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Oxidation Evolution and Activity Origin of N-Doped Carbon in the Oxygen Reduction Reaction

Transactions of Tianjin University 2024年第4期30卷 369-379页

作者： Jiaqi Wu Chuanqi Cheng Shanshan Lu Bin Zhang Yanmei Shi department of Chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China School of Materials science and Engineering Institute of New Energy MaterialsTianjin UniversityTianjin 300072China Tianjin Key Laboratory of Molecular Optoelectronic science Collaborative Innovation Center of Chemical Science and EngineeringTianjin 300072China

N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively ***,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon ***,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not *** this study,we discover a two-step oxida-tion process of N-doped carbon during the *** fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional *** oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)***,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant *** also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.

关键词： Oxygen reduction reaction N-doped carbon Reaction path Structural evolution Oxidation in reduction

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Transition Metal/Lanthanide-Nitrogen Double Bonds Co-stabilized in a Carbon Cage

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Precision Chemistry 2024年第5期2卷 193-199页

作者： Zhanxin Jiang Ziqi Hu Yang-Rong Yao Wenhao Xiang Xinyi Han Jinpeng Xin Huaimin Jin Shangfeng Yang Key Laboratory of Precision and Intelligent Chemistry Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)Department of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Metal−nitrogen double bonds have been commonly reported for conventional metal complexes,but the coexistence of both transition metal−nitrogen and lanthanide−nitrogen double bonds bridged by nitrogen within one compound has never been ***,by encapsulating a ternary transition metallanthanide heteronuclear dimetallic nitride into a C_(84) fullerene cage,transition metal−nitrogen and lanthanide-nitrogen double bonds are costabilized simultaneously within the as-formed clusterfullerene TiCeN@C_(1)(12)-C_(84),which is a representative heteronuclear dimetallic nitride *** molecular structure was unambiguously determined by single-crystal X-ray diffraction,revealing a slightly bentμ2-bridged nitride cluster with short Ti−N(1.761Å)and Ce−N(2.109Å)bond lengths,which are comparable to the corresponding Ti=N and Ce=N double bonds of reported metal complexes and consistent with the theoretically predicted values,confirming their coexistence within TiCeN@C_(1)(12)-C_(84).Density functional theory(DFT)calculations unveil three-center two-electron(3c-2e)bonds delocalized over the entire TiCeN cluster,which are responsible for costabilization of Ti�N and Ce�N double *** electronic configuration of Ti4+Ce^(3+)N^(3−)@C_(84)^(4−)is proposed featuring an intramolecular four-electron transfer,drastically different from the analogous actinide dimetallic nitride clusterfullerene(U_(2))^(9+)N^(3−)@C_(80)^(6−)and trimetallic nitride clusterfullerene(Sc_(2))^(6+)Ti^(3+)^(N3−)@C_(80)^(6−),indicating the peculiarity of 4-fold negatively charged fullerene cage in stabilizing the heteronuclear dimetallic nitride cluster.

关键词： Fullerene metallofullerene transitionmetal lanthanide metal−nitrogen multiplebond

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Strong nonlinear optical processes with extraordinary polarization anisotropy in inversionsymmetry broken two-dimensional PdPSe

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Light(science & Applications) 2024年第8期13卷 1524-1533页

作者： Song Zhu Ruihuan Duan Xiaodong Xu Fangyuan Sun Wenduo Chen Fakun Wang Siyuan Li Ming Ye Xin Zhou Jinluo Cheng Yao Wu Houkun Liang Junichiro Kono Xingji Li Zheng Liu Qi Jie Wang School of Electrical and Electronic Engineering Nanyang Technological University639798 SingaporeSingapore School of Material science and Engineering Nanyang Technological University639798 SingaporeSingapore CINTRA CNRS/NTU/THALES UMI 3288Research Techno PlazaNanyang Technological University637371 SingaporeSingapore School of Materials science and Engineering Harbin Institute of Technology150001 HarbinChina department of Chemistry National University of Singapore117543 SingaporeSingapore GPL Photonics Lab State Key Laboratory of Applied OpticsChangchun Institute of OpticsFine Mechanics and PhysicsChinese Academy of Sciences130033 ChangchunChina School of Electronics and Information Engineering Sichuan University610064 ChengduSichuanChina School of Physical and Mathematical sciences Nanyang Technological University637371 SingaporeSingapore departments of Electrical and Computer Engineering Physics and Astronomyand Materials Science and NanoEngineeringRice UniversityHoustonTXUSA

Nonlinear optical activities,especially second harmonic generation(SHG),are key phenomena in inversion-symmetrybroken two-dimensional(2D)transition metal dichalcogenides(TMDCs).On the other hand,anisotropic nonlinear optical processes are important for unique applications in nano-nonlinear photonic devices with polarization functions,having become one of focused research topics in the field of nonlinear ***,the strong nonlinearity and strong optical anisotropy do not exist simultaneously in common 2D ***,we demonstrate strong secondorder and third-order susceptibilities of 64 pm/V and 6.2×10^(-19)m^(2)/V^(2),respectively,in the even-layer PdPSe,which has not been discovered in other common TMDCs(e.g.,MoS2).Strikingly,it also simultaneously exhibited strong SHG anisotropy with an anisotropic ratio of~45,which is the largest reported among all 2D materials to date,to the best of our *** addition,the SHG anisotropy ratio can be harnessed from 0.12 to 45(375 times)by varying the excitation wavelength due to the dispersion ofχ^(2)*** an illustrative example,we further demonstrate polarized SHG imaging for potential applications in crystal orientation identification and polarization-dependent spatial *** findings in 2D PdPSe are promising for nonlinear nanophotonic and optoelectronic applications.

关键词： materials anisotropy nonlinear

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Imitating and exploring the human brain's resting and task-performing states via brain computing: scaling and architecture

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National science Review 2024年第5期11卷 17-28页

作者： Wenlian Lu Longbin Zeng Jiexiang Wang Shitong Xiang Yang Qi Qibao Zheng Ningsheng Xu Jianfeng Feng DTB Consortium Institute of science and Technology for Brain-Inspired Intelligence Fudan University Key Laboratory of Computational Neuroscience and Brain-Inspired Intelligence(Fudan University) Ministry of Education Fudan University Shanghai Center for Mathematical sciences Fudan University department of Computer science University of Warwick Zhangjiang Fudan International innovation Center Fudan University

A computational human brain model with the voxel-wise assimilation method was established based on individual structural and functional imaging data. We found that the more similar the brain model is to the biological counterpart in both scale and architecture, the more similarity was found between the assimilated model and the biological brain both in resting states and during tasks by quantitative metrics. The hypothesis that resting state activity reflects internal body states was validated by the interoceptive circuit's capability to enhance the similarity between the simulation model and the biological brain. We identified that the removal of connections from the primary visual cortex(V1) to downstream visual pathways significantly decreased the similarity at the hippocampus between the model and its biological counterpart,despite a slight influence on the whole brain. In conclusion, the model and methodology present a solid quantitative framework for a digital twin brain for discovering the relationship between brain architecture and functions, and for digitally trying and testing diverse cognitive, medical and lesioning approaches that would otherwise be unfeasible in real subjects.

关键词： digital twin brain computational cortico-subcortical model fMRI data assimilation interoceptive circuit

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Thick Electrodes of a Self-Assembled MXene Hydrogel Composite for High-Rate Energy Storage

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Energy & Environmental Materials 2024年第4期7卷 255-261页

作者： Leiqiang Qin Jianxia Jiang Lintao Hou Fengling Zhang Johanna Rosen department of Physics Chemistry and Biology (IFM) Link?ping University Flexible Electronics innovation Institute (FEII) Jiangxi Key Laboratory of Flexible Electronics Jiangxi Science and Technology Normal University Guangzhou Key Laboratory of Vacuum Coating Technologies and New Energy Materials Physics Department Jinan University

Supercapacitors based on two-dimensional MXene （Ti3C2Tz） have shown extraordinary performance in ultrathin electrodes with low mass loading,but usually there is a significant reduction in high-rate performance as the thickness increases,caused by increasing ion diffusion *** limitations include restacking of the nanosheets,which makes it challenging to realize the full potential of these electrode materials.

关键词： energy storage high-rate hydrogel MXene self-assemble

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Graphene photodetectors integrated with silicon and perovskite quantum dots

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Microsystems & Nanoengineering 2024年第3期10卷 21-33页

作者： Kashif Abbas Peirui Ji Naveed Ullah Shareen Shafique Ze Zhang Muhammad Faizan Ameer Shenghan Qin Shuming Yang State Key Laboratory for Manufacturing Systems Engineering Xi’an Jiaotong UniversityXi’an 710049China department of Microelectronic science and Engineering Laboratory of Clean Energy Storage and ConversionSchool of Physical Science and TechnologyNingbo Collaborative Innovation Center of Nonlinear Calamity System of Ocean and AtmosphereNingbo UniversityNingbo 315211China

Photodetectors(PDs)play a crucial role in imaging,sensing,communication systems,***(Gr),a leading two-dimensional material,has demonstrated significant potential for photodetection in recent ***,its relatively weak interaction with light poses challenges for practical *** integration of silicon(Si)and perovskite quantum dots(PQDs)has opened new avenues for Gr in the realm of next-generation *** review provides a comprehensive investigation of Gr/Si Schottky junction PDs and Gr/PQD hybrid PDs as well as their *** operating principles,design,fabrication,optimization strategies,and typical applications of these devices are studied and *** these discussions,we aim to illuminate the current challenges and offer insights into future directions in this rapidly evolving field.

关键词： quantum discussions summarized

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Pressure-induced magnetic phase and structural transition in SmSb2

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Chinese Physics B 2024年第6期33卷 484-489页

作者：李涛王舒阳陈绪亮陈春华房勇杨昭荣 science Island Branch of Graduate School University of Science and Technology of China Anhui Key Laboratory of Low-Energy Quantum Materials and Devices High Magnetic Field LaboratoryHFIPS Chinese Academy of Sciences Jiangsu Laboratory of Advanced Functional Materials Department of Physics Changshu Institute of Technology Institutes of Physical science and Information Technology Anhui University Collaborative innovation Center of Advanced Microstructures

Motivated by the recent discovery of unconventional superconductivity around a magnetic quantum critical point in pressurized CeSb2,here we present a high-pressure study of an isostructural antiferromagnetic（AFM） SmSb2through electrical transport and synchrotron x-ray diffraction *** PC～2.5 GPa,we found a pressure-induced magnetic phase transition accompanied by a Cmca→P4/nmm structural phase *** the pristine AFM phase below PC,the AFM transition temperature of SmSb2is insensitive to pressure;in the emergent magnetic phase above PC,however,the magnetic critical temperature increases rapidly with increasing *** addition,at ambient pressure,the magnetoresistivity（MR） of SmSb2increases suddenly upon cooling below the AFM transition temperature and presents linear nonsaturating behavior under high field at 2 *** increasing pressure above PC,the MR behavior remains similar to that observed at ambient pressure,both in terms of temperature-and field-dependent *** leads us to argue an AFM-like state for SmSb2above *** the investigated pressure of up to 45.3 GPa and the temperature of down to 1.8 K,we found no signature of superconductivity in SmSb2.

关键词： high pressure antiferromagnet magnetoresistivity structural transition

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Effective Capacity of URLLC over Parallel Fading Channels with Imperfect Channel State Information

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China Communications 2024年第5期21卷 45-63页

作者： Peng Hongsen Tao Meixia department of Electronic Engineering and the Cooperative Medianet innovation Center Shanghai Jiao Tong UniversityShanghai 200240China

This paper investigates the effective capacity of a point-to-point ultra-reliable low latency communication(URLLC)transmission over multiple parallel sub-channels at finite blocklength(FBL)with imperfect channel state information(CSI).Based on reasonable assumptions and approximations,we derive the effective capacity as a function of the pilot length,decoding error probability,transmit power and the sub-channel *** we reveal significant impact of the above parameters on the effective capacity.A closed-form lower bound of the effective capacity is derived and an alternating optimization based algorithm is proposed to find the optimal pilot length and decoding error *** results validate our theoretical analysis and show that the closedform lower bound is very *** addition,through the simulations of the optimized effective capacity,insights for pilot length and decoding error probability optimization are provided to evaluate the optimal parameters in realistic systems.

关键词： effective capacity finite blocklength regime imperfect CSI parallel fading channels URLLC

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Borohydride Ammoniate Solid Electrolyte Design for All-Solid-State Mg Batteries

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Energy & Environmental Materials 2024年第1期7卷 100-106页

作者： Yuepeng Pang Zhengfang Nie Fen Xu Lixian Sun Junhe Yang Dalin Sun Fang Fang Shiyou Zheng School of Materials and Chemistry University of Shanghai for Science and TechnologyShanghai 200093China Guangxi Key Laboratory of Information Materials&Guangxi Collaborative innovation Centre of Structure and Property for New Energy and Materials Guilin University of Electronic TechnologyGuilin 541004China department of Materials science Fudan UniversityShanghai 200433China

Searching for novel solid electrolytes is of great importance and challenge for all-solid-state Mg *** this work,we develop an amorphous Mg borohydride ammoniate,Mg(BH_(4))_(2)·2NH_(3),as a solid Mg electrolyte that prepared by a NH_(3)redistribution between 3D framework-γ-Mg(BH_(4))_(2)and Mg(BH_(4))_(2)·6NH_(3).Amorphous Mg(BH_(4))_(2)·2NH_(3)exhibits a high Mg-ion conductivity of 5×10^(-4)S cm^(-1)at 75℃,which is attributed to the fast migration of abundant Mg vacancies according to the theoretical ***,amorphous Mg(BH_(4))_(2)·2NH_(3)shows an apparent electrochemical stability window of 0-1.4 V with the help of in-situ formed interphases,which can prevent further side reactions without hindering the Mg-ion *** on the above superiorities,amorphous Mg(BH_(4))_(2)·2NH_(3)enables the stable cycling of all-solid-state Mg cells,as the critical current density reaches 3.2 mA cm^(-2)for Mg symmetrical cells and the reversible specific capacity reaches 141 mAh g^(-1)with a coulombic efficiency of 91.7%(first cycle)for Mg||TiS_(2)cells.

关键词： all-solid-state Mg batteries amorphization Mg borohydride ammoniate Mg vacancy migration solid electrolyte

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Quasinormal modes and isospectrality of Bardeen(Anti-)de Sitter black holes

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Chinese Physics C 2024年第3期48卷 191-202页

作者：赵莹刘文韬张超房熊俊荆继良 department of Physics Key Laboratory of Low Dimensional Quantum Structures and Quantum Control of Ministry of Educationand Synergetic Innovation Center for Quantum Effects and ApplicationsInstitute of Interdisciplinary StudiesHunan Normal UniversityChangsha 410081China department of Physics Faculty of ScienceTokyo University of Science1-3KagurazakaShinjuku-kuTokyo 162-8601Japan

Black holes(BHs)exhibiting coordinate singularities but lacking essential singularities throughout the spacetime are referred to as regular black holes(RBHs).The initial formulation of RBHs was presented by Bardeen,who considered the Einstein equation coupled with a nonlinear electromagnetic *** this study,we investigate the gravitational perturbations,including the axial and polar sectors,of the Bardeen(Anti-)de Sitter black *** derive the master equations with source terms for both axial and polar perturbations and subsequently compute the quasinormal modes(QNMs)through numerical *** the Bardeen de Sitter black hole,we employ the 6thorder WKB *** numerical results reveal that the isospectrality is broken in this ***,the QNM frequencies are calculated using the HH method for the Bardeen Anti-de Sitter black hole.

关键词： Bardeen quasinormal modes master equation

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