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Nano Research 2024年第4期17卷 2438-2443页

作者： Ran Li Taotao Gao Wenxi Qiu Minghao xie Zhaoyu Jin Panpan Li College of Materials Science and Engineering Sichuan UniversityChengdu 610065China Institute for Advanced Study Chengdu UniversityChengdu 610106China Materials Science and Engineering Program and Walker Department of Mechanical Engineering The University of Texas at AustinAustinTexas 78712USA Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China

The electrocatalytic nitrate reduction reaction(NitRR)represents a promising approach toward achieving economically and environmentally sustainable ***,it remains a challenge to regulate the size effect of electrocatalysts to optimize the catalytic activity and ammonia ***,the Cu-based catalysts were tailored at the atomic level to exhibit a size gradient ranging from single-atom catalysts(SACs,0.15–0.35 nm)to single-cluster catalysts(SCCs,1.0–2.8 nm)and nanoparticles(NPs,20–30 nm),with the aim of studying the size effect for the NO_(3)^(-)-to-Nh_(3) reduction ***,the Cu SCCs exhibit enhanced metal–substrate and metal–metal interactions by taking advantageous features of Cu SACs and Cu ***,Cu SCCs achieve exceptional electrocatalytic performance for the NitRR with a maximum Faradaic efficiency of ca.96%Nh_(3)and the largest yield rate of ca.1.99 mg·h^(-1)·cm^(-2) at-0.5 V *** hydrogen electrode(RhE).The theoretical calculation further reveals the size effect and coordination environment on the high catalytic activity and selectivity for the *** work provides a promising various size-controlled design strategy for aerogel-based catalysts effectively applied in various electrocatalytic reactions.

关键词： nitrate electroreduction ammonia electrosynthesis size effect single-cluster catalyst

Insight into the Role and Evidence of Oxygen Vacancies in Porous Single-Crystalline Oxide to Enhance Catalytic Activity and Durability

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Research 2024年第2期2023卷 675-683页

作者： Lingting Ye Jiaming Ma Jie Zhang Wen Yin Yuanguang Xia Kui xie Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujan Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China FuzhouFujian 350108China Advanced Energy Science and Technology Guangdong Laboratory 29 Sanxin North RoadHuizhouGuangdong 116023China Spallation Neutron Source Science Center DongguanGuangdong 523803China

Introducing and stabilizing oxygen vacancies in oxide catalysts is considered to be a promising strategy for improving catalytic activity and ***,we quantitatively create oxygen vacancies in the lattice of porous single-crystallineβ-Ga_(2)O_(3)monoliths by reduction treatments and stabilize them through the long-range ordering of crystal lattice to enhance catalytic activity and *** combination analysis of time-of-flight neutron powder diffraction and extended x-ray absorption fine structure discloses that the preferential generation of oxygen vacancy tends to occur at the site of tetrahedral coordination oxygen ions(O_(Ⅲ)sites),which contributes to the formation of unsaturated Ga-O coordination in the monoclinic *** oxygen vacancies are randomly distributed in lattice even though some of them are present in the form of domain defect in the PSC Ga_(2)O_(3)monoliths after the reduction *** number of oxygen vacancies in the reduced monoliths gives 2.32×10^(13),2.87×10^(13),and 3.45×10^(13)mg^(-1)for the Ga_(2)O_(2.952),Ga_(2)O_(2.895),and Ga_(2)O_(2.880),*** therefore demonstrate the exceptionally high C_(2)h_(4)selectivity of~100%at the C_(2)h_(6)conversion of~37%for nonoxidative dehydrogenation of C_(2)h_(6)to C_(2)h_(4).We further demonstrate the excellent durability even at 620℃for 240 h of continuous operation.

关键词： durability coordination Oxygen

Internal Polarization Field Induced hydroxyl Spillover Effect for Industrial Water Splitting Electrolyzers

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Nano-Micro Letters 2024年第2期16卷 438-449页

作者： Jingyi xie Fuli Wang Yanan Zhou Yiwen Dong Yongming Chai Bin Dong State Key Laboratory of heavy Oil Processing College of Chemistry and Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580People’s Republic of China

The formation of multiple oxygen intermediates supporting efficient oxygen evolution reaction(OER)are affinitive with hydroxyl ***,ability of the catalyst to capture hydroxyl and maintain the continuous supply at active sits remains a tremendous ***,an affordable Ni2P/FeP2 heterostructure is presented to form the internal polarization field(IPF),arising hydroxyl spillover(hOSo)during *** by IPF,the oriented hOSo from FeP2 to Ni2P can activate the Ni site with a new hydroxyl transmission channel and build the optimized reaction path of oxygen intermediates for lower adsorption energy,boosting the OER activity(242 mV *** at 100 mA cm-2)for least 100 *** interestingly,for the anion exchange membrane water electrolyzer(AEMWE)with low concentration electrolyte,the advantage of hOSo effect is significantly amplified,delivering 1 A cm^(-2)at a low cell voltage of 1.88 V with excellent stability for over 50 h.

关键词： hydroxyl spillover effect Internal polarization field heterostructure Oxygen reduction reaction Anion exchange membrane water electrolysis

Asymmetric copolyimide membranes fabricated by nonsolvent-induced phase separation for he/Ch_(4) and he/N_(2) separation

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Frontiers of Chemical Science and Engineering 2024年第4期18卷 97-106页

作者： Ying Li Lu Wang Junyan xie Yong Dai Xuehong Gu Xuerui Wang State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China Quzhou Membrane Material Innovation Institute Quzhou 324000China

Membrane gas separation is considered an energy-saving technique to extract he from natural gas due to no phase change and room temperature ***,the membrane performance was strongly limited by the trade-off between permeance and ***,novel 4,4′-(hexafluoroisopropylidene)diphthalic anhydride(6FDA)-2,2′-bis(3-amino-4-hydroxyphenyl)hexafluoropropane(APAF)-5-amino-2-(4-aminobenzene)benzimidazole(BIA)asymmetric membranes with a thickness of 300 nm were successfully prepared by the non-solvent induced phase separation *** membrane performance was modulated by regulating dope solution compositions(e.g.,tetrahydrofuran and polymer concentration).The ideal he/Ch_(4) selectivity was 124 and the optimized he permeance reached 87 GPU,beyond the current upper ***/Ch_(4) selectivity was 75 and he permeance was 73 GPU for the binary mixture feed containing 0.2 mol%*** membrane showed good resistance to CO_(2) and C_(2)h_(6),which are the typical impurities in natural *** 6FDA-APAF-BIA membranes have good stability(>160 h),which can provide great potential in he extraction from natural gas.

关键词： he separation membrane natural gas copolyimide

Oxygen and hydrogen isotope characteristics of different water bodies in the Burqin River Basin of the Altay Mountains,China

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Journal of Arid Land 2024年第10期16卷 1365-1379页

作者： xie Yida WANG Feiteng LIU Shuangshuang Key Laboratory of Cryospheric Science and Frozen Soil Engineering Northwest Institute of Eco-Environment and ResourcesChinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China

Characterization of the spatial and temporal variability of stable isotopes in surface water is essential for interpreting hydrological *** this study,we collected the water samples of river water,groundwater,and reservoir water in the Burqin River Basin of the Altay Mountains,China in 2021,and characterized the oxygen and hydrogen isotope variations in different water bodies via instrumental analytics and *** showed significant seasonal variations in stable isotope ratios of oxygen and hydrogen(δ18O andδ2h,respectively)and significant differences inδ18O andδ2h among different water ***δ18O andδ2h values were mainly found in river water,while groundwater and reservoir water had lower isotope *** water and groundwater showed differentδ18O-δ2h relationships with the local meteoric water line,implying that river water and groundwater are controlled by evaporative enrichment and multi-source recharge *** evaporative enrichment experienced by reservoir water was less significant and largely influenced by topography,recharge sources,local moisture cycling,and anthropogenic *** deuterium excess(d-excess)value of 14.34‰for river water probably represented the isotopic signature of combined contributions from direct precipitation,snow and glacial meltwater,and groundwater *** average annual d-excess values of groundwater(10.60‰)and reservoir water(11.49‰)were similar to the value of global precipitation(10.00‰).The findings contribute to understanding the hydroclimatic information reflected in the month-by-month variations in stable isotopes in different water bodies and provide a reference for the study of hydrological processes and climate change in the Altay Mountains,China.

关键词： water bodies stable isotopes deuterium excess(d-excess) hybrid Single-Particle Lagrangian Integrated Trajectory(hYSPLIT)model Burqin River Basin Altay Mountains

Construction of 2D/2D Ti_(3)C_(2)T_(x)MXene/CdS heterojunction with photothermal effect for efficient photocatalytic hydrogen production

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Journal of Materials Science & Technology 2024年第4期171卷 1-9页

作者： T.Y.huang Z.Yang S.Y.Yang Z.h.Dai Y.J.Liu J.h.Liao G.Y.Zhong Z.J.xie Y.P.Fang S.S.Zhang Key Laboratory for Biobased Materials and Energy of Ministry of Education Guangdong Laboratory for Lingnan Modern AgricultureCollege of Materials and EnergySouth China Agricultural UniversityGuangzhou 510643China School of Physics and Optoelectronics South China University of TechnologyGuangzhou 510640China School of Chemical Engineering and Energy Technology Guangdong Provincial Key Laboratory of Distributed Energy SystemsDongguan University of TechnologyDongguan 523808China

The insensitivity of semiconductors to visible and infrared light is a key constraint on the utilization of light energy in photocatalytic *** photocatalysts with full-spectrum absorption through surface engineering is an effective approach to fully harnessing light energy in semiconductor ***,a novel stable Ti_(3)C_(2)T_(x)MXene/CdS heterojunction catalyst is obtained by in-situ epitaxial growth of two-dimensional(2D)CdS nanosheets on 2D MXene interface via a solvothermal *** exceptional light absorption properties of MXene confer outstanding full-spectrum driven photocat-alytic hydrogen evolution capability upon the heterogeneous *** unique 2D/2D structure effectively mitigated the recombination of photogenerated carriers,enhancing the photocatalytic performance of the ***,the composite catalyst exhibits a significantly higher surface temperature of 80.4℃under visible light irradiation at an intensity of 0.1 W/cm^(2),which is 1.84 times higher than that of *** irradiation of visible and near infrared light,the composite catalyst with photothermal ef-fect demonstrates a remarkable hydrogen evolution rate of 65.4 mmol g^(-1)h^(-1),which is 7.2 times higher than that of CdS *** study introduces a novel approach for constructing full-spectrum absorption catalysts and expands the application of the photothermal effect in photocatalytic hydrogen evolution research.

关键词： Two-dimensional structure heterostructure Photothermal effect Photocatalyst hydrogen evolution

Porous S-doped carbon nitride foam with accelerated charge dynamics for synchronous photocatalytic hydrogen production and highly selective oxidation of amines

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Nano Research 2024年第8期17卷 6860-6869页

作者： Yu he Aiping Wu Nan Wang Ying xie Chungui Tian honggang Fu Key Laboratory of Functional Inorganic Material Chemistry(Ministry of Education of the People’s Republic of China) Heilongjiang UniversityHarbin 150080China

Photocatalytic hydrogen evolution coupled with organic oxidation holds great promise for converting solar energy into high-valueadded chemicals,but it is hampered by sluggish charge dynamics and limited redox ***,a porous S-doped carbon nitride(S-C_(3)N_(4−y))foam assembled from ultrathin nanosheets with rich nitrogen vacancies was synthesized using a molecular selfassembly *** S dopants and N vacancies synergistically adjusted the band structure,facilitating light absorption and enhancing the oxidation ***,the ultrathin nanosheets and porous structure provided more exposed active sites and facilitated mass and charge ***,S-C_(3)N_(4−y) foam exhibited enhanced photocatalytic activities for synchronous hydrogen evolution(4960μmol/(h·g))and benzylamine oxidation to N-benzylidenebenzylamine(4885μmol/(h·g))with high selectivity of>99%,which were approximately 17.6 and 72.9 times higher than those of bulk CN,*** photocatalytic coupling pairing reaction promotes the water splitting by consuming h2O2,thereby improving the hydrogen evolution efficiency and achieving the production of high value-added *** study provides an effective route for regulating the morphology and band structure of carbon nitride for synthesizing highly valuable chemicals.

关键词： photocatalysis S-doped carbon nitride band structure regulation hydrogen evolution coupled with benzylamine oxidation reaction mechanism

Temporal and environmental factors drive community structure and function of methanotrophs in volcanic forest soils

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Journal of Forestry Research 2024年第2期35卷 1-13页

作者： Rusong Chai hongjie Cao Qingyang huang Lihong xie Fan Yang hongbin Yin heilongjiang Forest Botanical Garden Harbin 150040People’s Republic of China 2 Institute of Natural Resources and Ecology Science Academy of Heilongjiang ProvinceHarbin 150040People’s Republic of China

Methanotrophs,organisms that obtain oxygen by oxidizing methane,are recognized as the only known biological sink for atmospheric Ch_4,and forest soil methanotrophs play crucial roles in mitigating global *** succession patterns of methanotrophic communities and functions in Wudalianchi volcano forest soils could provide a basis for the study of evolutionary mechanisms between soil microorganisms,the environment,and carbon cycling of temperate forest ecosystems under climate *** this study,the characteristics and drivers of methanotrophic community structure and function of two volcanic soils at different stages of development are analyzed,including an old volcano and a new volcano,which most recently erupted 300 years and 17-19×10^(5)years ago,respectively,and a non-volcano hills as control,based on space for time substitution and Miseq sequencing and bioinformation *** results showed that Ch_(4) fluxes were significantly higher in old-stage volcano forest soils than new-stage forest soils and non-volcano forest *** were significant differences in the community composition and diversity of soil methanotrophs from different volcano forest *** was the dominant genus in all soil ***,the relative abundance of Methylococcus,along with Clonothrix,Methyloglobulus,Methylomagum,Methylomonas and Methylosarcina,were the important genera responsible for the differences in methanotrophic community structure in different volcano forest *** relative abundance of methanotroph belonging toγ-proteobacteria was significantly higher than that belonging toα-proteobacteria(Phao1,Shannon and Simpson indices of soil methanotrophic community were significantly lower in new-stage volcanos and were significantly affected by bulk density,total porosity,p h,nitrate,dissolved organic carbon and dissolved organic *** were significant differences in community structure between new-stage and old-stage volcano

关键词： Methanotrophs pmo A Soil development stage Volcanoes Forest soils

Factors hindering the degradation of pharmaceuticals from human urine in an iron-activated persulfate system

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Journal of Environmental Sciences 2024年第1期135卷 130-148页

作者： Yiruiwen xie Dao Guan Yangfan Deng Yugo Sato Yu Luo Guanghao Chen Department of Civil and Environmental Engineering Water Technology LabHong Kong Branch of Chinese National Engineering Research Center for Control&Treatment of Heavy Metal PollutionThe Hong Kong University of Science&TechnologyHong Kong 999077China

This study investigated the degradation of clofibric acid(CFA),bezafibrate(BZF),and sulfamethoxazole(SMX)in synthetic human urine using a novel mesoporous iron powderactivated persulfate system(mFe-PS system),and identified the factors limiting their degradation in synthetic human urine.A kinetic model was established to expose the radical production in various reaction conditions,and experiments were conducted to verify the modeling *** the phosphate-containing mFe-PS system,the 120 min removal efficiency of CFA decreased from 95.1%to 76.6%as the phosphate concentration increased from 0.32 to 6.45 mmol/L,but recovered to 90.5%when phosphate concentration increased to 16.10 mmol/***,the increased concentration of phosphate from 0.32 to 16.10mmol/L reduced the BZF degradation efficacy from 91.5%to 79.0%,whereas SMX removal improved from 37.3%to 62.9%.The m Fe-PS system containing(bi)carbonate,from 4.20 to166.70 mmol/L,reduced CFA and BZF removal efficiencies from 100%to 76.8%and 80.4%,respectively,and SMX from 83.5%to 56.7%within a 120-min reaction *** addition,alkaline conditions(ph≥8.0)inhibited CFA and BZF degradations,while nonacidic ph(ph≥7.0)remarkably inhibited SMX *** of the kinetic model indicated the formation of phosphate(h_(2)PO_(4)^(·)/hPO_(4)^(·-))and/or carbonate radicals(CO_(3)^(·-))could limit pharmaceutical *** transformation products(TPs)of the pharmaceuticals revealed more incompletely oxidized TPs occurred in the phosphate-and(bi)carbonate-containing m Fe-PS systems,and indicated that h_(2)PO_(4)^(·)/hPO_(4)^(·-)mainly degraded pharmaceuticals via a benzene ring-opening reaction while CO_(3)^(·-)preferentially oxidized pharmaceuticals via a hydroxylation reaction.

关键词： Pharmaceutical degradation human urine Iron-activated persulfate system Phosphate radicals Carbonate radicals Transformation products

Re-delocalization of localized d-electrons in VO_(2)(R)-VS_(4)hetero-structure enables high performance of rechargeable Mg-ion batteries

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Journal of Magnesium and Alloys 2024年第5期12卷 1830-1840页

作者： Lijiao Zhou Chao Shen Xueyang hou Zhao Fang Ting Jin Keyu xie School of Materials Science and Engineering Northwestern Polytechnical UniversityXi’an 710072China School of Metallurgical Engineering Xi’an University of Architecture and TechnologyXi’an 710055China

Rechargeable Mg-ion batteries(MIBs)have attracted much more attentions by virtue of the high capacity from the two electrons ***,the reversible Mg^(2+)diffusion in cathode materials is restricted by the strong interactions between the high-polarized bivalent Mg^(2+)ions and anionic ***,we design and propose a hetero-structural VO_(2)(R)-VS_(4)cathode,in which the re-delocalized d-electrons can effectively shield the polarity of Mg^(2+)***,the electrons should spontaneously transfer from VS_(4)to VO_(2)(R)through the interfaces of hetero-structure due to the lower work function value of VS_(4).Furthermore,the internal electrons transfer lead to the electronic injection into VO_(2)(R)from VS_(4)and the partially broken V-V dimers,indicating the presence of lone pair electrons and charge *** from the shield effect of re-delocalized electrons,and the weakened attraction between cations and O/S anions enables more S^(2-)-S_(2)^(2-)redox groups to participate the electrochemical reactions and compensate the double charge of Mg^(2+)***,VO_(2)(R)-VS_(4)hetero-structure exhibits a high specific capacity of 554 mA h g^(-1)at 50 mA g^(-1).It is believed that the charge re-delocalization of cathode extremely boost the Mg^(2+)ions migration for the high-capacity of MIBs.

关键词： Mg-ion batteries Cathode Charge delocalization Electronic structure heterostructure