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

Aggregate

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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

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Vibronic coupling effect on intersystem crossing rates of TADF emitters

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Chinese Journal of Structural chemistry 2024年第6期43卷 22-24页

作者： Xin Huang Yi Zhao Wanzhen Liang State Key laboratory of physical chemistry of Solid Surfaces iChEMFujian Provincial Key Lab of Theoretical and Computational ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China

To take advantage of all the singlet and triplet excitons and then achieve 100%internal quantum efficiency in OLED devices,the scientists have proposed the thermally activated delayed fluorescence(TADF)strategy which tries to achieve"delayed"fluorescence by converting triplet excitons to singlet excitons through a reverse intersystem crossing(ISC/RISC)process with the help of thermal activation[1].In the early days,the efficient RISC processes were facilitated by a negligible energy gap(△E_(ST))and a large spin-orbit coupling(SOC)matrix element(SOCME)between the first singlet(S_(1))and triplet(T_(1))excited states.

关键词： coupling system emitter

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Preliminary discussion on the ignition mechanism of exploding foil initiators igniting boron potassium nitrate

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Defence Technology（防务技术） 2024年第2期32卷 222-231页

作者： Haotian Jian Guoqiang Zheng Lejian Chen Zheng Ning Guofu Yin Peng Zhu Ruiqi Shen School of chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China Micro-Nano Energetic Devices Key laboratory of MIIT Nanjing University of Science and TechnologyNanjing 210094China Anhui Province Key laboratory of Microsystem the 43rd Research Institute of CETCHefei 230088China Science and Technology on applied physical and chemistry laboratory Shanxi Applied Physics and Chemistry Research Institute Xi'an 710061China

Exploding foil initiator(EFI)is a kind of advanced device for initiating explosives,but its function is unstable when it comes to directly igniting *** solve the problem,this research aims to reveal the ignition mechanism of EFIs directly igniting *** oscilloscope,a photon Doppler velocimetry,and a plasma spectrum measurement system were employed to obtain information of electric characteristics,impact pressure,and plasma *** results of the electric characteristics and the impact pressure were inconsistent with ignition *** only thing that the ignition success tests had in common was that their plasma all had a relatively long period of high-temperature duration(HTD).It eventually concludes that the ignition mechanism in this research is the microconvection heat transfer rather than the shock initiation,which differs from that of exploding foil initiators detonating ***,the methods for evaluating the ignition success of semiconductor bridge initiators are not entirely applicable to the tests mentioned in this *** HTD is the critical parameter for judging the ignition success,and it is influenced by two factors:the late time discharge and the energy of the electric *** longer time of the late time discharge and the more energy of the electric explosion,the easier it is to expand the HTD,which improves the probability of the ignition success.

关键词： Exploding foil initiator PDV Plasma spectrum Ignition mechanism Boron potassium nitrate

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Could π-aromaticity cross an unsaturated system to a fully saturated one?

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Chinese Chemical Letters 2024年第6期35卷 298-302页

作者： Shicheng Dong Jun Zhu State Key laboratory of physical chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials(iChem)Fujian Provincial Key Laboratory of Theoretical and Computational ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China School of Science and Engineering The Chinese University of Hong KongShenzhen 518172China

The classification of π-/σ-aromaticity depends on the electrons with the dominating ***,π-andσ-aromaticity are used to describe the unsaturated and saturated systems,***,it is rarely reported that π-aromaticity is dominated in a saturated *** we demonstrate that π-aromaticity could be dominating in several fully saturated four-membered rings(4MRs),supported by various aromaticity indices including ΔBL,NICS,EDDB,MCI,and Ad *** origin of suchπ-aromaticity in saturated rings could be attributed to an introduction of two additional electrons into the π-type LUMO of the parent neutral *** findings represent a novel approach to achieve π-aromaticity into a fully saturated system which has traditionally been dominated by σ-aromaticity.

关键词： π-Aromaticity Saturated rings Silicon

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Rational design of vitamin C/defective carbon van der Waals heterostructure for enhanced activity,durability and storage stability toward oxygen reduction reaction

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Journal of Energy chemistry 2024年第1期88卷 103-111,I0003页

作者： Ruiqi Cheng Kaiqi Li Huanxin Li Tianshuo Zhao Yibo Wang Qingyue Xue Jiao Zhang Chaopeng Fu Shanghai Key laboratory of Advanced High-temperature Materials and Precision Forming School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Christopher Ingold laboratory Department of ChemistryUniversity College LondonLondon WC1H 0AJUK Department of chemistry Physical&Theoretical Chemistry LaboratoryUniversity of OxfordSouth Parks RoadOxford OX13QZUK

Metal-free defective carbon materials with abundant active sites have been widely studied as low-cost and efficient oxygen reduction reaction(ORR)electrocatalysts in metal-air ***,the active sites in defective carbon are easily subjected to serious oxidation or hydroxylation during ORR or storage,leading to rapid degradation of ***,we design a van der Waals heterostructure comprised of vitamin C(VC)and defective carbon(DC)to not only boost the activity but also enhance the durability and storage stability of the DC-VC *** formation of VC van der Waals between DC and VC is demonstrated to be an effective strategy to protect the defect active sites from oxidation and hydroxylation degradation,thus significantly enhancing the electrochemical durability and storage anti-aging ***,the DC-VC van der Waals can reduce the reaction energy barrier to facilitate the *** findings are also confirmed by operando Fourier transform infrared spectroscopy and density functional theory *** is necessary to mention that the preparation of this DC-VC electrocatalyst can be scaled up,and the ORR performance of the largely produced electrocatalyst is demonstrated to be very ***,the DC-VC-based aluminum-air batteries display very competitive power density with good performance maintenance.

关键词： Van der Waals heterostructure Oxygen reduction reaction Stability Scalable production Aluminum-air battery

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Understanding Bonding Nature ofα-Keggin Polyoxometalates[XW_(12)O_(40)]^(n−)(X=Al,Si,P,S):A Generalized Superatomic Perspective

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Energy & Environmental Materials 2024年第6期7卷 176-183页

作者： Rui Li Yulei Shi Famin Yu Rui Wang Haitao Yan Boon K.Teo Zhigang Wang Department of Physics Capital Normal UniversityBeijing 100048China Key laboratory of Material Simulation Methods&Software of Ministry of Education College of PhysicsJilin UniversityChangchun 130012China Institute of Atomic and Molecular Physics Jilin UniversityChangchun 130012China State Key laboratory for physical chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Institute of theoretical chemistry College of ChemistryJilin UniversityChangchun 130012China

α-Keggin polyoxometalates(POMs)[XW_(12)O_(40)]^(n−)(X=Al,Si,P,S)are widely used in batteries owing to their remarkable redox ***,the mechanism underlying the applications appears inconsistent with the widely accepted covalent bonding ***,first-principles calculations show that XW_(12)are core–shell structures composed of a shell and an XO_(4)^(n−)core,both are stabilized by covalent ***,owing to the presence of a substantial number of electrons in W_(12)O_(36)shell,the frontier molecular orbitals of XW_(12)are not only strongly delocalized but also exhibit superatomic properties with high-angular momentum electrons that do not conform to the Jellium *** analysis indicates that energetically high lying filled molecular orbitals(MOs)have reached unusually high-angular momentum characterized by quantum number K or higher,allowing for the accommodation of numerous *** attribute confers strong electron acceptor ability and redox activity to XW_(12).Moreover,electrons added to XW_(12)still occupy the K orbitals and will not cause rearrangement of the MOs,thereby maintaining the stability of these *** findings highlight the structure–activity relationship and provide a direction for tailor-made POMs with specific properties at atomic level.

关键词： first principles molecular orbital polyoxometalate redox activity superatom

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All-inorganic nitrate electrolyte for high-performance lithium oxygen battery

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Nano Research 2024年第5期17卷 4163-4170页

作者： Dongyue Yang Jiayi Du Kai Chen Haoran Zhang Gang Huang Tong Liu Xinbo Zhang Hongjie Zhang State Key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Lithium-oxygen(Li-O_(2))batteries have been regarded as an expectant successor for next-generation energy storage systems owing to their ultra-high theoretical energy ***,the comprehensive properties of the commonly utilized organic salt electrolyte are still unsatisfactory,not to mention their expensive prices,which seriously hinders the practical production and application of Li-O_(2) ***,we have proposed a low-cost all-inorganic nitrate electrolyte(LiNO_(3)-KNO_(3)-DMSO)for Li-O_(2) *** inorganic nitrate electrolyte exhibits higher ionic conductivity and a wider electrochemical stability window than the organic salt *** existence of K+can stabilize the O_(2)-intermediate,promoting the discharge process through the solution pathway with an enlarged *** at an ultra-low concentration of 0.01 M,the K+can still remain stable to promote the solution discharge process and also possess a new function of inhibiting the dendrite growth by electrostatic shielding,further enhancing the battery stability and contributing to the long cycle *** a result,in the 0.99 M LiNO_(3)-0.01 M KNO_(3)-DMSO electrolyte,the Li-O_(2) batteries exhibit prolonged cycling performance(108 cycles)and excellent rate performance(2 A·g^(-1)),significantly superior to the organic salt one.

关键词： Li-O_(2)batteries potassium ions inorganic nitrate electrolyte solution pathway mechanism

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Synergetic Control of Li^(+)Transport Ability and Solid Electrolyte Interphase by Boron-Rich Hexagonal Skeleton Structured All-Solid-State Polymer Electrolyte

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Energy & Environmental Materials 2024年第3期7卷 154-163页

作者： Yanan Li Shunchao Ma Yuehua Zhao Silin Chen Tingting Xiao Hongxing Yin Huiyu Song Xiumei Pan Lina Cong Haiming Xie Department of chemistry National&Local United Engineering Laboratory for Power BatteryNortheast Normal UniversityChangchun 130024China State Key laboratory of Electroanalytical chemistry Changchun Institute of Applied Chemistry Chinese Academy of SciencesChangchun 130022China

High Li^(+)transference number electrolytes have long been understood to provide attractive candidates for realizing uniform deposition of Li^(+).However,such electrolytes with immobilized anions would result in incomplete solid electrolyte interphase(SEI)formation on the Li anode because it suffers from the absence of appropriate inorganic components entirely derived from anions ***,a boron-rich hexagonal polymer structured all-solid-state polymer electrolyte(BSPE+10%LiBOB)with regulated intermolecular interaction is proposed to trade off a high Li^(+)transference number against stable SEI *** Li^(+)transference number of the as-prepared electrolyte is increased from 0.23 to 0.83 owing to the boron-rich cross-linker(BC)*** intriguingly,for the first time,the experiments combined with theoretical calculation results reveal that BOB^(-)anions have stronger interaction with B atoms in polymer chain than TFSI^(-),which significantly induce the TFSI^(-)decomposition and consequently increase the amount of LiF and Li3N in the SEI ***,a LiFePO_(4)|BSPE+10%LiBOBlLi cell retains 96.7%after 400 cycles while the cell without BC-resisted electrolyte only retains 40.8%.BSPE+10%LiBOB also facilitates stable electrochemical cycling of solid-state Li-S *** study blazes a new trail in controlling the Li^(+)transport ability and SEI properties,synergistically.

关键词： all-solid-state electrolyte boron-rich polymer lithium metal batteries lithium-ion transference number solid electrolyte interphase layer

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Screening of transition metal oxides for electrocatalytic nitrate reduction to ammonia at large currents

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Nano Research 2024年第5期17卷 3902-3910页

作者： Qiongfei Wu Weijie Zhu Dongxu Ma Chao Liang Zhoucheng Wang Hanfeng Liang State Key laboratory of physical chemistry of Solid Surfaces Tan Kah Kee Innovation LaboratoryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China College of Chemical Engineering Tianjin UniversityTianjin 300072China

Electrochemical nitrate reduction reaction(NO_(3)RR)towards ammonia,as an emerging and appealing technology alternative to the energy-intensive Haber-Bosch process and inefficient nitrogen reduction reaction,has recently aroused wide concern and ***,the current research of the NO_(3)RR towards ammonia lacks the overall performance comparison of various *** this,we here make a comparison of 12 common transition metal oxide catalysts for the NO_(3)RR under a high cathodic current density of 0.25 A·cm^(-2),wherein Co_(3)O_(4) catalyst displays the highest ammonia Faradaic efficiency(85.15%)and moderate activity(ca.-0.25 V *** hydrogen electrode).Other external factors,such as nitrate concentrations in the electrolyte and applied potential ranges,have also been specifically investigated for the NO_(3)RR.

关键词： nitrate reduction reaction ammonia production transition metal oxides Co_(3)O_(4)

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