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Diatomic Fe-Co catalysts synergistically catalyze oxygen evolution reaction

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Nano Research 2024年第5期17卷 3794-3800页

作者： Tianmi Tang Jingyi Han Zhenlu Wang Xiaodi Niu Jingqi Guan Institute of physical chemistry College of ChemistryJilin UniversityChangchun 130021China College of Food Science and Engineering Jilin UniversityChangchun 130062China

The design of diatomic catalysts with uniformly dispersed metal atoms is expected to improve catalytic performance,which is conducive to the intensive comprehending of the synergistic mechanism between dual-metal sites for the oxygen evolution reaction(OER)at the atomic ***,we design a strategy to immobilize bimetallic Fe-Co atoms onto nitrogen-doped graphene to obtain a diatomic catalyst(DA-FC-NG)with FeN_(3)-CoN_(3) *** DA-FC-NG shows excellent OER activity with a low overpotential(η_(10)=268 mV),which is superior to commercial iridium dioxide *** calculations uncover that the excellent activity of DA-FC-NG is due to the interaction between Fe and Co diatoms,which causes charge rearrangement and induces the adsorption of intermediates on the Fe-O-Co bridge structure,thus improving the catalytic OER *** work is of great significance for the design of highly active diatomic catalysts to replace noble metal catalysts for energy-related applications.

关键词： oxygen evolution reaction diatomic catalyst FeN_(3)-CoN_(3) X-ray absorption spectroscopy(XAS)spectrum theoretical calculation

Switching on/off phosphorescent or non-radiative channels by aggregation-induced quantum interference

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Aggregate

Aggregate 2024年第1期5卷 175-184页

作者： Yi Kong Yu-Chen Wang Xunkun Huang WanZhen Liang Yi Zhao department of chemistry State Key Laboratory of Physical Chemistry of Solid SurfacesiChEMFujian Provincial Key Laboratory of Theoretical and Computational Chemistryand College of Chemistry and Chemical EngineeringXiamen UniversityXiamenPeople’s Republic of China

Pure organic materials with persistent and efficient room-temperature phosphorescence have recently aroused great research interest due to their vast potential in *** crucial design principle for such materials is to suppress as much as possible the non-radiative decay of the triplet exciton while maintaining a moderate phosphorescent radiative ***,molecular engineering often exhibits similar regulation trends for the two ***,we propose that the quantum interference caused by aggregation can be utilized to control the phosphorescent and non-radiative decay *** systematically analyze various constructive and destructive transition pathways in aggregates with different molecular packing types and establish clear relationships between the luminescence characters and the signs of the singlet and triplet excitonic *** is shown that the decay channels can be flexibly switched on or off by regulating the packing type and excitonic *** importantly,an enhanced phosphorescent decay and a completely suppressed non-radiative decay can be simultaneously realized in the aggregate packed with inversion *** work lays the theoretical foundation for future experimental realization of quantum interference effects in phosphorescence.

关键词： excitonic coupling intersystem crossing organic aggregates organic room temperature phosphorescence quantum interference

Quantitative lithium substitution of carboxyl hydrogens in polyacrylic acid binder enables robust SiO electrodes with durable lithium storage stability

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Journal of Energy chemistry 2024年第10期97卷 352-360页

作者： Weihua Wang Wenyi Li Siyi Jing Huiping Yang Huiqun Wang Ling Huang Yuxiang Mao Xikun Pang Yudai Huang Li Zhang State Key Laboratory of physical chemistry of Solid Surfaces Department of Chemical and Biochemical Engineering College of Chemistry and Chemical EngineeringCollaborative Innovation Centre of Chemistry for Energy Materials (iChEM) Xiamen University State Key Laboratory of chemistry and Utilization of Carbon-Based Energy Resources College of Chemistry Xinjiang University

The design of advanced binders plays a critical role in stabilizing the cycling performance of large-volume-effect silicon monoxide（SiO） *** the classic polyacrylic acid（PAA） binder,the self-association of-COOH groups in PAA leads to the formation of intramolecular and intermolecular hydrogen bonds,greatly weakening the bonding force of the binder to SiO ***,strengthening the binder-material interaction from the perspective of binder molecular regulation poses a significant ***,a modified PAA-Lix（0.25 ≤x≤1） binder with prominent mechanical properties and adhesion strength is specifically synthesized for SiO anodes by quantitatively substituting the carboxylic hydrogen with *** appropriate lithium substitution（x=0.25） not only effectively increases the number of hydrogen bonds between the PAA binder and SiO surface owing to charge repulsion effect between ions,but also guarantees moderate entanglement between PAA-Lixmolecular chains through the ion-dipole *** such,the PAA-Li0.25/SiO electrode exhibits exceptional mechanical properties and the lowest volume change,as well as the optimum cycling(1237.3 mA h g-1after 100cycles at 0.1 C) and rate performance(1000.6 mA h g-1at 1 C),significantly outperforming the electrode using pristine PAA *** work paves the way for quantitative regulation of binders at the molecular level.

关键词： Adhesion strength Charge repulsion effect Polyacrylic acid binder Quantitative lithium substitution SiO anode

High-rate lithium-ion battery performance of a ternary sea urchin-shaped CoNiO_(2)@NiP_(6)Mo_(18)/CNTs composites

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Journal of Energy chemistry 2024年第9期96卷 516-525页

作者： Li-ping Cui Shuang Sun Kai Yu Shu Zhang Mei-lin Wang Jia-jia Chen Bai-bin Zhou Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Chemistry and Chemical EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina State Key Laboratory of physical chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringCollaborative Innovation Centre of Chemistry for Energy MaterialsXiamen UniversityXiamen 361005FujianChina

Bimetallic oxides are attractive anode materials for lithium-ion batteries(LIBs)due to their large theoretical ***,the low conductivity,short cycle life,and poor rate capability are the bottlenecks for their further *** overcome above issues,the basket-like polymolybdate(NiP_(6)Mo_(18))and carbon nanotubes(CNTs)were uniformly embedded on the urchin-shaped CoNiO_(2)nanospheres to yield a ternary composites CoNiO_(2)@NiP_(6)Mo_(18)/CNTs via electrostatic *** multi-level morphology of urchin spinules accelerates the diffusion rate of Li^(+);CNT improves the conductivity and enhances cycle stability of the material;and heteropoly acid contributes more redox activity ***,CoNiO_(2)@NiP_(6)Mo_(18)/CNTs as an anode of LIBs exhibits a high initial capacity(1396.7 mA h g^(−1)at 0.1 A g^(−1)),long-term cycling stability(750.2 mA h g^(−1)after 300 cycles),and rate performance(450.3 mA h g^(−1)at 2 A g^(−1)),which are superior to reported metallic oxides anode of *** density functional theory(DFT)and kinetic mechanism suggest that CoNiO_(2)@NiP_(6)Mo_(18)/CNTs delivers an outstanding pseudocapacitance and rapid Li^(+)diffusion behaviors,which is due to the rich surface area of the urchin-like CoNiO_(2)with the uniform embeddedness of NiP_(6)Mo_(18)and *** study provides a new idea for optimizing the performance of bimetallic oxides and developing high-rate lithium-ion battery composites.

关键词： Bi-metal oxides Transition metal oxides Polyoxometalates Nanocomposite LIBs

Na_(3)P interphase reduces Na nucleation energy enabling stable anode-less sodium metal batteries

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Journal of Energy chemistry 2024年第9期96卷 448-455页

作者： Haizhao Yang Haifeng Lv En Zhou Xiaohao Ji Chunnian Chen Haolei Yu Zhaowei Sun Dawei Zhang Hongchang Jin Xianghua Kong Hengxing Ji department of chemistry and Chemical Engineering Hefei University of TechnologyHefei 230009AnhuiChina Hefei National Research Center for physical Sciences at the Microscale School of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230026AnhuiChina

Sodium metal batteries(SMBs)are rising as viable alternatives to lithium-ion systems due to their superior energy density and sodium's relative ***,SMBs face significant impediments,particularly the exceedingly high negative-to-positive capacity ratios(N/P ratios)which severely encumber energy density and hinder their practical ***,a novel nucleophilic Na_(3)P interphase on aluminum foil has been designed to significantly lower the nucleation energy barrier for sodium atom deposition,resulting in a remarkable reduction of nucleation overpotential and efficient mitigation of dendritic growth at high sodium deposition of 5 mA h cm^(−2).The interphase promotes stable cycling in anode-less SMB configurations with a low N/P ratio of 1.4 and high cathode mass loading of 11.5 mg cm^(−2),and demonstrates a substantial increase in high capacity retention of 92.4%after 500 cycles even under 1 C rate *** innovation signifies a promising leap forward in the development of high-energy-density,anode-less SMBs,offering a potential solution to the longstanding issues of cycle stability and energy efficiency.

关键词： Anode-less Phosphorus anode Nucleation buffer layer Sodium metal Dendrite-free

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

Construction of a Metallacyclopentadiene Ring through the Attack of Carbanions to M≡C Bond Followed by C—H Activation

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Chinese Journal of chemistry 2024年第3期42卷 235-242页

作者： Chun Tang Shengjie Zhang Zhengyu Lu Qian Li Ming Luo Dafa Chen Haiping Xia State Key Laboratory of physical chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringCollaborative Innovation Center of Chemistry for Energy MaterialsXiamen UniversityXiamenFujian361005 China Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Catalysis Department of ChemistrySouthern University of Science and TechnologyShenzhenGuangdong518055 China

Metallacyclopentadienes are important metallacycles and regarded as intermediates in many reactions,therefore,new methods to achieve them are *** this study,a formal[3+2]method,through the reactions of an osmapentalyne with benzyl carbanions,was *** reactions underwent a nucleophilic attack of carbanions to the Os≡C bond,followed by C—H activation to form the five-membered osmacyclopentadiene *** of the reactions were carried out at room temperature,the substituents on the aromatic rings of benzyl carbanions are diverse,and the resulting products contain an Os—H bond,representing a novel type of 10C-carbolong *** work provides a new convenient route to construct metallacyclopentadienes,which is expected to further promote the development of such a type of substances.

关键词： Metallacyclopentadiene Carbolong chemistry Osmium C–H activation Nucleophilic addition

Observation of high ionic conductivity of polyelectrolyte microgels in salt-free solutions

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Chinese Chemical Letters 2024年第4期35卷 255-259页

作者： Qiangwei Wang Huijiao Liu Mengjie Wang Haojie Zhang Jianda Xie Xuanwei Hu Shiming Zhou Weitai Wu State Key Laboratory for physical chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsThe Key Laboratory for Chemical Biology of Fujian Provinceand Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China School of Materials Science and Engineering Xiamen University of TechnologyXiamen 361024China Hefei National Laboratory for physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China School of chemistry and Chemical Engineering Ningxia UniversityYinchuan 750021China

Here, we report an observation that illustrate the potential of polyelectrolyte microgels in salt-free solutions to display a high ionic conductivity. Laser light scattering and ionic conductivity tests on very dilute aqueous dispersions of the microgels indicate that both small size and swollen state of gel particles play vital roles, which should favor the counterions to freely penetrate and leave gel particles, and thus can contribute to the ion-conducting property. Upon discovering this on microgels that are composed of imidazolium-based poly(ionic liquid), we also illustrate the generality of the finding to single lithium-ion polyelectrolyte microgels that are of more technically relevant features for applications, for instance, as injectable liquid “microgel-in-solution” electrolytes of high conductivity(ca. 8.2 × 10^(-2)S/m at 25.0 ℃ for1.0 × 10^(-2)g/m L of microgels in a LiNO_(3)-free 1:1 v/v mixture of 1,2-dioxolane and dimethoxymethane) and high lithium-ion transference number(0.87) for use in the rechargeable lithium-sulfur battery.

关键词： Polyelectrolhyte Stimuli-responsive Single-ion conducting Liquid electrolyte Lithium metal battery

Counterion-Mediated Hydrogen Bonding Making Strong Polyelectrolytes pH-Responsive:Current Understanding and Perspectives

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Chinese Journal of Polymer Science 2024年第9期42卷 1270-1277,I0005页

作者： Yue Huang Guang-Tao Mei Zan Hua Guang-Ming Liu Hefei National Research Center for physical Sciences at the Microscale Department of Chemical PhysicsKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesUniversity of Science and Technology of ChinaHefei230026China The Key Laboratory of Functional Molecular Solids Ministry of Educationand Department of Materials ChemistrySchool of Chemistry and Materials ScienceAnhui Normal UniversityWuhu214002China

The counterion-mediated hydrogen bonding(CMHB)is related to the hydrogen bonding between bound counterions and polyelectrolyte chains in polyelectrolyte systems,where the counterions can both electrostatically bind to the charged groups of polyelectrolyte chains and act as hydrogen bond donors or acceptors to form hydrogen bonds with the hydrogen bond sites associated with polyelectrolyte chains simultaneously.A large number of literatures illustrate that strong polyelectrolytes(SPs)are insensitive to pH,which severely limmits the applications of SPs as smart ***,our studies have demonstrated that the CMHB makes SPs *** perspective discusses the mechanism of pH responsiveness of SPs and the pH-tunable properties of SPs,based on the pH-controlled CMHB *** future research directions on the pH responsiveness of SPs are also discussed *** is anticipated that the study of the pH responsiveness of SPs not only will provide a new understanding of the fundamental properties of SPs,but also will greatly expand the applications of SPs in the field of smart materials.

关键词： Counterion binding Hydrogen bond Polyelectrolyte brush Polyelectrolyte complexation