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Computational design of bimetallic Tm_(2)@g-C_(9)N_(4)electrocatalysts for enhanced CO reduction toward C_(2)products

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Chinese Chemical Letters 2024年第7期35卷 484-490页

作者： Jiajun Wang guolin yi Shengling Guo Jianing Wang Shujuan Li Ke Xu Weiyi Wang Shulai Lei Tianjin Key Laboratory of Structure and Performance for Functional Molecules College of ChemistryTianjin Normal UniversityTianjin 300387China Department of Chemical Physics&Hefei National Laboratory for Physical Sciences at Microscale University of Science and Technology of ChinaHefei 230026China Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices Hubei University of Arts and ScienceXiangyang 441053China Hubei Longzhong Laboratory Xiangyang 441053China

Electrochemical CO reduction(ECOR)as a potential strategy for producing valuable chemicals and fuels has captured substantial ***,the currently available electrocatalysts suffer from poor selectivity and low Faradaic efficiency,limiting their industrial ***,we systematically investigate the potential of homonuclear bimetallic electrocatalysts,Tm_(2)@C_(9)N_(4)(TM=Fe,Co,Ni,and Cu),for the ECOR through extensive density functional theory *** findings suggest that all four proposed monolayers exhibit exceptional stability,making them highly suitable for experimental synthesis and practical ***,these transition-metal dual atoms anchored on C_(9)N_(4)monolayers show great potential in facilitating the production of high-value C_(2)products,such as C_(2)H_(5)OH and C_(2)H_(4),due to the significantly low limiting potentials(-0.06~-0.46 V)and small kinetic energy barriers(0.54–1.08 eV)for the CO coupling ***,with the exception of Ni_(2)@C_(9)N_(4),these bimetallic catalysts demonstrate the impressive suppression of the competitive hydrogen evolution reaction(HER),leading to a high selectivity for C_(2)products in *** predictions would accelerate the development of high-performance C_(9)N_(4)-based dual-atom catalysts for the ECOR.

关键词： C_(9)N_(4)monolayer Double-atom catalysts CO electroreduction Multi-carbon products Density functional theory

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Computational prediction of Mo_(2)@g-C_(6)N_(6) monolayer as an efficient electrocatalyst for N_(2) reduction

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Chinese Chemical Letters 2022年第10期33卷 4623-4627页

作者： Jiajun Wang Mengyao Shi guolin yi Lu Wang Shulai Lei Ke Xu Shujuan Li Jianshuai Mu Tianjin Key Laboratory of Structure and Performance for Functional Molecules College of ChemistryTianjin Normal UniversityTianjin 300387China Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices Hubei University of Arts and ScienceXiangyang 441053China Institute of Mathematics Free University of BerlinBerlin D-14195Germany

Electrocatalytic nitrogen reduction reaction(NRR)is an environmentally friendly method for sustainable ammonia synthesis under ambient *** for efficient NRR electrocatalysts with high activity and selectivity is currently urgent but remains great ***,we systematically investigate the NRR catalytic activities of single and double transition metal atoms(TM=Fe,Co,Ni and Mo)anchored on g-C_(6)N_(6) monolayers by performing first-principles *** on the stability,activity,and selectivity analysis,Mo_(2)@g-C_(6)N_(6) monolayer is screened out as the most promising candidate for *** exploration of the reaction mechanism demonstrates that the Mo dimer anchored on g-C_(6)N_(6) can sufficiently activate and efficiently reduce the inert nitrogen molecule to ammonia through a preferred distal pathway with a particularly low limiting potential of -0.06 *** addition,we find that Mo_(2)@g-C_(6)N_(6) has excellent NRR selectivity over the competing hydrogen evolution reaction,with the Faradaic efficiency being 100%.Our work not only predicts a kind of ideal NRR electrocatalyst but also encouraging more experimental and theoretical efforts to develop novel double-atom catalysts(DACs)for NRR.

关键词： g-C_(6)N_(6)monolayer Double-atom catalysts Nitrogen reduction reaction Hydrogen evolution reaction Limiting potential Density functional theory

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ON LOCALIZATION IN SENSOR NETWORK WITH INACCURATE AND INCOMPLETE DISTANCE MEASUREMENTS

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Journal of Electronics(China) 2007年第1期24卷 60-63页

作者： Sun guolin Wang yi Guo Wei School of Commun. and Info. Eng. Univ. of Electronic Sci. and Tech. of China Chengdu 610054 China

The sensor network localization problem has received a lot of attention in recent years because many important applications resort to node position information. In contrast to the many interesting algorithms proposed in the literature,this paper provides a relatively straightforward procedure that can tackle localization problem for sensor network in a Least Squares Euclidean Dis-tance Matrix Approximation (LS-EDMA) framework. Simulation results reveal that our proposed algorithm is more robust than another popular Multi-Dimensional Scaling (MDS) and Semi-Definite Programming (SDP) based localization techniques,especially with inaccurate and incomplete distance measurements.

关键词： Localization Sensor network Least squares approximation

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Shor's algorithm does not factor large integers in the presence of noise

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Science China(Information Sciences) 2024年第7期67卷 305-320页

作者： Jin-yi CAI College of Letters and Science University of Wisconsin

We consider Shor's quantum factoring algorithm in the setting of noisy quantum gates. Under a generic model of random noise for(controlled) rotation gates, we prove that the algorithm does not factor integers of the form pq when the noise exceeds a vanishingly small level in terms of n—the number of bits of the integer to be factored, where p and q are from a well-defined set of primes of positive density. We further prove that with probability 1-o(1) over random prime pairs(p, q), Shor's factoring algorithm does not factor numbers of the form pq, with the same level of random noise present.

关键词： random noise Shor's algorithm rotation gates quantum computing prime factorization

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How to build a habitable planet:an interview with Charles H. Langmuir

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National Science Review 2024年第6期11卷 76-80页

作者： yi-Gang Xu the Guangzhou Institute of Geochemistry Chinese Academy of Sciences

Earth is the only known habitable planet in the solar system. Understanding how Earth developed its unique habitability has been the frontier of Earth sciences and has become one of the main themes of current deep-space explorations. What are the decisive factors that led to a habitable planet? What is the role of solid Earth processes in the origin of life and in modulating the surface environment? Are Earth’s habitability studies relevant to current challenges that human beings face? These questions have attracted the interest of both scientists and the public alike.

关键词： Earth (planet)

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Optimal Cooperative Secondary Control for Islanded DC Microgrids via a Fully Actuated Approach

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IEEE/CAA Journal of Automatica Sinica 2024年第2期11卷 405-417页

作者： yi Yu Guo-Ping Liu yi Huang Peng Shi IEEE Shenzhen Key Laboratory of Control Theory and Intelligent Systems Southern University of Science and TechnologyShenzhen 518055China School of Electrical Engineering and Automation Wuhan UniversityWuhan 430072China School of Electrical and Mechanical Engineering the University of AdelaideSA 5005Australia Research and Innovation Centre Obuda University1034 BudapestHungary

DC-DC converter-based multi-bus DC microgrids(MGs) in series have received much attention, where the conflict between voltage recovery and current balancing has been a hot topic. The lack of models that accurately portray the electrical characteristics of actual MGs while is controller design-friendly has kept the issue active. To this end, this paper establishes a large-signal model containing the comprehensive dynamical behavior of the DC MGs based on the theory of high-order fully actuated systems, and proposes distributed optimal control based on this. The proposed secondary control method can achieve the two goals of voltage recovery and current sharing for multi-bus DC MGs. Additionally, the simple structure of the proposed approach is similar to one based on droop control, which allows this control technique to be easily implemented in a variety of modern microgrids with different configurations. In contrast to existing studies, the process of controller design in this paper is closely tied to the actual dynamics of the MGs. It is a prominent feature that enables engineers to customize the performance metrics of the system. In addition, the analysis of the stability of the closed-loop DC microgrid system, as well as the optimality and consensus of current sharing are given. Finally, a scaled-down solar and battery-based microgrid prototype with maximum power point tracking controller is developed in the laboratory to experimentally test the efficacy of the proposed control method.

关键词： DC microgrids distributed control high-order fully actuated system approach linear quadratic regulator microgrid modeling secondary control

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Self-assembly of perovskite nanocrystals:From driving forces to applications

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Journal of Energy Chemistry 2024年第1期88卷 561-578,I0013页

作者： yi Li Fei Zhang School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China

Self-assembly of metal halide perovskite nanocrystals(NCs)into superlattices can exhibit unique collective properties,which have significant application values in the display,detector,and solar cell *** review discusses the driving forces behind the self-assembly process of perovskite NCs,and the commonly used self-assembly methods and different self-assembly structures are ***,we summarize the collective optoelectronic properties and application areas of perovskite superlattice ***,we conclude with an outlook on the potential issues and future challenges in developing perovskite NCs.

关键词： Self-assembly Metal halide perovskite Nanocrystals Driving forces

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The Functional Redundancy of Neddylation E2s and E3s in Modulating the Fitness of Regulatory T Cells

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Research 2024年第2期2023卷 373-387页

作者： Di Wu yi Sun Cancer Institute(Key Laboratory of Cancer Prevention and Intervention China National Ministry of Education)of the Second Affiliated Hospital and Institute of Translational MedicineZhejiang University School of MedicineHangzhou 310029China Cancer Center of Zhejiang University Hangzhou 310029China Zhejang Provincial Clinical Research Center for Cancer Zhejang ProvinceChina Key Laboratory of Molecular Biology in Medical Sciences Zhejang ProvinceChina Research Center for Life Science and Human Health Binjiang Institute of Zhejiang UniversityHangzhou 310053China

Neddylation is necessary for activation of Cullin-RING ligases(CRLs),which degrade various immune regulatory *** recent study showed that while depletion of neddylation E2-E3 pair Ube2f-Sag in regulatory T(T_(reg))cells had no obvious phenotype,the same depletion of either Ube2m or Rbx1 caused inflammation disorders with different *** these E2s or E3s compensate each other in functional regulations of T_(reg)cells is,however,previously *** this report,we generated Foxp3^(Cre);Ube2m^(fl/fl);Ube2f^(fl/fl)or Foxp3^(Cre);Rbx1^(fl/fl);Sag^(fl/fl)double-null mice by simultaneous deletion of both neddylation E2s or E3s in T_(reg)cells,***,Ube2m&Ube2f double-null mice developed much severe autoimmune phenotypes than did Ube2m-null mice,indicating that Ube2m markedly compensates Ube2f in T_(reg)*** minor worsened autoimmune phenotypes seen at the very early stage in Rbx1&Sag double-null than Rbx1-null mice is likely due to already severe phenotypes of the later,indicating a minor compensation of Rbx1 for *** RNA profiling-based analyses revealed that up-and down-regulations of few signaling pathways in T_(reg)cells are associated with the severity of autoimmune ***,severer inflammation phenotypes seen in mice with double E3-null than with double E2-null T_(reg)cells indicate a neddylation-independent mechanism of 2 E3s,also known to serve as the RING component of CRLs in regulation of T_(reg)cell fitness.

关键词： Foxp3 inflammation markedly

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Effect of the yaw angle on turbulent flow structures around the submarine model

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Journal of Hydrodynamics 2024年第3期36卷 421-434页

作者： yi-jing Hu yi Qu Qin Wu Biao Huang School of Mechanical Engineering Beijing Institute of TechnologyBeijing100081China Beijing Institute of Electronic System Engineering Beijing100854China

The objective of this paper is to investigate the turbulent flow structures around the submarine model and evaluate the effect of the yaw angle on the turbulent flow *** large eddy simulation based on the boundary data immersion method is used to *** computational domain consists of 1.2×10^(8)uniformly distributed Cartesian orthogonal grid nodes to capture the basic flow characteristics around the *** pressure coefficient,friction coefficient and wake velocity distribution are in good agreement with the experimental *** different types of vortex structures were mainly captured around the model,including horseshoe vortex,sail tip vortex and crossflow separation *** the increase of the yaw angle,the asymmetry of the horseshoe vortex and the tip vortex gradually increases,and the vortex strength of the vortex leg on the windward of the horseshoe vortex and the vortex strength of the tip vortex also increase *** the crossflow separation vortex,the flow separation zone gradually expands and migrates downstream with the increase of the yaw angle.

关键词： Vortex structure submarine model boundary data immersion method yaw angle

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Vanadium(V) Complexes Containing Unsymmetrical N-Heterocyclic Carbene Ligands: Highly Efficient Synthesis and Catalytic Behavior towards Ethylene/Propylene Copolymerization

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Chinese Journal of Polymer Science 2024年第1期42卷 32-41,I0006页

作者： yi-Cong Wang Hui Zhat Pei-yi Cheng Shu Zhang Xiang-Wei Liu yi-Xian Wu State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBejing 100029China

The highly efficient method has been developed for the synthesis of NHC·VOCl_(3) containing symmetrical or unsymmetrical Nheterocyclic carbene(NHC) ligands by the transmetallation reaction of NHC·AgCl with VOCl_(3).The total isolated yield of VOCl_(3)[1,3-(2,4,6-Me_(3)C_(6)H_(2))_(2)(NCH=)_(2)C:](V4') reached 86% by transmetallation reaction,which is much higher than that(48%) by direct coordination *** methodology has also been used to synthesize the novel vanadium complexes containing unsymmetrical NHC ligands of VOCl_(3)[PhCH_(2)NCH=CHNR)C:](V5',R=2,4,6-Me_(3)C_(6)H_(2);V6',R=2,4-Me_(2)-6-Ph-C_(6)H_(2);V7',R=2,6-^(i)Pr_(2)-C_(6)H_(3)) with high yield,which could not be obtained by direct coordination *** catalytic activity and copolymerization ability would be improved by introducing unsymmetrical NHC ligands due to their less steric bulky *** vanadium complex V5' containing unsymmetrical NHC ligand exhibits higher catalytic activity(3.7×10^(5)g_(copolymer)·mol^(-1) of V·h^(-1)) than that of V4' containing symmetrical NHC ***,the higher propylene incorporation ratio(45.6 mol%) in the copolymers of ethylene with propylene could be obtained by using V5' than that(39.9%) by using V4'.The results would provide a highly efficient strategy for the synthesis of early transition metal complexes containing versitile NHC ligands,affording the catalyst with both high catalytic activity and copolymerization ability for the synthesis of high performance polyolefin elastomers.

关键词： Vanadium complex N-heterocyclic carbene ligand Transmetallation reaction Copolymerization of ethylene with propylene

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