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Atomic Catalysts Unlocked by Vintage Theory
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《Bulletin of the Chinese Academy of Sciences》 2025年第2期80-80,共1页
Single-atom catalysts(SACs),in which isolated metal atoms such as palladium(Pd)are anchored on solid supports,promise breakthroughs in energy conversion and catalysis.However,balancing their activity(reaction speed)an... Single-atom catalysts(SACs),in which isolated metal atoms such as palladium(Pd)are anchored on solid supports,promise breakthroughs in energy conversion and catalysis.However,balancing their activity(reaction speed)and stability(longevity)remains challenging,as the interplay between metal atoms,supports,and reactants is poorly understood. 展开更多
关键词 single atom catalysts solid supports metal atomssupportsand SACs PALLADIUM energy conversion atomic catalysts metal atoms
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Numerical Simulation of the Atomization Process for Blast Furnace Slag Granulation
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作者 Li-Li Wang Hong-Xing Qin Nan Dong 《Fluid Dynamics & Materials Processing》 2025年第6期1489-1503,共15页
The so-called close-coupled gas atomization process involves melting a metal and using a high-pressure gas jet positioned close to the melt stream to rapidly break it into fine,spherical powder particles.This techniqu... The so-called close-coupled gas atomization process involves melting a metal and using a high-pressure gas jet positioned close to the melt stream to rapidly break it into fine,spherical powder particles.This technique,adapted for blast furnace slag granulation using a circular seam nozzle,typically aims to produce solid slag particles sized 30–140μm,thereby allowing the utilization of slag as a resource.This study explores the atomization dynamics of liquid blast furnace slag,focusing on the effects of atomization pressure.Primary atomization is simulated using a combination of the Volume of Fluid(VOF)method and the Shear Stress Transport k-ωturbulence model,while secondary atomization is analyzed through the Discrete Phase Model(DPM).The results reveal that primary atomization progresses in three stages:the slag column transforms into an umbrella-shaped liquid film,whose leading edge fragments into particles while forming a cavity-like structure,which is eventually torn into ligaments.This primary deformation is driven by the interplay of airflow velocity in the recirculation zone and the guide tube outlet pressure(Fp).Increasing the atomization pressure amplifies airflow velocity,recirculation zone size,expansion and shock waves,though the guide tube outlet pressure variations remain irregular.Notably,at 4.5 MPa,the primary deformation is most pronounced.Secondary atomization yields finer slag particles as a result of more vigorous primary atomization.For this pressure,the smallest average particle size and the highest yield of particles within the target range(30–140μm)are achieved. 展开更多
关键词 Blast furnace slag granulation close-coupled gas atomization atomization pressure atomization process
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Deep learning-based workflow for atomic image denoising and chemical identification
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作者 Ke Ma Shiqiang Feng +3 位作者 Haihui Hu Yimeng Cai Dechao Chen Lili Han 《Chinese Journal of Structural Chemistry》 2025年第5期63-68,共6页
Aberration-corrected annular dark-field scanning transmission electron microscopy(ADF-STEM)is a powerful tool for structural and chemical analysis of materials.Conventional analyses of ADF-STEM images rely on human la... Aberration-corrected annular dark-field scanning transmission electron microscopy(ADF-STEM)is a powerful tool for structural and chemical analysis of materials.Conventional analyses of ADF-STEM images rely on human labeling,making them labor-intensive and prone to subjective error.Here,we introduce a deep-learning-based workflow combining a pix2pix network for image denoising and either a mathematical algorithm local intensity threshold segmentation(LITS)or another deep learning network UNet for chemical identification.After denoising,the processed images exhibit a five-fold improvement in signal-to-noise ratio and a 20%increase in accuracy of atomic localization.Then,we take atomic-resolution images of Y–Ce dual-atom catalysts(DACs)and Fe-doped ReSe_(2) nanosheets as examples to validate the performance.Pix2pix is applied to identify atomic sites in Y–Ce DACs with a location recall of 0.88 and a location precision of 0.99.LITS is used to further differentiate Y and Ce sites by the intensity of atomic sites.Furthermore,pix2pix and UNet workflow with better automaticity is applied to identification of Fe-doped ReSe_(2) nanosheets.Three types of atomic sites(Re,the substitution of Fe for Re,and the adatom of Fe on Re)are distinguished with the identification recall of more than 0.90 and the precision of higher than 0.93.These results suggest that this strategy facilitates high-quality and automated chemical identification of atomic-resolution images. 展开更多
关键词 atomic-resolution image Deep learning Chemical identification Dual-atoms catalyst atomic dopant Scanning transmission electron microscopy DENOISING
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Atomically dispersed metal site materials for hydrogen energy utilization:Theoretical and experimental study in fuel cells and water electrolysis
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作者 Xinxing Zhan Xin Tong +5 位作者 Hao Ye Zijian Gao Juan Tian Jinliang Zhuang Gaixia Zhang Shuhui Sun 《DeCarbon》 2025年第1期1-12,共12页
Atomically dispersed metal site(ADMS)materials have emerged as a promising class of materials for electrocatalysis reactions in the field of energy conversion.Characterized by individual metal atoms dispersed on suita... Atomically dispersed metal site(ADMS)materials have emerged as a promising class of materials for electrocatalysis reactions in the field of energy conversion.Characterized by individual metal atoms dispersed on suitable supports,ADMS materials provide unique catalytic sites with highly tunable electronic structures.This review summarizes recent advancements in the field,with a focus on the critical roles of support materials,coordination environments,and the mechanisms underlying catalytic activity at the atomic level.First,commonly used density functional theory(DFT)simulations are reviewed,emphasizing their pivotal role in elucidating reaction mechanisms and predicting the behavior of ADMS in electrochemical reactions for hydrogen energy utilization.Then,advancements in ADMS for half-cell electrochemical reactions,including oxygen evolution reaction,hydrogen evolution reaction,and oxygen reduction reaction,as well as their applications in fuel cells and water splitting,are summarized.Finally,the challenges and future prospects of ADMS are discussed.This review underscores the transformative potential of ADMS in electrocatalysis,paving the way for innovative and sustainable energy conversion technologies. 展开更多
关键词 atomically dispersed metal sites catalysts Single-atom catalysts Dual-atom catalysts Fuel cell Water electrolysis
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Recent advances in single-and dual-atom catalysts for efficient nitrogen electro-reduction and their perspectives
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作者 Joyjit Kundu Toshali Bhoyar +3 位作者 Saehyun Park Haneul Jin Kwangyeol Lee Sang-Il Choi 《Advanced Powder Materials》 2025年第2期115-141,共27页
Electrochemical nitrogen reduction reaction(ENRR)is emerging as a favorable option to the power-intensive Haber-Bosch process for ammonia synthesis.However,obstacles such as poor selectivity,low production rates,and c... Electrochemical nitrogen reduction reaction(ENRR)is emerging as a favorable option to the power-intensive Haber-Bosch process for ammonia synthesis.However,obstacles such as poor selectivity,low production rates,and competition against the hydrogen evolution reaction hinder its practical implementation.To address these,the design of highly active catalysts is critical.Single-atom catalysts(SACs)have shown great potential because of their maximized atom utilization,but their limited stability and low metal loading restrict their performances.On the other hand,dual-atom catalysts(DACs)are atomic catalysts with two metal atoms nearby and offer enhanced electrocatalytic performances by aligning with the N≡N bond to enhance N2 reduction efficiency,potentially overcoming the limitations of SAC.This review discusses recent advances in SACs and more importantly DACs for ENRR,highlighting their advantages,limitations,and the need for advanced characterization techniques to better understand catalyst behavior.The review concludes by underscoring the importance of research to optimize these catalysts for efficient and sustainable nitrogen fixation. 展开更多
关键词 Single atom catalyst Dual atom catalyst Nitrogen fixation ENRR AMMONIA
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Regio-and enantioselective hydrofluorination of internal alkenes via nickel-catalyzed hydrogen atom transfer
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作者 Fan Chen Xiaoyu Zhao +3 位作者 Weihang Miao Yingying Li Ye Yuan Lingling Chu 《Chinese Chemical Letters》 2025年第5期237-242,共6页
Here we present a highly efficient protocol utilizing nickel-hydride hydrogen atom transfer catalysis for the regio-and enantioselective hydrofluorination of internal alkenes.This method efficiently assembles a wide a... Here we present a highly efficient protocol utilizing nickel-hydride hydrogen atom transfer catalysis for the regio-and enantioselective hydrofluorination of internal alkenes.This method efficiently assembles a wide array of enantioenrichedβ-fluoro amides with excellent regio-and enantioselectivity from internal unactivated alkenes.Mechanistic investigations suggest that this transformation proceeds via a NiHhydrogen atom transfer to alkene,followed by a stereoselective fluorine atom transfer process.The weak coordination effect of the tethered amide group is identified as a crucial factor governing the observed regio-and enantioselectivity. 展开更多
关键词 ALKENES HYDROFLUORINATION Hydrogen atom transfer Fluorine atom transfer Nickel catalysis
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Atomic Mass Engineering of Ultra-High Thermal Conductivity in Large Bandgap Materials:A Case Study with Boron Arsenide
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作者 Tingting Wang Xiaozhe Li +4 位作者 Zhuo Ju Gang Zhang Dengke Ma Wu Li Lifa Zhang 《Chinese Physics Letters》 2025年第7期454-466,共13页
Heat dissipation highly relies on the thermal conductivity(κ)of materials.Materials with large bandgaps and signifcant atomic mass ratios,such as BAs,SiC,andθ-TaN,have attracted considerable attention due to their p... Heat dissipation highly relies on the thermal conductivity(κ)of materials.Materials with large bandgaps and signifcant atomic mass ratios,such as BAs,SiC,andθ-TaN,have attracted considerable attention due to their potential for achieving ultra-highκ,with BAs serving as a particularly representative example due to its unique combination of large bandgap and high thermal conductivity.In this paper,the efects of atomic mass modifcation on phonon bandgap andκare systematically investigated using a BAs model,accounting for both three-and four-phonon scattering processes.A 20%increase inκcan be obtained by substituting B,achieved through widening the phonon bandgap,which suppresses phonon scattering.Notably,the AAOO four-phonon scattering channel is more suppressed than the AAO three-phonon channel,leading to an increased phonon lifetime(τ).For As,κcan also be enhanced by 5%when replaced by lighter atoms,such as^(69)As,primarily due to the increased phonon group velocity(υ).We systematically clarify how atomic-mass-induced bandgap variations afectτ,υ,and thereforeκin wide-bandgap systems.Our work provides a specifc scheme for further improving the ultra-highκof materials with large bandgaps,which possesses great guiding signifcance. 展开更多
关键词 phonon bandgap phonon lifetime phonon scattering thermal conductivity atomic mass modifcation group velocity atomic mass engineering heat dissipation
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Cavity-Enhanced Rydberg Atom Microwave Receiver
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作者 Bang Liu Li-Hua Zhang +11 位作者 Qi-Feng Wang Yu Ma Tian-Yu Han Zong-Kai Liu Zheng-Yuan Zhang Shi-Yao Shao Jun Zhang Qing Li Han-Chao Chen Yu-Long Han Dong-Sheng Ding Bao-Sen Shi 《Chinese Physics Letters》 2025年第5期7-11,共5页
Developing microwave electric field sensing based on Rydberg atoms has received significant attention due to its unique advantages. However, achieving effective coupling between Rydberg atoms and the microwave electri... Developing microwave electric field sensing based on Rydberg atoms has received significant attention due to its unique advantages. However, achieving effective coupling between Rydberg atoms and the microwave electric field in the sensing process is a challenging problem that greatly impacts the sensitivity. To address this, we propose using a microwave resonant cavity to enhance the effective coupling between the Rydberg atoms and the microwave electric field. In our experiment, Rydberg atoms are prepared via a three-photon excitation scheme, and the electric fields are measured without and with a microwave cavity in which the vapor cell is placed inside, respectively. As a result, we achieved an 18 dB enhancement of power sensitivity by adding the cavity,which is an effective enhancement in electric field pulse signal detection. This experimental testing provides a promising direction for enhancing the sensitivity of Rydberg atomic electric field sensors and paves the way for their application in precision electric field measurements. 展开更多
关键词 rydberg atoms enhance effective coupling microwave electric field cavity enhanced microwave electric field sensing sensing process microwave resonant cavity Rydberg atoms
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In-situ SEIRAS for dynamic single-atom catalysis
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作者 Haifeng Qi Graham J.Hutchings 《Chinese Journal of Catalysis》 2025年第10期1-3,共3页
Single-atom catalysis has revolutionized heterogeneous catalysis,which offers unparalleled atomic efficiency,well-defined active sites,and unique electronic properties.Unlike traditional nanoparticle catalysts,single-... Single-atom catalysis has revolutionized heterogeneous catalysis,which offers unparalleled atomic efficiency,well-defined active sites,and unique electronic properties.Unlike traditional nanoparticle catalysts,single-atom catalysts(SACs)maximize metal utilization and exhibit distinct catalytic behaviors due to their atomically dispersed nature.Over the past decade,SACs have demonstrated exceptional performance in various electrochemical and thermocatalytic reactions[1–3].However,despite these promising developments,several fundamental challenges hinder their practical implementation and large-scale commercialization.SACs face three major challenges:catalytic activity,stability,and scalable synthesis.Their isolated nature limits multi-electron transfer processes,making reaction kinetics highly sensitive to the coordination environment.To enhance catalytic activity,strategies such as secondary coordination effect,doping,and/or dual-atom configuration can be employed.Stability is another key issue,as single atoms tend to aggregate or undergo oxidation under reaction conditions,leading to performance decay.Strategies like strong metal-support interaction and ligand stabilization can be adopted to improve the durability of SACs. 展开更多
关键词 single atom catalysts catalytic activity heterogeneous catalysiswhich scalable synthesis electrochemical thermocatalytic reactions howeverdespite coordination environment nanoparticle catalystssingle atom strong metal support interaction
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Martian atmosphere sputtering escape generated by penetrating hydrogen energetic neutral atoms
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作者 JiJie Ma LingGao Kong +13 位作者 Hao Gu WenYa Li YuMing Wang YuTian Chi BinBin Tang XiaoPeng Liu YiFan Song BaiQu Pu FuHao Qiao LiMin Wang Jun Cui Yong Wei AiBing Zhang Chi Wang 《Earth and Planetary Physics》 2025年第6期1147-1156,共10页
Atmospheric escape plays a critical role in shaping the long-term climate evolution of Mars.Among the various escape mechanisms,energetic neutral atoms(ENAs)generated through charge exchange between solar wind ions an... Atmospheric escape plays a critical role in shaping the long-term climate evolution of Mars.Among the various escape mechanisms,energetic neutral atoms(ENAs)generated through charge exchange between solar wind ions and exospheric neutrals serve as an important diagnostic for ion-neutral interactions and upper atmospheric loss.This study presents direct observations of hydrogen ENAs(H-ENAs)on the dayside of Mars by using the Mars Ion and Neutral Particle Analyzer(MINPA)onboard China’s Tianwen-1 orbiter.By analyzing H-ENA data during a coronal mass ejection and a stream interaction region from December 29,2021,to January 1,2022,and comparing these data with MAVEN/SWIA(Mars Atmosphere and Volatile EvolutioN/Solar Wind Ion Analyzer)solar wind measurements,we examine the temporal evolution of H-ENA flux and the associated sputtered escape of atmospheric constituents.The observed H-ENA velocity is consistent with upstream solar wind ions,and the H-ENA-to-ion intensity ratio is used to infer variations in exospheric density,revealing a delayed response to enhanced solar wind activity.Penetrating H-ENA intensities reach up to 5.3×10^(6)s^(−1) cm^(−2),with energy fluxes on the order of(0.5-8.1)×10^(−3) mW/m^(2).The estimated oxygen sputtered escape rate driven by penetrating H-ENAs ranges from 5.5×10^(23)s^(−1) to 5.2×10^(24)s^(−1),comparable to or exceeding previous estimates based on penetrating ions.The findings highlight the need for low-altitude H-ENA observations to better quantify their atmospheric interactions and refine our understanding of nonthermal escape processes at Mars. 展开更多
关键词 penetrating energetic neutral atoms sputtered escape Mars atmosphere loss Tianwen-1 future energetic neutral atom observations
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Compact Cold-Atom Platform Based on Optical Grating and Planar Coil Chips
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作者 Chang-Jiang Huang Lei Xu +4 位作者 Liang Chen Chuan-Feng Li Guang-Can Guo Chang-Ling Zou Guo-Yong Xiang 《Chinese Physics Letters》 2025年第6期58-62,共5页
We present a compact cold atom platform where an optical grating chip and planar coil chip are placed inside a compact vacuum chamber to create a magneto-optical trap.This approach significantly reduces the system vol... We present a compact cold atom platform where an optical grating chip and planar coil chip are placed inside a compact vacuum chamber to create a magneto-optical trap.This approach significantly reduces the system volume to about 20×20×20 cm^(3) compared to conventional vacuum systems and offers greater flexibility in accessing the trapped atoms.We demonstrate the trapping of 3×10^(5) cold rubidium atoms at a temperature of 100μK in a vacuum pressure below 10^(−7) mbar.The simplified optical geometry,low power consumption,and high degree of integration make this a promising platform for portable and versatile cold-atom devices in quantum sensing,timing,and information processing. 展开更多
关键词 optical grating chip conventional vacuum systems planar coil chip rubidium atoms compact cold atom platform compact vacuum chamber
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Engineering atomic Rb-N configurations to tune radical pathways for highly selective photocatalytic H_(2)O_(2) synthesis coupled with biomass valorization
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作者 Jiaye Li Shuang Pan +1 位作者 Yihuang Chen Qiong Liu 《Journal of Energy Chemistry》 2025年第1期215-225,共11页
Photocatalytic oxygen reduction for hydrogen peroxide(H_(2)O_(2))synthesis presents a green and costeffective production method.However,achieving highly selective H_(2)O_(2)synthesis remains challenging,necessitating ... Photocatalytic oxygen reduction for hydrogen peroxide(H_(2)O_(2))synthesis presents a green and costeffective production method.However,achieving highly selective H_(2)O_(2)synthesis remains challenging,necessitating precise control over free radical reaction pathways and minimizing undesirable oxidative by-products.Herein,we report for the visible light-driven simultaneous co-photocatalytic reduction of O2to H_(2)O_(2)and oxidation of biomass using the atomic rubidium-nitride modified carbon nitride(CNRb).The optimized CNRb catalyst demonstrates a record photoreduction rate of 8.01 mM h^(-1)for H_(2)O_(2)generation and photooxidation rate of 3.75 mM h^(-1)for furfuryl alcohol to furoic acid,achieving a remarkable solar-to-chemical conversion(SCC)efficiency of up to 2.27%.Experimental characterizations and DFT calculation disclosed that the introducing atomic Rb–N configurations allows for the high-selective generation of superoxide radicals while suppressing hydroxyl free radical formation.This is because the Rb–N serves as the new alternative site to perceive a stronger connection position for O2adsorption and reinforce the capability to extract protons,thereby triggering a high selective redox product formation.This study holds great potential in precisely regulating reactive radical processes at the atomic level,thereby paving the way for efficient synthesis of H_(2)O_(2)coupled with biomass valorization. 展开更多
关键词 atomic economy Radical pathway regulation Photocatalytic H_(2)O_(2)synthesis Rubidium atom coordination Biomass valorization
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“One stone, two birds”: Salt template enabling porosity engineering and single metal atom coordinating toward high-performance zinc-ion capacitors
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作者 Chunliu Zhu Huanyu Liang +7 位作者 Ping Li Chenglong Qiu Jingyi Wu Jingwei Chen Weiqian Tian Yue Zhu Zhi Li Huanlei Wang 《Journal of Energy Chemistry》 2025年第1期637-645,共9页
Zinc-ion hybrid capacitors (ZIHCs) have received increasing attention as energy storage devices owing to their low cost,high safety,and environmental friendliness.However,their progress has been hampered by low energy... Zinc-ion hybrid capacitors (ZIHCs) have received increasing attention as energy storage devices owing to their low cost,high safety,and environmental friendliness.However,their progress has been hampered by low energy and power density,as well as unsatisfactory long-cycle stability,mainly due to the lack of suitable electrode materials.In this context,we have developed manganese single atoms implanted in nitrogen-doped porous carbon nanosheets (MnSAs/NCNs) using a metal salt template method as cathodes for ZIHCs.The metal salt serves a dual purpose in the synthesis process:It facilitates the uniform dispersion of Mn atoms within the carbon matrix and acts as an activating agent to create the porous structure.When applied in ZIHCs,the MnSAs/NCNs electrode demonstrates exceptional performance,including a high capacity of 203 m Ah g^(-1),an energy density of 138 Wh kg^(-1)at 68 W kg^(-1),and excellent cycle stability with 91%retention over 10,000 cycles.Theoretical calculations indicate that the introduced Mn atoms modulate the local charge distribution of carbon materials,thereby improving the electrochemical property.This work demonstrates the significant potential of carbon materials with metal atoms in zinc-ion hybrid capacitors,not only in enhancing electrochemical performance but also in providing new insights and methods for developing high-performance energy storage devices. 展开更多
关键词 Zinc ion hybrid capacitors Cathodes Carbon materials HETEROatomS Single atoms
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Proximity defect inductive effect of atomic Ni-N_(3) sites by Te atoms doping for efficient oxygen reduction and hydrogen evolution
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作者 Min Li Xiuhui Zheng +3 位作者 Han Guo Xiang Feng Yunqi Liu Yuan Pan 《Journal of Energy Chemistry》 2025年第7期446-454,共9页
The development of single atom catalysts(SACs)with asymmetric active sites by defect regulation provides an encourage potential for oxygen reduction reaction(ORR)and hydrogen evolution reaction(HER),but highly challen... The development of single atom catalysts(SACs)with asymmetric active sites by defect regulation provides an encourage potential for oxygen reduction reaction(ORR)and hydrogen evolution reaction(HER),but highly challenging.Herein,N-doped carbon(N-C)anchored atomically dispersed Ni-N_(3)site with proximity defects(Ni-N_(3)D)induced by Te atoms doping is reported.Benefitting from the inductive effect of proximity defect,the Ni-N_(3)D/Te-N-C catalyst performs excellent ORR and HER performance in alkaline and acid condition.Both in situ characterization and theoretical calculation reveal that the existence of proximity defect effect is conducive to lower rate-determining-step energy barrier of ORR and HER,thus accelerating the multielectron reaction kinetics.This work paves a novel strategy for constructing highactivity bifunctional SACs by defect engineering for development of sustainable energy. 展开更多
关键词 Proximity defect engineering Single atom catalyst Heteroatom doping Oxygen reduction reaction Hydrogen evolution reaction
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Single-atomic Fe sites modulated by Sn regulator for enhanced electrochemical CO_(2)reduction
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作者 Chenghong Hu Yue Zhang +4 位作者 Yi Zhang Qintong Huang Kui Shen Liyu Chen Yingwei Li 《Chinese Journal of Catalysis》 2025年第5期222-229,共8页
Single-atom Fe catalysts show significant promise in the electrocatalytic reduction of CO_(2)(CO_(2)RR),while their performance remains inferior to that of precious metal catalysts due to the overly strong binding of^... Single-atom Fe catalysts show significant promise in the electrocatalytic reduction of CO_(2)(CO_(2)RR),while their performance remains inferior to that of precious metal catalysts due to the overly strong binding of^(*)CO intermediates.Although the introduction of heteroatoms or transition metal sites can modulate the binding strength of^(*)CO on Fe sites,these regulators often induce competitive hydrogen evolution reaction(HER)with reduced Faraday efficiency(FE).In this work,we employ HER-inert Sn as a regulator to tune the electronic structure of Fe,weakening^(*)CO adsorption and enhancing CO_(2)RR performance.Diatomic Fe-Sn pairs supported on N-doped carbon(Fe-Sn/NC)were synthesized,achieving FE for CO exceeding 90%over a broad potential range from−0.4 to−0.9 V versus the reversible hydrogen electrode.Fe-Sn/NC shows a high turnover frequency of 1.5×10^(4)h^(-1),much higher than that of Fe/NC.Characterization results and theoretical calculations demonstrate that bonding Sn site to Fe generates electron-rich Fe centers,effectively reducing the adsorption strength of^(*)CO without triggering HER.Additionally,Fe-Sn/NC exhibits exceptional activity in hydrazine oxidation performance(HzOR).The HzOR-assisted CO_(2)RR system using Fe-Sn/NC as electrodes reduces energy consumption by 38%compared with the conventional CO_(2)RR coupled oxygen evolution reaction system. 展开更多
关键词 atomically dispersed catalyst Electrochemical CO_(2)reduction Electronic modification Diatomic pairs Main-group element
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Single-atomic iron synergistic atom-cluster induce remote enhancement toward oxygen reduction reaction
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作者 Yayin Li Haomin Jiang +2 位作者 Liu Lin Zemin Sun Genban Sun 《Journal of Energy Chemistry》 2025年第3期413-420,共8页
The oxygen reduction reaction(ORR)could be effectively regulated by adjusting electron configurations and optimizing chemical bonds.Herein,we have achieved the modulation of electron distribution in Fe single atomic(F... The oxygen reduction reaction(ORR)could be effectively regulated by adjusting electron configurations and optimizing chemical bonds.Herein,we have achieved the modulation of electron distribution in Fe single atomic(Fe_(SA))sites through Fe atomic clusters(Fe_(AC))via a confined pyrolysis approach,thereby enhancing their intrinsic ORR activity.X-ray absorption spectroscopy has confirmed that the presence of iron atomic dusters could influence the electron distribution at Fe-N_(4)sites.The Fe_(SA)/Fe_(AC)-NC catalyst exhibits a half-wave potential of 0.88 V,surpassing the individual Fe_(SA)-NC structure.Through electronic structure analysis,it could be seen that iron atom clusters can affect Fe-N_(4)sites through long-range effects,and then effectively lower reaction barriers and enhance the reaction kinetics at Fe-N_(4)sites.The synthetic approach might pave the way for constructing highly active catalysts with tunable atomic structures,representing an effective and universal technique for electron modulation in M-N-C systems.This work provides enlightenment for the exploration of more efficient single-atom electrocatalysts and the optimization of the performance of atomic electrocatalysts.Furthermore,a zinc-air battery assembled using it on their cathode deliver a high peak power density(205.7 mW cm^(-2))and a high-specific capacity of 807.5 mA h g^(-1).This study offers a fresh approach to effectively enhance the synergistic interaction of between Fe single atom and Fe atomic clusters for improving ORR activity and energy storage. 展开更多
关键词 Single atomic catalysts atom-cluster induce effect Oxygen reduction reaction Fe-N4 sites
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Atomic-scale investigation on the evolution of T_(1) precipitates in an aged Al-Cu-Li-Mg-Ag alloy 被引量:1
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作者 Xinyue Zhao Juan Ding +2 位作者 Daihong Xiao Lanping Huang Wensheng Liu 《Journal of Materials Science & Technology》 2025年第6期139-148,共10页
The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the compl... The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the complex precipitation sequences.Here,a detailed investigation has been carried out on the atomic struc-tural evolution of T_(1) precipitate in an aged Al-Cu-Li-Mg-Ag alloy using state-of-the-art Cs-corrected high-angle annular dark field(HAADF)-coupled with integrated differential phase contrast(iDPC)-scanning transmission electron microscopy(STEM)and energy-dispersive X-ray spectroscopy(EDXS)techniques.An intermediate T_(1)’phase between T_(1p) and T_(1) phase,with a crystal structure and orientation rela-tionship consistent with T_(1),but exhibiting different atomic occupancy and chemical composition was found.We observed the atomic structural transformation from T_(1p) to T_(1)’phase(fcc→hcp),involving only 1/12<112>Al shear component.DFT calculation results validated our proposed structural models and the precipitation sequence.Besides,the distributions of minor solute elements(Ag,Mg,and Zn)in the pre-cipitates exhibited significant differences.These findings may contribute to a further understanding of the nucleation mechanism of T_(1) precipitate. 展开更多
关键词 PRECIPITATE Chemical composition atomic structure Aluminium alloy STEM
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Boosting bidirectional sulfur conversion enabled by introducing boron-doped atoms and phosphorus vacancies in Ni_(2)P for lithium-sulfur batteries 被引量:1
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作者 Lin Peng Yu Bai +3 位作者 Hang Li Meixiu Qu Zhenhua Wang Kening Sun 《Journal of Energy Chemistry》 2025年第1期760-769,共10页
Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish ... Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion. 展开更多
关键词 B-doped atoms P vacancies Nickel phosphide Bidirectional sulfur conversion Lithium-sulfur batteries
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Biomass-derived single atom catalysts with phosphorus-coordinated Fe-N_(3)P configuration for efficient oxygen reduction reaction 被引量:1
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作者 Peng-Peng Guo Abrar Qadir +6 位作者 Chao Xu Kun-Zu Yang Yong-Zhi Su Xin Liu Ping-Jie Wei Qinggang He Jin-Gang Liu 《Green Energy & Environment》 2025年第5期1064-1072,共9页
Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-perform... Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion. 展开更多
关键词 Oxygen reduction reaction Biomass-derived electrocatalyst Single atom catalyst Phosphorus dopant Zn-air battery
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Rare Earth Oxide Surface Modification of Porous SiO_(2) Film Prepared by Atomic Layer Deposition
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作者 JIN Jianfei LÜLin +3 位作者 LI Ying YAN Lu CAO Yunzhen LI Wei 《无机材料学报》 北大核心 2025年第9期1029-1036,I0003,共9页
Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous Si... Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous SiO_(2) refractive index gradient anti-reflective film prepared by atomic layer deposition(ALD).A porous SiO_(2) film with gradual porosity was obtained by phosphoric acid etching of Al_(2)O_(3)/SiO_(2) multilayers with gradient Al2O3 ratios,achieving a gradual decrease in refractive index from the substrate to the surface.The film exhibited an average transmittance as high as 97.8%within the wavelength range from 320 nm to 1200 nm.The environmental adaptability was further enhanced by surface modification using rare earth oxide(REO)La_(2)O_(3),resulting in formation of a lotus leaf-like structure and achieving a water contact angle of 100.0°.These data proved that the modification significantly improved hydrophobic self-cleaning capability while maintaining exceptional transparency of the film.The surface structure of the modified film remained undamaged even after undergoing wipe testing,demonstrating its excellent surface durability. 展开更多
关键词 porous SiO_(2) rare earth oxide atomic layer deposition anti-reflective SELF-CLEANING
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