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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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Microscopic growth mechanism and edge states of monolayer 1T'-MoTe2

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Chinese Physics B 2024年第4期33卷 474-480页

作者：赵海鹏刘隐杨胜国林陈昉陈明星 Kai Braun 罗心仪李思宇潘安练王笑 Key Laboratory for Micro-Nano Physics and Technology of Hunan Province School of Physics and ElectronicsCollege of Materials Science and Engineering Hunan University Key Laboratory of Low-Dimensional Quantum Structures and Quantum Control of Ministry of Education Synergetic Innovation Centre for Quantum Effects and Applications (SICQEA) Hunan Normal University State Key Laboratory of Powder Metallurgy Central South University institute of physical and theoretical chemistry and lisa+ University of Tübingen

Transition metal ditellurides（TMTDs） have versatile physical properties,including non-trivial topology,Weyl semimetal states and unique spin *** growth of high-quality and large-scale monolayer TMTDs with preferred crystal phases is crucial for their ***,we demonstrate the epitaxial growth of 1T'-MoTe2on Au（111）and graphitized silicon carbide（Gr/SiC） by molecular beam epitaxy（MBE）.We investigate the morphology of the grown1T'-MoTe2at the atomic level by scanning tunnelling microscopy（STM） and reveal the corresponding microscopic growth *** is found that the unique ordered Te structures preferentially deposited on Au（111） regulate the growth of monolayer single crystal 1T'-MoTe2,while the Mo clusters were preferentially deposited on the Gr/SiC substrate,which impedes the ordered growth of monolayer *** confirm that the size of single crystal 1T'-MoTe2grown on Au（111）is nearly two orders of magnitude larger than that on Gr/*** scanning tunnelling spectroscopy（STS）,we observe that the STS spectrum of the monolayer 1T'-MoTe2nano-island at the edge is different from that at the interior,which exhibits enhanced conductivity.

关键词： 1T′-MoTe2 microscopic growth mechanism scanning tunneling microscopy/spectroscopy (STM/S) transition metal ditellurides

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K-core attack, equilibrium K-core,and kinetically constrained spin system

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Chinese Physics B 2024年第6期33卷 14-26页

作者：周海军 institute of theoretical Physics Chinese Academy of SciencesBeijing 100190China MinJiang Collaborative Center for theoretical Physics MinJiang UniversityFuzhou 350108China School of physical Sciences University of Chinese Academy of SciencesBeijing 100049China

Kinetically constrained spin systems are toy models of supercooled liquids and amorphous solids. In this perspective,we revisit the prototypical Fredrickson–Andersen(FA) kinetically constrained model from the viewpoint of K-core combinatorial optimization. Each kinetic cluster of the FA system, containing all the mutually visitable microscopic occupation configurations, is exactly the solution space of a specific instance of the K-core attack problem. The whole set of different jammed occupation patterns of the FA system is the configuration space of an equilibrium K-core problem. Based on recent theoretical results achieved on the K-core attack and equilibrium K-core problems, we discuss the thermodynamic spin glass phase transitions and the maximum occupation density of the fully unfrozen FA kinetic cluster, and the minimum occupation density and extreme vulnerability of the partially frozen(jammed) kinetic clusters. The equivalence between K-core attack and the fully unfrozen FA kinetic cluster also implies a new way of sampling K-core attack solutions.

关键词： Fredrickson–Andersen model K-core attack spin glass jamming

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Energy-information trade-off induces continuous and discontinuous phase transitions in lateral predictive coding

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Science China(Physics,Mechanics & Astronomy) 2024年第6期67卷 79-85页

作者： Zhen-Ye Huang Ruyi Zhou Miao Huang Hai-Jun Zhou Key Laboratory for theoretical Physics Institute of Theoretical PhysicsChinese Academy of SciencesBeijing 100190China School of physical Sciences University of Chinese Academy of SciencesBeijing 100049China School of Optics and Photonics Beijing Institute of TechnologyBeijing 100081China Minjiang Collaborative Center for theoretical Physics Minjiang UniversityFuzhou 350108China

Lateral predictive coding is a recurrent neural network that creates energy-efficient internal representations by exploiting statistical regularity in sensory ***,we analytically investigate the trade-off between information robustness and energy in a linear model of lateral predictive coding and numerically minimize a free energy *** observed several phase transitions in the synaptic weight matrix,particularly a continuous transition that breaks reciprocity and permutation symmetry and builds cyclic dominance and a discontinuous transition with the associated sudden emergence of tight balance between excitatory and inhibitory *** optimal network follows an ideal gas law over an extended temperature range and saturates the efficiency upper bound of energy *** results provide theoretical insights into the emergence and evolution of complex internal models in predictive processing systems.

关键词： predictive coding recurrent neural network phase transition internal model free energy

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Evolution exploration and structure prediction of Keggin-type group IVB metal-oxo clusters

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Chinese Chemical Letters 2024年第5期35卷 487-492页

作者： Run-Han Li Tian-Yi Dang Wei Guan Jiang Liu Ya-Qian Lan Zhong-Min Su School of chemistry South China Normal UniversityGuangzhou 510006China institute of Functional Material chemistry Faculty of ChemistryNortheast Normal UniversityChangchun 130024China institute of theoretical chemistry Jilin UniversityChangchun 130023China

The fascinating chemical structure and broad application prospect of Keggin-type polyoxometalates(POMs)have attracted many chemists to explore and discover *** the traditional Keggin,larger metal atomic radius,higher metal coordinated numbers,lower metal valence states and other features allow the group IVB metal-based Keggin(IVB-Keggin)more space and unknown in terms of structure and ***,density functional theory(DFT)calculations were performed to explore the influences including cores,shells,caps,and terminal ligands,et *** IVB-Keggin,and analyze the possibility of novel structure *** the perspective of multi-layer onion-like clusters,molecular energy level,host-guest interaction energy,surface charge and covalent bond polarity can be further adjusted to achieve the oriented design of functional *** insights are expected to provide theoretical support for experimental synthesis,opening a new perspective to understand the growth of Keggin.

关键词： Keggin Metal-oxo clusters Group IVB Onion pattern DFT

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Asymmetric nucleation processes in spontaneous mode switch of active matter

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Communications in theoretical Physics 2024年第5期76卷 154-158页

作者：杨冰王延颋 CAS Key Laboratory of theoretical Physics Institute of Theoretical PhysicsChinese Academy of SciencesBeijing 100190China School of physical Sciences University of Chinese Academy of SciencesBeijing 100049China

Flocking and vortical are two typical motion modes in active *** it is known that the two modes can spontaneously switch between each other in a finite-size system,the switching dynamics remain *** this work,by computer simulation of a two-dimensional Vicsek-like system with 1000 particles,we find from the perspective of the classical nucleation theory that the forward and backward switching dynamics are asymmetric:going from flocking to vortical is a one-step nucleation process,while the opposite is a two-step nucleation process,with the system staying in a metastable state before reaching the final flocking state.

关键词： active matter dynamics classical nucleation theory

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Color-kinematics duality and dual conformal symmetry for a four-loop form factor in N=4 SYM

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Science China(Physics,Mechanics & Astronomy) 2024年第4期67卷 64-71页

作者： Guanda Lin Gang Yang Siyuan Zhang CAS Key Laboratory of theoretical Physics Institute of Theoretical PhysicsChinese Academy of SciencesBeijing 100190China School of physical Sciences University of Chinese Academy of SciencesBeijing 100049China School of Fundamental Physics and Mathematical Sciences Hangzhou Institute for Advanced StudyUCASHangzhou 310024China International Centre for theoretical Physics Asia-Pacific Beijing/Hangzhou 310024China

We obtain the integrand of full-color four-loop three-point form factor of the stress-tensor supermultiplet in N=4 SYM,based on the color-kinematics(CK)duality and generalized unitarity *** result not only manifests all dual Jacobi relations via CK duality but also contains 133 free *** suggests the constructibility of the form factor at even higher loops via CK *** also find that the planar form factor has a hidden dual conformal symmetry in the lightlike limit of the operator momentum,which is checked up to four loops.

关键词： S-matrix supersymmetric model perturbative calculations

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Cobalt-nanoparticle catalysts derived from zeolitic imidazolate framework@MXene composites for efficient oxidative self-coupling of benzylamines

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Frontiers of Chemical Science and Engineering 2024年第1期18卷 95-106页

作者： Jie Chen Mingyuan Jian Deqiong Xie Kecan Dou Deli Chen Weidong Zhu Fumin Zhang Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China

In this study,we synthesize a catalyst comprising cobalt nanoparticles supported on MXene by pyrolyzing a composite in a N2 ***,the composite comprises a bimetallic Zn/Co zeolitic imidazole framework grown in situ on the outer surface of *** catalytic efficiency of the catalyst is tested for the self-coupling of 4-methoxybenzylamine to produce value-added imine,where atmospheric oxygen(1 atm)is used as the *** on the results,the catalyst displayed impressive catalytic activity,achieving 95.4%yield of the desired imine at 383 K for 8 ***,the catalyst showed recyclability and tolerance toward benzylamine substrates with various functional *** outstanding performance of the catalyst is primarily attributed to the synergetic catalytic effect between the cobalt nanoparticles and MXene support,while also benefiting from the three-dimensional porous ***,a preliminary investigation of potential reaction mechanisms is conducted.

关键词： MXene sacrificial template oxidative self-coupling Co nanoparticles imine

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Covalent triazine frameworks modified by ultrafine Pt nanoparticles for efficient photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 4908-4915页

作者： Xu Han Xueying Ge Wen-Wen He Wangwang Shen Tao Zhou Jian-Sen Wang Rong-Lin Zhong Abdullah MAl-Enizi Ayman Nafady Shengqian Ma School of chemistry and Life Science Advanced Institute of Materials ScienceChangchun University of TechnologyChangchun 130012China Laboratory of theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China Department of chemistry University of North Texas1508 W.Mulberry St.DentonTX 76201USA Department of chemistry College of ScienceKing Saud UniversityRiyadh 11451Saudi Arabia

Pt nanoparticles(PtNPs)as active species have always been considered as one of the best semiconductor materials for photocatalytic hydrogen *** this study,a Schottky heterojunction has been successfully constructed by evenly loading ultrafine PtNPs onto a triazine-based covalent organic frameworks(COFs).This strategy maintained the high activity of these ultra-small PtNPs while maximizing the utilization of the Pt active *** fabricated PtNPs@covalent triazine-based framework-1(CTF-1)composite accomplished a significantly high rate of hydrogen evolution(20.0 mmol·g^(−1)·h^(−1),apparent quantum efficiency(AQE)=7.6%,atλ=450 nm)with 0.40 wt.%Pt loading,giving rise to a 44-fold-increase in the efficiency of the photocatalytic hydrogen production compared to the pristine *** calculations revealed that the strong electron transfer(Q(Pt)=−0.726 qe,in the analysis of Bader charge,Q(Pt)is the charge quantity transferred from Pt cluster to CTF-1,and qe is the unit of charge transfer quantity)between PtNPs and CTF-1 triggers a strong interaction,which makes PtNPs being firmly attached to the structure of CTF-1,thereby enabling high stability and excellent hydrogen production ***,the hydrogen binding free energy(ΔGH*)of PtNPs@CTF-1 is much lower than that of the unmodified CTF-1,leading to a much lower intermediate state and hence a significant improvement in photocatalytic *** overall findings of this work provide a new platform to incorporate metallic NPs into COFs for the design and fabrication of highly efficient photocatalysts.

关键词： Pt nanoparticles covalent triazine-based framework-1(CTF-1) photocatalysts hydrogen evolution reaction

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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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