responsive block copolymers by exploring the effects of various conditions on the phase transition temperature of temperature-sensitive polymers to explore the relationship between their properties and environment and structure to make them more selective in terms of temperature application range and regulation *** is very interesting that the introduction of poly-acrylic acid(PAA) segments in the middle of di-block copolymer PSBMA_(55)-b-PNIPAAm_(80) to form PSBMA_(55)-b-PAA_(x)-b-PNIPAAm_(80) results in a reversal of temperature-responsive behaviors from 'U'(LCST UCST) type,while the copolymer PSBMA_(55)-b-P(NIPAAm_(80)-co-AA_(x)) *** work provides a clue for tuning the phase transition behavior of polymers for manufacture of extreme smart materials.

关键词： Temperature responsive polymers High critical solubility temperature(UCST) Low critical solubility temperature(LCST) Block copolymers

Responses of runoff to changes in climate and human activities in the Liuhe River Basin, China

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Journal of Arid Land 2024年第8期16卷 1023-1043页

作者： LI Mingqian WANG he DU wei GU Hongbiao ZHOU Fanchao CHI Baoming school of Ecology and environment Institute of Disaster PreventionLangfang 065201China hebei Key Laboratory of Resource and environmental Disaster Mechanism and Risk Monitoring Sanhe 065201China Suzhou Qianxing environmental Engineering Co. Ltd.Suzhou 215000China College of Transportation Engineering Nanjing Tech UniversityNanjing 210000China Tianjin North China Geological Exploration General Institute Tianjin 300000China

Since the 1950s,numerous soil and water conservation measures have been implemented to control severe soil erosion in the Liuhe River Basin(LRB),*** these measures have protected the upstream soil and water ecological environment,they have led to a sharp reduction in the downstream flow and the deterioration of the river ecological ***,it is important to evaluate the impact of soil and water conservation measures on hydrological processes to assess long-term runoff *** the Soil and Water Assessment Tool(SWAT)models and sensitivity analyses based on the Budyko hypothesis,this study quantitatively evaluated the effects of climate change,direct water withdrawal,and soil and water conservation measures on runoff in the LRB during different periods,including different responses to runoff discharge,hydrological regime,and flood *** runoff series were divided into a baseline period(1956-1969)and two altered periods,i.e.,period 1(1970-1999)and period 2(2000-2020).Human activities were the main cause of the decrease in runoff during the altered periods,contributing 86.03%(-29.61 mm),while the contribution of climate change was only 13.70%(-4.70 mm).The impact of climate change manifests as a decrease in flood volume caused by a reduction in precipitation during the flood *** of two flood cases indicated a 66.00%-84.00%reduction in basin runoff capacity due to soil and water conservation measures in the upstream *** and water conservation measures reduced the peak flow and total flood volume in the upstream runoff area by 77.98%and 55.16%,respectively,even with nearly double the *** runoff coefficient in the reservoir area without soil and water conservation measures was 4.0 times that in the conservation *** results contribute to the re-evaluation of soil and water conservation hydrological effects and provide important guidance for water resource planning and water conservation policy formu

关键词： runoff soil and water conservation climate variability flood human activities Liuhe River Basin

Phosphotungstic acid ionic liquid for efficient photocatalytic desulfurization:Synthesis,application and mechanism

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Chinese Journal of Chemical Engineering 2024年第5期69卷 101-111页

作者： Chenchao Hu Suhang Xun Desheng Liu Junjie Zhang Minqiang he wei Jiang Huaming Li Wenshuai Zhu Institute of environmental health and Ecological Security School of Environment and Safety EngineeringJiangsu UniversityZhenjiang 212013China school of Chemistry and Chemical Engineering Institute for Energy ResearchJiangsu UniversityZhenjiang 212013China Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment Suzhou University of Science and TechnologySuzhou 215009China

An efficient mass transfer process is a critical factor for regulating catalytic activity in a photocatalytic desulfurization ***,a phosphotungstic acid(HPW)active center is successfully composited with a quaternary ammonium phosphotungstate-based hexadecyltrimethylammonium chloride ionic liquid(CTAC-HPW)by the ion exchange method for the photocatalytic oxidative desulfurization of dibenzothiophene *** keggin structure of HPW and highly mass transfer performance of organic cations synergistically enhanced the photocatalytic activity towards the effective convertion of dibenzothiophene(DBT)with the excitation of visible *** deep desulfurization(10 mg·kg^(-1))is attained within 30 min,and well stability is demonstrated within 25 ***,the CTAC-HPW photocatalyst projects well selectivity to interference from coexisting compounds such as olefins and aromatic hydrocarbons and universality of dibenzothiophenes,for example,4-methyldibenzothiophene(4-MDBT)and 4,6-dimethyldibenzothiophene(4,6-DMDBT).Ultimately,a possible photocatalytic desulfurization mechanism is proposed according to the Gaschromatography-mass spectrometry(GC-MS),proving that the final product is the corresponding *** trapping experiment and electron spin resonance(ESR)analysis confirmed that h^(+)and,COOH played critical roles in the oxidation *** work offers a practicable strategy for efficiently converting DBT to DBTO_(2) with added value.

关键词： Photocatalytic desulfurization Extraction Ionic liquid CTAC-HPW

Attribution analysis of groundwater level fluctuation in the Xinxiang section of the Lower Yellow River's suspended river after the construction of the Xiaolangdi Reservoir

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Journal of Geographical Sciences 2024年第7期34卷 1348-1370页

作者： LI he PING Jianhua LENG wei MEI Xuemei ZHANG Min LIU Jiaqi school of Water Conservancy and Transportation Zhengzhou UniversityZhengzhou450001China College of Ecology and environment Zhengzhou UniversityZhengzhou450001China Geothermal and Ecological Geology Research Center Zhengzhou UniversityZhengzhou450001China Institute of Geology and Geophysics CASBeijing100101China

The clear identification and quantification of the factors affecting groundwater systems is crucial for protecting groundwater resources and ensuring safety in agricultural *** Lower Yellow River(LYR)is a suspended river that replenishes groundwater continuously due to clear differences in the water head,especially in the Xinxiang *** its construction,the Xiaolangdi Reservoir has reversed the LYR’s *** accurately determine the factors influencing the groundwater level(GWL),the study area was divided into five subzones based on hydrogeology.A dynamic factor model(DFM),variational mode decomposition(VMD),and a multiple linear regression model were used to identify and quantify the factors influencing the *** impact of the suspended river on the groundwater before and after the construction of the Xiaolangdi Reservoir was *** results show that:(1)The rate of decrease in the GWL was 8.53×10^(–4)m/month,and the rate of decrease in the Yellow River water level(RWL)was 4.63×10^(–4)m/month.(2)Mountain front recharge(MFR)(scale=3 months)and precipitation(scale=9 months)were the dominant factors in subzones I and II,accounting for more than 40%of the fluctuation in the *** III was dominated by exploitation(scale=7 months)and precipitation(scale=12months),accounting for 28.43%,and 23.44%of changes in the GWL,*** subzone IV,agricultural irrigation(scale=12 months)was the major factor,accounting for32.47%of GWL changes,while in subzone V,the RWL(scale=12 months)accounted for52.52%of these changes.(3)The Xiaolangdi Reservoir has increased the lateral seepage of the suspended river and altered the inter-annual *** results of this study can provide a valuable reference for controlling groundwater overexploitation and ensuring water supply security.

关键词： groundwater level influencing factor dynamic factor analysis Xiaolangdi Reservoir Lower Yellow River lateral seepage of the Yellow River