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Surface reconstruction and structural transformation of twodimensional Ni-Fe MOFs for oxygen evolution in seawater media

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Nano Research 2024年第4期17卷 2429-2437页

作者： Liyuan Xiao Xue Bai Jingyi Han Tianmi Tang Siyu Chen Hui Qi Changmin Hou Fuquan Bai Zhenlu Wang Jingqi Guan Institute of Physical chemistry College of ChemistryJilin UniversityChangchun 130021China The Second Hospital of Jilin University Changchun 130021China State Key Laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China Laboratory of Theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryChangchun 130023China

As a four-electron transfer reaction,oxygen evolution reaction(OER)is limited by large overpotential and slow ***,we in-situ synthesized two-dimensional(2D)Ni-Fe metal-organic framework nanosheets on nickel foam(NixFe-TPA/NF,TPA=terephthalic acid)for oxygen evolution in alkaline and alkaline seawater *** 1 M KOH,Ni3Fe-TPA/NF shows a low overpotential(η10)of 189 mV at 10 mA·cm^(-2) and an ultra-low overpotential of only 260 mV at 500 mA·cm^(-2).In alkaline seawater,Ni3Fe-TPA/NF still provides impressive OER performance,with anη10 of 265 ***-situ Raman characterization results show that the phase transition occurs during the OER,and Ni3FeOOH with more oxygen vacancies is in-situ formed,reducing the OER energy *** functional theory(DFT)reveals that the synergy between Ni and Fe reduces the energy barrier and accelerates the rate-determining *** addition,the ultra-thin 2D sheet structure and the close combination of Ni3FeOOH and highly conductive NF support ensure the high catalytic OER ***,the surface reconstruction and structural modification strategy can be used to design and prepare high-performance OER electrocatalysts for energy-related applications.

关键词： density functional theory(DFT)calculation Ni3FeOOH oxygen evolution reaction seawater electrolysis surface reconstruction

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Emerging perovskite materials for supercapacitors:Structure,synthesis,modification,advanced characterization,theoretical calculation and electrochemical performance

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Journal of Energy chemistry 2024年第2期89卷 41-70,I0003页

作者： Yuehua Qian Qingqing Ruan Mengda Xue Lingyun Chen Department of Applied chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China

As a new generation electrode materials for energy storage,perovskites have attracted wide attention because of their unique crystal structure,reversible active sites,rich oxygen vacancies,and good *** this review,the design and engineering progress of perovskite materials for supercapacitors(SCs)in recent years is ***,the review will focus on four types of perovskites,perovskite oxides,halide perovskites,fluoride perovskites,and multi-perovskites,within the context of their intrinsic structure and corresponding electrochemical performance.A series of experimental variables,such as synthesis,crystal structure,and electrochemical reaction mechanism,will be carefully analyzed by combining various advanced characterization techniques and theoretical *** applications of these materials as electrodes are then featured for various ***,we look forward to the prospects and challenges of perovskite-type SCs electrodes,as well as the future research direction.

关键词： Perovskite Modification engineering Oxygen vacancy Theoretical calculation methodology Supercapacitor

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Micro/nanoelectrode-based electrochemical methodology for single cell and organelle analysis

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Nano Research 2024年第1期17卷 196-206页

作者： Chuchu Xu De Yang Yuchan Wang Ruolin Liu Fan Wang Zhongqun Tian Keke Hu Department of chemistry College of Chemistry&Chemical EngineeringXiamen UniversityXiamen 361005China

Cells are the basic unit of *** analysis of single cells/organelles is essential for uncovering the molecular mechanisms of physiological and pathological processes that are difficult to elucidate on a larger *** paper provides an overview of the commonly used fabrication methods for micro/nanoelectrodes applied in the investigations of single cells/organelles as well as the corresponding electrochemical measurements over the last four years including extracellular measurement,combination of extra and intracellular measurement,intracellular reactive oxygen species and reactive nitrogen species(ROS/RNS)measurement,and isolated organelles measurement.

关键词： single cell/organelle micro/nanoelectrode electrochemical measurement chemical transmitters

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Interfacial oxidized Pd species dominate catalytic hydrogenation of polar unsaturated bonds

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Nano Research 2024年第1期17卷 228-234页

作者： Pengyao You Shaoqi Zhan Pengpeng Ruan Ruixuan Qin Shiguang Mo Yazhou Zhang Kunlong Liu Lansun Zheng Nanfeng Zheng State Key Laboratory for Physical chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Department of chemistry BMCUppsala UniversityBMC Box 576Uppsala S-75123Sweden Department of chemistry University of OxfordOxford OX13QZUK

The determination of catalytically active sites is crucial for the design of efficient and stable catalysts toward desired ***,the complexity of supported noble metal catalysts has led to controversy over the locations of catalytically active sites(e.g.,metal,support,and metal/support interface).Here we develop a structurally controllable catalyst system(Pd/SBA-15)to reveal the catalytic active sites for the selective hydrogenation of ketones to alcohol using acetophenone hydrogenation as model *** investigations demonstrated that unsupported Pd nanocrystals have no catalytic activity for acetophenone ***,oxidized Pd species were catalytically highly active for acetophenone *** catalytic activity decreased with the decreased oxidation state of *** work provides insights into the hydrogenation mechanism of ketones but also other unsaturated compounds containing polar bonds,e.g.,nitrobenzene,N-benzylidene-benzylamine,and carbon dioxide.

关键词： oxidized Pd metal/oxide interface constant particle size Pd/SBA-15 acetophenone hydrogenation

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Access to High-Molecular-Weight Polyethylenes through High Temperature Ethylene Polymerization Catalysed by Ethylene-Bridged ansa-(3-R-Cyclopentadienyl)(Fluorenyl) Zirconocene Complexes

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Chinese Journal of Polymer Science 2024年第1期42卷 42-51,I0007页

作者： Bo Li Haiyan Ma Jiling Huang Shanghai Key Laboratory of Functional Materials chemistry and Laboratory of Organometallic chemistry School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

A series of C1-symmetric ethylene-bridged ansa-(3-R-cyclopentadienyl)(fluorenyl) metallocene complexes(Zr: 1-5;Hf: 6) have been synthesized, characterized and investigated as catalyst precursors for the high temperature ethylene polymerization. Using methylaluminoxane(MAO) as the cocatalyst, zirconium complexes 1-5 bearing a bulky substituent on the 3-position of the cyclopendienyl ring showed high catalytic activities up to 1.48×10^(7) g PE·mol_(Zr)^(-1)·h^(-1) toward the polymerization of ethylene and afforded polyethylenes with high molecular weights(1.49×10^(5)-6.31×10^(5) g/mol), meanwhile exhibting great thermal stability at high temperatures up to 120 ℃ together with a long catalytic life time up to 2 h. By adopting low Al/Zr ratios, such as 125, polyethylenes with ultra high molecular weights up to 2.86×106 g/mol were obtained. It is worthy of noting that zirconium complexes 1-4 bearing a substituent with an aryl pendant showed temperature-dependent activities, which increased rapidly with the increase of polymerization temperature, thus weak interaction of the pendent aryl group with the cationic active center is proposed to account for the very low activities displayed at low temperatures. In contrast to zirconocene complexes 1-5, hafnocene complex 6 only displayed very low catalytic activities toward the polymerization of ethylene and afforded polyethylenes with molecular weights ten times smaller than those obtained by zirconocene complexes 1-5. Zirconocene complexes 1-5 were also able to catalyse the polymerization of propylene at high temperatures, but only afforded waxes with low molecular weights.

关键词： ansa-Metallocene Ethylene Propylene Polymerization High temperature

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In situ embedded bismuth nanoparticles among highly porous carbon fibers for efficient carbon dioxide reduction

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Rare Metals 2024年第9期43卷 4312-4320页

作者： Wei-Jian Guo Ao Zhou Wen-Wen Cai Jin-Tao Zhang Key Laboratory for Colloid and Interface chemistry (Ministry of Education) School of Chemistry and Chemical EngineeringShandong University

Electrocatalysis provides an optimal approach for the conversion of carbon dioxide(CO2) into high-value chemicals, thereby presenting a promising avenue toward achieve carbon neutrality. However, addressing the selectivity and stability challenges of metal catalysts in electrolytic reduction remains a daunting task. In this study, the electrospinning method is employed to fabricate porous carbon nanofibers loaded with bismuth nanoparticles with the help of in situ pyrolysis. The porous carbon nanofibers as conductive support would facilitate the dispersion of bismuth active sites while inhibiting their aggregation and promoting the mass transfer, thus enhancing their electrocatalytic activity and stability. Additionally, nitrogen doping induces electron delocalization in bismuth atoms through metal-support interactions, thus enabling efficient adsorption of intermediates for improving selectivity based on the theoretical calculation. Consequently, Bi@PCNF-500 exhibits the exceptional selectivity and stability across a wide range of potential windows. Notably, its faradaic efficiency(FE) of formate reaches 92.7% in H-cell and94.9% in flow cell, respectively, with good electrocatalytic stability. The in situ characterization and theoretical calculations elucidate the plausible reaction mechanism to obtain basic rules for designing efficient electrocatalyst.

关键词： Carbon dioxide reduction Electron delocalization N-doping Porous carbon nanofiber

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Combining cisplatin and a STING agonist into one molecule for metalloimmunotherapy of cancer

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National Science Review 2024年第1期11卷 107-119页

作者： Shuren Zhang Dongfan Song Wenhao Yu Ji Li Xiaoyu Wang Yachao Li Zihan Zhao Qi Xue Jing Zhao Jie P.Li Zijian Guo State Key Laboratory of Coordination chemistry School of Chemistry and Chemical EngineeringChemistry and Biomedicine Innovation Center (ChemBIC) Nanjing University Department of Urology Afflliated Drum Tower HospitalMedical SchoolNanjing University Nanchuang (Jiangsu)Institute of chemistry and Health

Mounting evidence suggests that strategies combining DNA-damaging agents and stimulator of interferon genes(STING) agonists are promising cancer therapeutic regimens because they can amplify STING activation and remodel the immunosuppressive tumor microenvironment. However, a single molecular entity comprising both agents has not yet been developed. Herein, we designed two PtIV-MSA-2 conjugates(Ⅰand Ⅱ) containing the DNA-damaging chemotherapeutic drug cisplatin and the innate immuneactivating STING agonist MSA-2; these conjugates showed great potential as multispecific small-molecule drugs against pancreatic cancer. Mechanistic studies revealed that conjugate Ⅰ upregulated the expression of transcripts associated with innate immunity and metabolism in cancer cells, significantly differing from cisplatin and MSA-2. An analysis of the tumor microenvironment demonstrated that conjugate I could enhance the infiltration of natural killer(NK) cells into tumors and promote the activation of T cells, NK cells and dendritic cells in tumor tissues. These findings indicated that conjugate I, which was created by incorporating a Pt chemotherapeutic drug and STING agonist into one molecule, is a promising and potent anticancer drug candidate, opening new avenues for small-molecule-based cancer metalloimmunotherapy.

关键词： platinum drug STING agonist single-molecule multitarget metalloimmunology

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A highly reduced Mo_(74) polyoxometalate featuring high proton conductivity accessed by building block strategy

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Science China chemistry 2024年第3期67卷 862-868页

作者： Shi-Yi Liu Xue-Xin Li Wei-Chao Chen Kui-Zhan Shao Xin-Long Wang Chao Qin Zhong-Min Su Key Laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China State Key Laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction *** we demonstrate that it is possible to employ the building block strategy to generate a highly reduced polyoxomolybdate(C_(2)H_(8)N)_(14)(NH_(4))_(4)H_(14)[Mo_(48)-ⅤMo_(26)ⅥO_(202)(OH)_(12)(SO_(4))_(6)]·46H_(2)O(Mo_(74)).The fundamental Mo-based{Mo_x}(x=4,5,and 6) building blocks,which are templated by tetra-coordinated anions{MoO_(4)}or{SO_(4)},not only lay foundation for the formation of Mo_(74) featuring an unprecedented reduction ratio of 65%,but also give rise to SBBs-mediated(secondary building blocks) supramolecular dense packing interactions among the isolated Mo_(74) clusters that are favorable for proton ***,high proton conductivity(2.04×10^(-2)S cm^(-1)) had been realized at 50℃ and 90% relative humidity,revealing one of the well-known POMs-based crystalline proton conducting *** result highlights that this building block approach possesses great potential in producing highly reduced POM systems that can achieve controllable reduced ratio and desirable properties.

关键词： polyoxometalate building block molybdenum highly reduced state proton conduction

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Performance enhancement and active sites identification of Cu-Cd bimetallic oxide derived catalysts for electrochemical CO_(2) reduction

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Journal of Energy chemistry 2024年第4期91卷 50-58页

作者： Cai Wang Xin Hu Bairong Chen Houan Ren Xiaoyu Wang Yilin Zhang Xinyu Chen Yuping Liu Qingxin Guan Wei Li State Key Laboratory of Elemento-Organic chemistry Key Laboratory of Adv.Energy Mater.Chemistry(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China

The development of earth-abundant electrocatalysts with high performance for electrochemical CO_(2)reduction(ECR)is of great ***-based catalysts have been widely investigated for ECR due to their unique ability to generate various carbonaceous products,but directing selectivity toward one certain product and identifying the real active sites during ECR are still full of ***,after the incorporation of CdO into CuO,the Cu_(0.5)Cd_(0.5)-O catalyst achieves a 10.3-fold enhancement for CO selectivity in comparison with CuO,and a CO faradic efficiency nearly 90%with a current density around20 mA cm^(-2)could maintain at least 60 ***,a wide CO/H_(2)ratio(0.07-10)is reached on Cu_(x)Cd_(1-x)-O catalysts by varying the Cu/Cd ratio,demonstrating the potential of syngas production using such *** results of ex situ XRD,XPS,and in situ Raman reveal that the real active sites of Cu_(0.5)Cd_(0.5)-O catalysts for CO production during ECR reaction are the reconstructed mixed phases of CuCd alloy and CdCO_(3).In situ FTIR and theoretical calculations further implicate the presence of Cd related species promotes the CO desorption and inhibits the H_(2)evolution,thus leading to an enhanced CO generation.

关键词： CO_(2)reduction Cu-Cd bimetallic Real active sites CO production

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Molecular solid solution of lanthanide-titanium-oxo clusters with enhanced photocatalytic hydrogen evolution

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Science China chemistry 2024年第2期67卷 529-535页

作者： Rong Chen Chao-Long Chen Hui Zhang Zi-Han Wang Fu-Li Sun Ming-Hao Du Gui-Lin Zhuang Cheng Wang La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Centre of chemistry for Energy Materials State Key Laboratory of Physical chemistry of Solid Surfaces and Department of chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China College of Chemical Engineering Zhejiang University of TechnologyHangzhou310032China

Molecular solid solutions of metal clusters containing different metal centers with well-defined structures can accurately regulate the HOMO-LUMO gap,but are rarely ***,a series of colorless lanthanide-titanium-oxo clusters Ln_(2)Ti_4(μ_(2)-O)_(2)(μ_(3)-O)_4(Piv)_(10)(THF)_(2)(Ln_(2)Ti_4,Ln = Eu,Gd,Tb,and Ce,HPiv = pivalic acid) were synthesized by the reaction of pivalic acid with Ln(Ac)_(3) and titanium *** light yellow crystal of cluster solid solutions Eu_(2)Ti_(4-x)Cd_(x),containing a mixture of Eu_(2)Ti_4 and Eu_(2)Ti_(3)Cd,was obtained by in situ doping Cd^(2+) and S^(2–).Eu_(2)Ti_(3.92)Cd_(0.08) displays efficient photocatalytic hydrogen evolution activity without a co-catalyst,which is up to 2.6 times that of Eu_(2)Ti_*** time-resolved transient absorption spectroscopy and spin-polarized density functional calculations showed that the enhanced photocatalytic performance of Eu_(2)Ti_(4-x)Cd_(x) can be attributed to the narrower HOMO-LUMO gap and lower LUMO position than that of Eu_(2)Ti_*** studyprovides an in situ doping method to realize the simple preparation of cluster solid solution.

关键词： molecular solid solution lanthanide-titanium-oxo clusters photocatalytic hydrogen evolution

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