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Introducing sulfur to nickel-iron selenide for high-efficiency alkaline seawater electrolysis

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Science China chemistry 2024年第8期67卷 2747-2754页

作者： Xuanwa Chen Yanhui Yu Xingqi Han Huan Wang Yingjie Hua Daoxiong Wu Peilin Deng Juanxiu Xiao Xinlong Tian Jing Li School of Marine Science and Engineering Hainan Provincial Key Lab of Fine ChemistrySchool of Chemistry and Chemical EngineeringHainan UniversityHaikou 570228China Key lab.ratory of Advanced Energy Materials chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China Key lab.ratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province School of Chemistry and Chemical EngineeringHainan Normal UniversityHaikou 571158China

Seawater electrolysis is an effective way to obtain hydrogen(H_(2))in a sustainable ***,the lack of electrocatalysts with high activity,stability,and selectivity for oxygen evolution reaction(OER)severely hinders the development of seawater electrolysis ***,sulfur-doped nickel-iron selenide nanosheets(S-NiFeSe_(2))were prepared by an ion-exchange strategy and served as highly active OER electrocatalyst for alkaline seawater *** overpotential is 367 m V,and it can run stably for over 50 h at 100 m A cm^(-2).Excitingly,the S-NiFeSe_(2)||Pt/C pair exhibits cell voltage of 1.54 V at 10 m A cm^(-2)under alkaline seawater conditions,which can run smoothly for 100 h without decay,and the efficiency of electricity-tohydrogen(ETH)energy conversion reaches more than 80%.Such electrode,with abundant accessible reactive sites and good corrosion resistance,is a good candidate for seawater ***,density functional theory calculations reveal that the surface sulfur atoms can activate the adjacent Ni sites and decrease the free energy changes of the associated intermediates at the adjacent Ni sites for OER,and the step of~*OH→~*O is the potential rate-limiting *** this work,the true reactive site in nickel-iron selenides is the Ni sites,but not the Fe sites as commonly believed.

关键词： S-doping nickel-iron selenide electrocatalysts oxygen evolution reaction alkaline seawater electrolysis

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Injection molding of highly filled microcrystalline cellulose/polycaprolactone composites with the aid of reversible Diels-Alder reaction

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Journal of Materials Science & Technology 2024年第3期170卷 246-254页

作者： Ze Pu Wang WenHong Ruan MinZhi Rong MingQiu Zhang Key lab.ratory for Polymeric Composite and Functional Materials of MOE GD HPPC LabIGCMESchool of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

To tackle the challenge of producing highly filled polymer composites using the traditional injection molding technique,which is characterized by the fairly high melt viscosity that makes mold filling difficult,the authors propose a solution based on dynamic covalent *** demonstrated by the proof-of-concept experiments,the 4-arm starshaped polycaprolactone(PCL)oligomers and microcrystalline cel-lulose(MCC)are crosslinked by the reversible Diels-Alder(DA)*** flowability of the compounds greatly decreases due to the dissociation of the intercomponent DA bonds at the retro-reaction tempera-ture,and the networked architecture is reconstructed during cooling as a result of the forward DA ***,the high-loading MCC fillers are well distributed in the matrix and covalently bonded to the nearby PCL,forming a striking contrast to the control in which linear PCL acts as the *** DA bonds crosslinked biodegradable PCL composites exhibit decent mechanical strength(20.7 MPa)even at the MCC fraction of 65 wt%,which is superior to those(5-12.2 MPa)of the highly filled PCL composites(with filler contents of 50-63.8 wt%)reported so *** proposed approach has sufficient expansibility for the fabrication of the highly filled polymer composites constructed by other types of matrix and fillers.

关键词： Polymer composites Microcrystalline cellulose Polycaprolactone Injection molding Dynamic reversible chemistry

Printable oil-NiO_(X)hole transport layer enables efficient n-i-p perovskite solar cells with a high thermal stability

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Science China chemistry 2024年第7期67卷 2335-2340页

作者： Yazhou Xu Zhaoyang Chu Hongyu Wang Zhi Xing Baojin Fan Xiaotian Hu Yiwang Chen College of chemistry and Chemical Engineering/Institute of Polymers and Energy chemistry(IPEC)/Film Energy chemistry for Jiangxi Provincial Key lab.ratory(FEC) Nanchang UniversityNanchang 330031China Key lab.of Fluorine and Silicon for Energy Materials and chemistry of Ministry of Education Jiangxi Normal University Nanchang 330022China Peking University Yangtze Delta Institute of Optoelectronics Nantong 226010China

Currently,highly efficient n-i-p perovskite solar cells rely on an organic interface layer for high efficiency,especially 2,2',7,7'-tetrakis[N,N-bis(4-methoxyphenyl)ami-no]-9,9′-spirobifluorene(spiro-OMeTAD),but the instability of organic materials in the photothermal field compromises device *** this study,we employ the oleic acid(YS)/oleamine(YA)end-sealing method to achieve uniform dispersion of NiO_(X)nanoparticles,effectively mitigating coagulation resulting from high local concentration and secondary motion ***,the conductivity of the hole transport layer and its energy level alignment with perovskite is enhanced by the additional 2,3,5,6-tetrafluoro-7,7',8,8'-tetracyanodimethyl-p-benzoquinone(F4TCNQ),leading to a remarkable improvement of open-circuit voltage and fill factor,thus the high efficiency of 25.17%and 24.36%on 0.1 and 1.01cm2,***,by realizing an all-inorganic interface layer,an initial efficiency exceeding 90%is maintained even after 2,800 h of heating at 85℃.

关键词： oil-NiO_(X) perovskite solar cells printing technology high efficiency thermal stability

Synthesis,Characterization of Polyethylene Ionomers and Their Antibacterial Properties

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Chinese Journal of Polymer Science 2024年第8期42卷 1077-1084页

作者： Jia-Jia Wu Fei Wang Peng-Qi Wan Li Pan Chun-Sheng Xiao Zhe Ma Yue-Sheng Li Tianjin Key lab.Composite&Functional Materials School of Materials Science and EngineeringTianjin UniversityTianjin 300350China Key lab.Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Owing to its high production volume and wide range of application s,polyethylene has gained a great deal of attention,but its low surface energy and non-polar nature have limited its application in some important *** this study,ethylene/11-iodo-1-undecene copolymers were prepared and used as the intermediates to afford a series of imidazolium-based ionomers bearing methanesulfonate(CH_(3)SO_(3)^(-)),trifluoromethanesulfonate(CF_(3)SO_(3)^(-)),or bis(trifluoromethane)sulfonimide(Tf_(2)N^(-))*** tensile test results showed that the stress-at-break(7.8-25.6 MPa)and the elongation-at-break(445%-847%)of the ionomers could be adjusted by changing the counterion species and the ionic group *** importantly,the ionomers exhibited marvelous antibacterial activities against Staphylococcus aureus(***)and Escherichia coli(***).The ionomers bearing Tf_(2)N^(-)exhibited antibacterial activities>99%against both *** and *** when ionic content reached 9.1%.The imidazolium-based ionomers prepared in this work demonstrated excellent comprehensive properties,especially highefficient and broad-spectrum antibacterial ability,exhibiting the potential fo r the application as the antibacterial materials in packaging,medical,and other fields.

关键词： Polyethylene Ionomer Polymerization catalysis Imidazolium Antibacterial material

Ir single atoms on NiFeZn-LDH matrix for exceptional oxygen evolution reaction

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Nano Research 2024年第8期17卷 7039-7044页

作者： Muhammad Israr Muhammad Humayun Jiaqi Zhang Khadim Shah Xin Tan Chen Chen Yadong Li Department of chemistry Tsinghua UniversityBeijing 100084China Energy Water and Environment LabCollege of Humanities and SciencePrince Sultan UniversityRiyadh11586Saudi Arabia

To address the sluggish kinetics of the oxygen evolution reaction(OER),a potential approach is to rationally design and fabricate extremely effective single atom catalysts(SACs).Using an appropriate matrix to stabilize single-atom active centers with optimal geometric and electronic structures is crucial for enhancing catalytic ***,we report the design and fabrication of Ir single atoms on NiFeZn layered double hydroxide(Ir-SAC/NiFeZn-LDH)electrocatalyst for highly efficient and stable *** is investigated that the NiFeZn support exhibits abundant defect sites and unsaturated coordination *** sites function to anchor and stabilize single Ir single atoms on the *** strong synergetic electronic interaction between the Ir single atoms and the NiFeZn matrix resulted in remarkable OER performance of the as-fabricated Ir-SAC/NiFeZn *** a loading Ir content of 1.09 wt.%,this catalyst demonstrates a highly stable OER activity,with an overpotential of 196 mV at 10 mA·cm^(−2)and a small Tafel slope of 35 mV·dec^(−1)for the OER in a 1 M KOH *** results significantly surpass the performance of the commercially availab.e IrO_(2)catalyst.

关键词： Ir single atoms layered double hydroxides rational design geometric optimization oxygen evolution reaction

From charge storage mechanism to performance:A strategy toward boosted lithium/sodium storage through heterostructure optimization

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Journal of Energy chemistry 2024年第1期88卷 112-124,I0003页

作者： Xiaoke Zhang Guangfa Deng Mianying Huang Zhaohui Xu Jianlin Huang Xuan Xu Zhiguang Xu Maochan Li Lei Hu Xiaoming Lin Key lab.ratory of Theoretical chemistry of Environment Ministry of EducationSchool of ChemistrySouth China Normal UniversityGuangzhou 510006GuangdongChina Anhui lab.ratory of Functional Coordinated Complexes for Materials chemistry and Application School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000AnhuiChina National Engineering Research Center for Carbohydrate Synthesis Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationJiangxi Normal UniversityNanchang 330022JiangxiChina

Solving the problems of low electrical conductivity and poor cycling durability in transition metal oxidesbased anode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has already turned into an urgent *** this paper,we successfully synthesized Co_(2)VO_(4)/Co compounds with Co-VMOF(metal-organic framework)as a sacrificial template and investigated their electrochemical mechanism in order to improve the electrochemical properties of LIBs and *** optimized heaping configuration and the existence of metallic Co catalyzed the formation of radical ions,thereby facilitating higher conductivity,shortening Li+and Na+transport paths,and providing more active ***_(2)VO_(4)/Co constructed with 2-methylimidazole as a ligand showed a discharge capacity of 1605.1 mA h g^(-1)after 300 cycles at 0.1 A g^(-1)in LIB and 677.2 mA h g^(-1)in *** functional theory(DFT)calculation emphasizes the crucial role of Co_(2)VO_(4)/Co in enhancing electrode conductivity,decreasing the migratory energy barrier,and thereby strengthening electrochemical *** heterostructure building technique may pave the way for the development of high-performance LIBs and ***,the problem of the low first-loop coulombic efficiency faced by transition metal oxides is improved.

关键词： Metal-organic framework Heterostructure Lithium-ion batteries Sodium-ion batteries DFT calculation

Self-supported NiFe-LDH nanosheets on NiMo-based nanorods as high-performance bifunctional electrocatalysts for overall water splitting at industrial-level current densities

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Nano Research 2024年第5期17卷 3769-3776页

作者： Yan Zhang Biao Feng MingLei Yan Zhen Shen Yiqun Chen Jingyi Tian Fengfei Xu Guanghai Chen Xizhang Wang Lijun Yang Qiang Wu Zheng Hu Key lab.ratory of Mesoscopic chemistry of Ministry of Education(MOE)and Jiangsu Provincial lab.for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China College of Water Conservancy and Hydropower Engineering Sichuan Agricultural UniversityYa’an 625014China

Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis ***,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-layered double hydroxide(NiFe-LDH)nanosheet arrays on the conductive NiMo-based nanorods deposited on Ni foam to form a three-dimensional(3D)architecture,which exhibits exceptional performances for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In overall water splitting,only the low operation voltages of 1.45/1.61 V are required to reach the current density of 10/500 mA·cm^(-2),and the continuous water splitting at an industrial-level current density of 500 mA·cm^(-2) shows a negligible degradation(1.8%)of the cell voltage over 1000 *** outstanding performance is ascribed to the synergism of the HER-active NiMo-based nanorods and the OER-active NiFe-LDH nanosheet arrays of the hybridized 3D ***,the dense NiFe-LDH nanosheet arrays enhance the local pH on cathode by retarding OH-diffusion and enlarge the electrochemically active surface area on anode,while the conductive NiMo-based nanorods on Ni foam much decrease the charge-transfer resistances of both *** study provides an efficient strategy to explore advanced bifunctional electrocatalysts for overall water splitting by rationally hybridizing HER-and OER-active components.

关键词： alkaline water splitting bifunctional electrocatalysts layered double hydroxides high durability industrial current densities

Real-time identification of multiple nanoclusters with a protein nanopore in single-cluster level

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Nano Research 2024年第1期17卷 262-269页

作者： Ling Zhang Peilei He Huang Chen Qingda Liu Libo Li Xun Wang Jinghong Li Department of chemistry Center for BioAnalytical ChemistryKey Laboratory of Bioorganic Phosphorus Chemistry&Chemical BiologyTsinghua UniversityBeijing 100084China School of chemistry and Chemical Engineering Guangdong Prov Key Lab Green Chem Prod TechnolSouth China University of TechnologyGuangzhou 510640China New Cornerstone Science lab.ratory Shenzhen 518054China Beijing Institute of Life Science and Technology Beijing 102206China Center for BioAnalytical chemistry Hefei National Laboratory of Physical Science at MicroscaleUniversity of Science and Technology of ChinaHefei 230026China

It is important and challenging to analyze nanocluster structure with atomic ***,α-hemolysin nanopore was used to identify nanoclusters at the single molecule level by providing two-dimensional(2D)dwell time–current blockage spectra and translocation event frequency which sensitively depended on their *** such as Anderson,Keggin,Dawson,and a few lacunary Dawson polyoxometalates with very similar structures,even with only a two-atom difference,could be *** nanopore device could simultaneously measure multiple nanoclusters in a mixture qualitatively and ***,molecular dynamics(MD)simulations provided microscopic understandings of the nanocluster translocation dynamics and yielded 2D dwell time–current blockage spectra in close agreement with *** nanopore platform provides a novel powerful tool for nanocluster characterization.

关键词： nanopore single-molecule nanocluster polyoxometalates real-time detection

Highly selective electrosynthesis of 3,4-dihydroisoquinoline accompanied with hydrogen production over three-dimensional hollow CoNi-based microarray electrocatalysts

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Nano Research 2024年第4期17卷 2509-2519页

作者： Yu Xin Liyu Chen Yingwei Li Kui Shen Guangdong Provincial Key lab.for Green Chemical Product Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China State Key lab.ratory of Pulp and Paper Engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

Electrocatalytic oxidation reaction of biomass-based derivatives is an excellent candidate to replace water oxidation for obtaining both value-added products and hydrogen(H_(2)),but the exploration of competent electrocatalysts is still highly ***,two new types of three-dimensional self-supported hollow microarrays containing CoNi layered double hydroxide(CoNi-LDH)and N-doped carbon nanosheets decorated with CoNi alloyed nanoparticles(CoNi-NC)on carbon cloth(CC)are prepared,which are further used as efficient electrocatalysts for tetrahydroisoquinoline(THIQ)electrooxidation and hydrogen evolution reaction(HER),*** demonstrate that the Co-modulated electronic environment for Ni(II)/Ni(Ⅲ)redox-looping in CoNi-LDH is the main factor to boost the selectivity of 3,4-dihydroisoquinoline(DHIQ)for the indirect electrooxidation process of *** functional theory(DFT)calculations reveal that the Ni(Ⅲ)/Co(Ⅲ)dual sites of CoNi-LDH exhibit enhanced adsorption for THIQ but poorer adsorption for DHIQ compared to pure Co(Ⅲ)or Ni(Ⅲ).Therefore,the Ni(Ⅲ)/Co(Ⅲ)dual sites can effectively inhibit the peroxidation of DHIQ to isoquinoline(IQ)over CoNi-LDH,thus improving the selectivity of DHIQ to nearly 100%,much higher than that of its pure Ni ***,CC@CoNi-NC can deliver high HER activity with low overpotential(40 mV@10 mA·cm^(-2))and high exchange current density(3.08 mA·cm^(-2)).Impressively,the assembled flow-cell device with CC@CoNi-LDH anode and CC@CoNi-NC cathode only requires low cell voltage and electricity consumption of 1.6 V and 3.50 kWh per cubic meter of H_(2)(@25 mA·cm^(-2)).

关键词： highly selective electrosynthesis dihydroisoquinolines hydrogen evolution reaction metal-organic frameworks hollow microarrays