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Assembling atomically dispersed tungsten co-catalysts on organometal halide perovskite for superior interfacial charge transfer and photocatalytic hydrogen production 认领 引用
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作者 Ting Xu Zexi Zhang +7 位作者 Shengliang Qi Hefeng Zhang Junhui Wang Yuying Gao Wenjun Fan Chenghua Sun Xu Zong Lianzhou Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第5期525-534,I0013,共10页
Intensifying the electronic metal-support interaction(EMSI)between organometal halide perovskites(OMHPs)photocatalysts and hydrogen evolution reaction(HER)co-catalyst is crucial for realizing efficient interfacial cha... Intensifying the electronic metal-support interaction(EMSI)between organometal halide perovskites(OMHPs)photocatalysts and hydrogen evolution reaction(HER)co-catalyst is crucial for realizing efficient interfacial charge transfer and solar-to-hydrogen(STH)conversion.Although atomically dispersed catalysts(ADCs)are prone to form stronger EMSI than nanoparticles with support,assembling ADCs on OMHPs remains a great challenge due to the ionic nature and thermal instability of OMHPs.Herein,we realize the design of two-dimensional(2D)OMHPP)loaded with nonnoble metal-based ADCs,namely tungsten ADCs(WADCs),for the first time.We show that WADCscoordinated with two sulfur and two oxygen atoms are anchored on the surface of PMA2PbI4via a W-O-Pb link.The resulting WADCs-decorated PMA2PbI4(WADCs/S-PMA2PbI4)exhibits an extraordinary interfacial charge transfer efficiency of 94.7%,which is much higher than that of Pt/PMA2PbI4(61.7%).Moreover,WADCscan effectively extend the lifetime of hot carriers and work as the active sites for HER.Consequently,WADCs/S-PMA2PbI4shows a photocatalytic HER activity superior to that of Pt/PMA2PbI4and 30 times that of bare PMA2PbI4with a record turnover frequency(TOF)of 516.3 h-1per W atom.This work opens a new avenue for designing cost-effective perovskite-based catalysts for solar hydrogen production. 展开更多
关键词 Atomically dispersed catalysts Organometal halide perovskites Photocatalytichydrogen production Co-catalyst Non-noble metal
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Atomically Dispersed Pt-Ru Dual-Atom Catalysts for Efficient Low-Temperature CO Oxidation Reaction 认领 引用 被引量：1
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作者 Yanan Qi Hongqiu Chen +12 位作者 Feng Hong Xiangbin Cai Zhehan Ying Jiangyong Diao Zhimin Jia Jiawei Chen Ning Wang Shengling Xiang Xiaowen Chen Guodong Wen Bo Sun Geng Sun Hongyang Liu 《Nano-Micro Letters》 SCIE EI CAS CSCD 2026年第5期816-830,共15页
Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the effica... Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10-2s-1at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10-2s-1)and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O2,and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale. 展开更多
关键词 CO oxidation Atomically dispersed Dual-atom catalysts Pt-Ru Synergistic effect
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Template-Assisted Construction of Atomically Dispersed Fe-N-C Catalysts With Dense Fe-N4C Sites for Enhanced Oxygen Reduction Reaction 认领 引用
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作者 Lijuan Wang Jie Hou +4 位作者 Wubo Wan Yongjie Mo Zhijian Liao Shengkui Zhong Linhua Zhu 《Rare Metals》 SCIE EI CAS CSCD 2026年第5期810-821,共12页
Atomically dispersed iron-nitrogen-carbon(Fe-N-C)catalysts have emerged as promising alternatives for oxygen reduction reaction(ORR)owing to their highly atomic utilization.However,maintaining both Fe atomic dispersio... Atomically dispersed iron-nitrogen-carbon(Fe-N-C)catalysts have emerged as promising alternatives for oxygen reduction reaction(ORR)owing to their highly atomic utilization.However,maintaining both Fe atomic dispersion and dense Fe-Nx sites(typically below 2 wt%)in Fe-N-C catalysts is still a key challenge.In this investigation,a template(1,2-dicyanobenzene;DCB)assisted strategy has been reported to achieve hierarchically porous Fe-N/CDCB0.2-900℃catalysts,which have atomically dispersed Fe-N4C active sites with a 5.45 wt%Fe loading and served for robust ORR.1,2-dicyanobenzene containing abundant nitrogen source not only efficiently enhances the coordinated environment for dense Fe sites,but also facilitates the formation of a hierarchical porous structure in Fe-N/CDCBO.2-900℃catalyst.Computational analysis demonstrated that template-assisted structural modification effectively reduces the energy barrier associated with*OOH intermediate formation while simultaneously adjusting the d-band center position of Fe-N4C coordination sites within the Fe-N/CDCB0.2-900℃system.This optimization enhances the stabilization of oxygen-bearing intermediates and promotes accelerated kinetics of the ORR.Consequently,the Fe-N/CDCB0.2-900℃exhibited a half-potential of 0.9 V versus RHE when evaluated in 0.1 M KOH electrolyte and achieved a peak power density of 220 mW cm-2 in a zinc-air battery,surpassing commercial Pt/C(0.88 V vs.RHE,194 mW cm-2).Such methodology provides a new avenue for constructing dense metal active sites for achieving functional,but not limited to,ORR,catalysts and applications. 展开更多
关键词 atomically dispersed dense Fe-Nx sites Fe-N-C catalysts oxygen reduction reaction template-assisted synthesis
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Atomically dispersed copper catalysts with dual reaction sites and high mass transfer efficiency for highly-efficient Fenton-like degradation 认领 引用
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作者 Haiyang Xie Yiming Liu +5 位作者 Yuhan Chen Yaolong Chen Yanjuan Zhang Zuqiang Huang Huayu Hu Tao Gan 《ENGINEERING Environment》 SCIE EI CAS CSCD 2026年第1期143-155,共13页
Atomically dispersed metal catalysts(ADMCs)with dual reaction sites have been extensively utilized in permonosulfate(PMS)-based Fenton-like systems for the degradation of antibiotic wastewater,yet challenges remain in... Atomically dispersed metal catalysts(ADMCs)with dual reaction sites have been extensively utilized in permonosulfate(PMS)-based Fenton-like systems for the degradation of antibiotic wastewater,yet challenges remain in synthesizing cost-effective and highly active Cu-based catalysts.Herein,atomically dispersed Cu catalysts supported on N-doped cellulose-derived carbon(Cu1/NC-700)are synthesized via a sol-gel combined with high-temperature pyrolysis method.The formed Cu?Nx and pyrrolic N dual reaction sites enhance the activation of PMS and adsorption of oxytetracycline(OTC),thereby shortening the migration distance of radicals towards the OTC.Moreover,graphitic N accelerates electron transfer to facilitate the Cu2+/Cu+cycle for the generation of highly efficient active species,including?OH,1O2,SO4??,and O2??.The Cu1/NC-700 exhibits significant catalytic activity for the degradation of OTC,achieving 96.6%degradation efficiency within 60 min at an initial substrate concentration of 50 mg/L,a high turnover frequency(0.279/min)and apparent rate constant(0.0827/min),which markedly surpassed those of Cu1/NC-600,Cu1/NC-800,and CuNPs/NC.The results of chemical quenching experiments,electron paramagnetic resonance,and electrochemical analysis show that 1O2-dominated non-radical pathway is the main mechanism rather than the radical pathway in the Cu1/NC-700+PMS+OTC system.This work presents a straightforward and cost-effective strategy for the synthesis of ADMCs for the treatment of tetracyclines wastewater. 展开更多
关键词 Atomically dispersed metal catalysts Dual reactive sites Sol-gel method Cellulosederived porous carbon Mass transfer efficiency
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Atomically Dispersed Platinum Sites Immobilized on NiFe LDH by Controlling Localized Amorphization for Efficient Alkaline Electrocatalytic Hydrogen Evolution 认领 引用
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作者 Yanhui Song Xiaohui Zhao +7 位作者 Zixuan Wang Guodong An Ziqi Wang Yi Zhang Yongqing Shen Peizhi Liu Hai Li Junjie Guo 《Rare Metals》 SCIE EI CAS CSCD 2026年第6期706-716,共11页
Platinum(Pt)single‐atom catalyst(SAC)shows great promise for hydrogen evolution reaction(HER),but faces a huge challenge in activity enhancement due to the isolated single‐atom sites.Fabricating support with partial... Platinum(Pt)single‐atom catalyst(SAC)shows great promise for hydrogen evolution reaction(HER),but faces a huge challenge in activity enhancement due to the isolated single‐atom sites.Fabricating support with partially amorphous(pa)structures to realize the synergetic interaction in neighboring single atoms could facilitate H2O dissociation and optimize H*adsorption.However,the electrocatalytic mechanism of SAC achieved by tailoring the different amorphous contents of the support has not been clearly explored yet.Herein,neighboring Pt SAs confined in NiFe LDH(Pt@pa‐NiFe LDH‐24)were successfully synthesized via a localized amorphization and impregnation strategy,resulting in significantly boosted HER performance.Experiments and calculations demonstrate that the Pt SAs can accelerate the adsorption/desorption of H2O and effectively promote the Volmer step of the partially amorphous substrate.Benefiting from this,the optimized Pt@pa‐NiFe LDH‐24 exhibits enhanced intrinsic activity,exhibiting a lower overpotential(η10:40 mV)than the commercial Pt/C catalyst.This partial amorphization strategy sheds new light on supporting noble metal single‐atom catalysts for designing efficient HER catalysts in water electrolysis. 展开更多
关键词 hydrogen evolution reaction layered double hydroxide partially amorphous Pt single atom
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Constructing Atomically Dispersed Bimetallic Electrocatalyst by a Topologically Confined Pre-Anchoring Strategy for Enhanced Oxygen Reduction Reaction and Zn-Air Battery 认领 引用
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作者 Yawei Zhang Xia Li Ziqian Xue 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2026年第1期257-262,共6页
The development of atomically dispersed multi-metallic catalysts is imperative for tailoring catalytic performance and elucidating structure-activity relationships.However,synthesizing such precisely engineered archit... The development of atomically dispersed multi-metallic catalysts is imperative for tailoring catalytic performance and elucidating structure-activity relationships.However,synthesizing such precisely engineered architectures while maintaining atomic dispersion of distinct metal centers remains a formidable challenge due to thermodynamic instability and synthetic complexity.We herein propose a topological confinement pre-anchoring strategy via pre-anchoring spatially resolved Zn/Fe dual-metal sources in a structurally engineered metal-organic framework precursor to synthesize atomically dispersed ZnFe bimetallic single-atom catalysts.Extended X-ray absorption fine structure measurements and X-ray absorption near-edge structure reveal that the atomically dispersed Zn/Fe metal sites and electronic redistribution in ZnFe bimetallic single-atom catalysts.The ultrahigh surface area,hierarchical pore,and synergistic effect between Zn/Fe can greatly favor the exposure of the active site,mass transport,and improvement of intrinsic activity.Consequently,the ZnFe bimetallic single-atom catalyst demonstrates superior oxygen reduction reaction performance,achieving a half-wave potential of 0.86 V and delivering a kinetic current density of 10.1 mA cm-2at 0.85 V versus RHE in 0.1 m KOH electrolyte.These metrics not only surpass those of commercial Pt/C,but also rival the highest-performing catalysts reported to date.The Zn-air battery built with ZnFe bimetallic single-atom catalyst exhibits high power density(278.5 mW cm-2)and specific discharging capacities(657 mAh g-1).This work provides a new design pathway for constructing atomically dispersed multi-metal electrocatalysts for high-performance energy-related applications. 展开更多
关键词 bimetallic single atom catalyst metal-organic frameworks oxygen reduction reaction Zn-air battery
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Atomically dispersed Fe-N4 sites on g-C3N4 enable highly selective CO2-to-CO electrocatalysis 认领 引用
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作者 Yongliang Ban Meng Zhang +4 位作者 Jianya He Chunfeng Shao Zhongliao Wang Wei Zhao Kai Dai 《Chinese Chemical Letters》 SCIE CAS CSCD 2026年第4期296-300,共5页
The development of efficient and cost-effective non-precious-metal single-atom catalysts(SACs)is crucial for advancing the practical application of electrocatalytic CO2 reduction(CO2RR).However,identifying highl... The development of efficient and cost-effective non-precious-metal single-atom catalysts(SACs)is crucial for advancing the practical application of electrocatalytic CO2 reduction(CO2RR).However,identifying highly active metal atoms and designing catalysts with uniform active center structures remain significant challenges.To address this,we developed a generic pyrolysis method to synthesize a series of transition metal-based SACs with atomically dispersed metal anchored on carbon nitride support(M-C3N4,M=Fe,Ni,Cu).Benefiting from the unique electronic structure of the Fe-N4 sites supported on C3N4,the Fe-C3N4 catalyst demonstrated exceptional performance,achieving a CO Faradaic efficiency of 99.6%and maintaining excellent stability.Theoretical calculations indicate that the Fe site exhibits a relatively stronger interaction with the*COOH intermediate,thereby helping to lower the energy barrier of the CO2 protonation process.This study provides valuable theoretical insights and practical synthesis strategies for designing high-performance non-precious-metal SACs for CO2RR. 展开更多
关键词 Electrocatalytic CO2reduction Single atom catalyst C3N4 Electron transfer Fe-N4sites
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Atomically Dispersed Precious-Metal Catalysts for Efficient H2O2 Electrosynthesis:Challenges and Opportunities 认领 引用
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作者 Hu Lingwei Hu Chunhong +1 位作者 Li Jitao Lu Shun 《分子催化（中英文）》 CAS CSCD 北大核心 2026年第4期552-569,I0006,共18页
The decentralized electrocatalytic production of hydrogen peroxide(H2O2)represents a sustainable,energyefficient alternative to the centralized,highly polluting anthraquinone process.While precious metals(e.g.,P... The decentralized electrocatalytic production of hydrogen peroxide(H2O2)represents a sustainable,energyefficient alternative to the centralized,highly polluting anthraquinone process.While precious metals(e.g.,Pt,Pd,Au,Ru,Ir)possess exceptional intrinsic electrocatalytic activity,their bulk and nanoparticulate forms typically suffer from poor selectivity toward the 2e−pathway due to contiguous active sites that facilitate O−O bond cleavage.The advent of atomically dispersed precious metal catalysts(ADPMCs),or single-atom catalysts,have revolutionized this field by completely isolating individual metal atoms.This geometric isolation intrinsically prevents the dual-site adsorption required for O−O scission,while precise tailoring of the metal's coordination environment enables rational modulation of the d-band center and the binding energy of the critical*OOH intermediate.This review comprehensively examines the thermodynamic principles and state-of-the-art developments of precious-metal SACs for both the cathodic 2e−oxygen reduction reaction and the anodic 2e−water oxidation reaction.We systematically evaluate the structure-property relationships of specific ADPMCs,highlighting the indispensable role of advanced operando characterization and density functional theory in unraveling reaction mechanisms.Finally,we outline the critical engineering bottlenecks impeding commercialization,specifically the paradoxical challenge of maximizing mass loading without triggering agglomeration and ensuring long-term stability under corrosive industrial conditions,and propose future directions including synergistic dual-atom catalysts,paired electrolysis configuration,and machine-learning-accelerated discovery. 展开更多
关键词 H2O2electrosynthesis oxygen reduction reaction water oxidation reaction atomically dispersed preciousmetal catalysts dual-atom catalysts
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Dye-stabilized atomically precise copper clusters for enhanced photocatalytic hydrogen evolution 认领 引用 被引量：1
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作者 Yan-Ling Li Yue Xu +2 位作者 Chen-Hong Wang Rui Wang Shuang-Quan Zang 《Chinese Chemical Letters》 SCIE CAS CSCD 2025年第10期318-322,共5页
Metal nanoclusters with well-defined atomic structures offer significant promise in the field of catalysis due to their sub-nanometer size and tunable organic-inorganic hybrid structural features.Herein,we successfull... Metal nanoclusters with well-defined atomic structures offer significant promise in the field of catalysis due to their sub-nanometer size and tunable organic-inorganic hybrid structural features.Herein,we successfully synthesized an 11-core copper(Ⅰ)-alkynyl nanocluster(Cu11),which is stabilized by alkynyl ligands derived from a photosensitive rhodamine dye molecule.Notably,this Cu11cluster exhibited excellent photocatalytic hydrogen evolution activity(8.13 mmol g-1h-1)even in the absence of a mediator and noble metal co-catalyst.Furthermore,when Cu11clusters were loaded onto the surface of TiO2nanosheets,the resultant Cu11@TiO2nanocomposites exhibited a significant enhancement in hydrogen evolution efficiency,which is 60 times higher than that of pure TiO2nanosheets.The incorporation of Cu11clusters within the Cu11@TiO2effectively inhibits the recombination of photogenerated electrons and holes,thereby accelerating the charge separation and migration in the composite material.This work introduces a novel perspective for designing highly active copper cluster-based photocatalysts. 展开更多
关键词 Copper cluster Atomically precise Nanocomposites Photoactive rhodamine-based ligand Photocatalytic hydrogen evolution
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Atomically Precise Cu Nanoclusters:Recent Advances,Challenges,and Perspectives in Synthesis and Catalytic Applications 认领 引用
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作者 Mengyao Chen Chengyu Guo +4 位作者 Lubing Qin Lei Wang Liang Qiao Kebin Chi Zhenghua Tang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2025年第4期130-165,共36页
Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalit... Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalities.Among that,Cu nanoclusters have been gaining continuous increasing research attentions,thanks to the low cost,diversified structures,and superior catalytic performance for various reactions.In this review,we first summarize the recent progress regarding the synthetic methods of atomically precise Cu nanoclusters and the coordination modes between Cu and several typical ligands and then discuss the catalytic applications of these Cu nanoclusters with some explicit examples to explain the atomical-level structure-performance relationship.Finally,the current challenges and future research perspectives with some critical thoughts are elaborated.We hope this review can not only provide a whole picture of the current advances regarding the synthesis and catalytic applications of atomically precise Cu nanoclusters,but also points out some future research visions in this rapidly booming field. 展开更多
关键词 Atomically precise Cu nanoclusters Controllable synthesis Catalytic applications Structure-performance relationship Challenges and perspectives
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Atomically dispersed Fe boosting elimination performance of g-C3N4 towards refractory sulfonic azo compounds via catalyst-contaminant interaction 认领 引用 被引量：3
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作者 Puying Liang Zhouping Wang +5 位作者 Shiyu Liao Yang Lou Jiawei Zhang Chengsi Pan Yongfa Zhu Jing Xu 《Advanced Powder Materials》 EI CAS CSCD 2025年第1期10-20,共11页
Herein,an oxygen-doped porous g-C3N4photocatalyst modified with atomically dispersed Fe(Fe1/OPCN)issuccessfully prepared and exhibits significant superiority in removing refractory sulfonic azo contaminants f... Herein,an oxygen-doped porous g-C3N4photocatalyst modified with atomically dispersed Fe(Fe1/OPCN)issuccessfully prepared and exhibits significant superiority in removing refractory sulfonic azo contaminants fromwater via catalyst-contaminant interaction.The elimination performance of Fe1/OPCN towards acid red 9,acidred 13 and amaranth containing similar azonaphthalene structure and increasing sulfonic acid groups increasesgradually.The amaranth degradation rate of Fe1/OPCN is 17.7 and 6.1 times as that of homogeneous Fenton andOPCN,respectively.In addition,Fe1/OPCN also has more outstanding removal activities towards other con-taminantswith sulfonic acid and azo groups alone.The considerable enhancement for removing sulfonic azocontaminants of Fe1/OPCN is mainly ascribed to the following aspects:(1)The modified Fe could enhance theadsorption towards sulfonic azo compounds to accelerate the mass transfer,act as e-acceptor to promoteinterfacial charge separation,and trigger the self-Fenton reaction to convert in-situ generated H2O2into·OH.(2)Fe(Ⅲ)could coordinate with-N=N-to form d-πconjugation,which could attract e-transfer to attack-N=N-bond.Meanwhile,the inhibited charge recombination could release more free hþto oxidize sulfonicacid groups into SO4-·.(3)Under the cooperation of abundant multiple active species(·O2-,hþ,e-,·OH,SO4-·)formed during the degradation reaction,sulfonic azo compounds could be completely mineralized into harmlesssmall molecules(CO2,H2O,etc.)by means of-N=N-cleavage,hydroxyl substitution,and aromatic ringopening.This work offers a novel approach for effectively eliminating refractory sulfonic azo compounds fromwastewater. 展开更多
关键词 g-C3N4photocatalyst Atomically dispersed Fe Sulfonic azo compounds Catalyst-contaminant interaction
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Single-atom catalysts supported on atomically thin materials for water splitting 认领 引用 被引量：1
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作者 Xiaomin Chen Ding Yuan +6 位作者 Chao Rong Chao Wu Porun Liu Hua Kun Liu Dingsheng Wang Shi Xue Dou Yuhai Dou 《Advanced Powder Materials》 EI CAS CSCD 2025年第5期83-97,共15页
Single-atom catalysts(SACs)have demonstrated exceptional performance in electrocatalytic water splitting,owing to their maximized atomic utilization efficiency and superior reaction kinetics.The incorporation of SACs ... Single-atom catalysts(SACs)have demonstrated exceptional performance in electrocatalytic water splitting,owing to their maximized atomic utilization efficiency and superior reaction kinetics.The incorporation of SACs typically depends on robust metal-support interactions,which stabilize the single atoms on the support through various unsaturated chemical sites or spatial confinement.A critical challenge lies in precisely modulating the electronic structure and coordination environment of metal atoms.However,current research primarily focuses on single-atom metals,often neglecting the significant role of support materials in SACs.Two-dimensional(2D)atomically thin materials(ATMs)possess unique physicochemical properties and tunable reaction environments,which can modulate catalytic performance via metal-support interactions,positioning them as promising platforms for SAC loading.This paper reviews the recent advancements and the current status of SACs supported on 2D ATMs(SACs@ATMs).The structural design theory and synthesis strategies of SACs@ATMs are systematically discussed.The significance of advanced characterization techniques in elucidating the coordination environment and metal-support interactions is highlighted.Additionally,the reaction mechanisms and applications of SACs in electrocatalytic water splitting are summarized.Finally,the future challenges and opportunities for SACs@ATMs are outlined.This paper aims to provide insights and guidance for the rational design of SACs@ATMs with high-performance electrocatalytic water splitting capabilities. 展开更多
关键词 Atomically thin materials Single-atom catalysts Structure regulation Coordination environment Electrochemical water splitting
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Specific Sn–O–Fe Active Sites from Atomically Sn‑Doping Porous Fe2O3for Ultrasensitive NO2Detection 认领 引用 被引量：1
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作者 Yihong Zhong Guotao Yuan +8 位作者 Dequan Bao Yi Tao Zhenqiu Gao Wei Zhao Shuo Li Yuting Yang Pingping Zhang Hao Zhang Xuhui Sun 《Nano-Micro Letters》 SCIE EI CAS CSCD 2025年第11期362-375,共14页
Conventional gas sensing materials(e.g.,metal oxides)suffer from deficient sensitivity and serve cross-sensitivity issues due to the lack of efficient adsorption sites.Herein,the heteroatom atomically doping strategy ... Conventional gas sensing materials(e.g.,metal oxides)suffer from deficient sensitivity and serve cross-sensitivity issues due to the lack of efficient adsorption sites.Herein,the heteroatom atomically doping strategy is demonstrated to significantly enhance the sensing performance of metal oxides-based gas sensing materials.Specifically,the Sn atoms were incorporated into porous Fe2O3in the form of atomically dispersed sites.As revealed by X-ray absorption spectroscopy and atomic-resolution scanning transmission electron microscopy,these Sn atoms successfully occupy the Fe sites in the Fe2O3lattice,forming the unique Sn-O-Fe sites.Compared to Fe-O-Fe sites(from bare Fe2O3)and Sn-O-Sn sites(from SnO2/Fe2O3with high Sn loading),the Sn-O-Fe sites on porous Fe2O3exhibit a superior sensitivity(Rg/Ra=2646.6)to 1 ppm NO2,along with dramatically increased selectivity and ultra-low limits of detection(10 ppb).Further theoretical calculations suggest that the strong adsorption of NO2on Sn-O-Fe sites(N atom on Sn site,O atom on Fe site)contributes a more efficient gas response,compared to NO2on Fe-O-Fe sites and other gases on Sn-O-Fe sites.Moreover,the incorporated Sn atoms reduce the bandgap of Fe2O3,not only facilitating the electron release but also increasing the NO2adsorption at a low working temperature(150°C).This work introduces an effective strategy to construct effective adsorption sites that show a unique response to specific gas molecules,potentially promoting the rational design of atomically modified gas sensing materials with high sensitivity and high selectivity. 展开更多
关键词 Atomically doping Specific Sn-O-Fe sites NO2detection Gas sensor Specific adsorption
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Structure and property evolution of atomically precise palladium clusters 认领 引用
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作者 Chang-Qing Meng Wan-Yu Cheng +6 位作者 Hao Yan Hui-Xin Xiang Chen-Hao Ruan Yue Zhao Cong-Qiao Xu Jun Li Chuan-Hao Yao 《Rare Metals》 SCIE EI CAS CSCD 2025年第4期2822-2829,共8页
Atomically precise palladium(Pd)clusters are emerging as versatile nanomaterials with applications in catalysis and biomedicine.This study explores the synthesis,structure evolution,and catalytic properties of Pd clus... Atomically precise palladium(Pd)clusters are emerging as versatile nanomaterials with applications in catalysis and biomedicine.This study explores the synthesis,structure evolution,and catalytic properties of Pd clusters stabilized by cyclohexanethiol(HSC6H11)ligands.Using electrospray ionization mass spectrometry(ESI-MS)and single-crystal X-ray diffraction(SXRD),structures of the Pd clusters ranging from Pd4(SC6H11)8 to Pd18(SC6H11)36 were determined.This analysis revealed a structure evolution from polygonal to elliptical geometries of the PdnS2n frameworks as the cluster size increased.UV-Vis-NIR spectroscopy,combined with quantum chemical calculations,elucidated changes in the electronic structure of the clusters.Catalytic studies on the Sonogashira cross-coupling reactions demonstrated a size-dependent decline in activity attributed to variations in structural arrangements and electronic properties.Mechanistic insights proposed a distinctive Pd(Ⅱ)-Pd(Ⅳ)catalytic cycle.This research underscores how ligands and cluster size influence the structures and properties of Pd clusters,offering valuable insights for the future design and application of Pd clusters in advanced catalysis and beyond. 展开更多
关键词 structure evolution catalytic properties quantum chemical calculations cyclohexanethiol ligands electrospray ionization mass spectrometry esi ms atomically precise palladium clusters sonogashira cross coupling reactions electronic structure
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Atomically dispersed Co sites on BiOCl nanosheets for efficient CO2photoreduction 认领 引用 被引量：1
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作者 Ting Peng Yiduo Wang +8 位作者 Ke Wang Kaini Zhang Yiqing Wang Yufei Xu Qingqing Guan Guofu Wang Wenjie Zhang Binglan Wu Shaohua Shen 《Green Energy & Environment》 SCIE EI CAS CSCD 2025年第9期1948-1955,共8页
Efficient CO2photoreduction to produce fuel remains a great challenge,due to the fast recombination of photogenerated charge carriers and the lack of effective reactive sites in the developed photocatalysts.Herein,... Efficient CO2photoreduction to produce fuel remains a great challenge,due to the fast recombination of photogenerated charge carriers and the lack of effective reactive sites in the developed photocatalysts.Herein,single Co atoms(CoSA)were highly dispersed on hydrothermally synthesized BiOCl nanosheets(BOC)by a facile two-step electrostatic self-assembly and pyrolysis method.The obtained CoSA-BOC could be performed for efficient CO2photoreduction to stoichiometrically produce CO and O2at the ratio of 2:1,with the CO evolution rate reaching 45.93 μmol g-1h-1,~4 times that of the pristine BOC.This distinctly improved photocatalytic performance for CoSA-BOC should benefit from the introduction of atomically dispersed Co–O4coordination structures,which could accelerate the migration of photogenerated charge carriers to surface by creating an impurity energy level in the forbidden band,and act as the reactive sites to deliver the photogenerated electrons to activate CO2molecules for CO production.This work provides a facile and reliable strategy to highly disperse single atoms on low-dimensional semiconductors for efficient CO2photoreduction to selectively produce CO. 展开更多
关键词 Photocatalysis CO2reduction BiOCl nanosheets Single Co atoms
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Atomically dispersed catalysts for formic acid oxidation reaction 认领 引用
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作者 Peizhu Xu Ziqi Zhang Lili Han 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第12期599-616,I0015,共18页
Formic acid holds great potential as a fuel for low-temperature proton-exchange membrane fuel cells and portable power devices because of its excellent safety profile and high energy density.However,formic acid oxidat... Formic acid holds great potential as a fuel for low-temperature proton-exchange membrane fuel cells and portable power devices because of its excellent safety profile and high energy density.However,formic acid oxidation reactions(FAOR)face challenges such as low catalytic activity,poor stability,and catalyst poisoning.Atomically dispersed catalysts(ADCs)address these issues by providing a direct oxidation pathway,inhibiting catalyst poisoning,and offering well-defined catalytic sites with ultimate atomic efficiency.This review provides a comprehensive summary of recent breakthroughs in ADCs for FAOR.First,we discuss the structural design and mechanism validation methods of ADCs using enhanced sensitivity,in situ/operando,and high-resolution techniques.Next,we summarize bottom-up optimization strategies for ADCs,guided by the structure-activity relationship and reaction mechanisms at the atomic and electronic levels.Finally,we offer insights into device design and scale-up efforts for FAOR applications and provide an overlook from fundamental catalyst design to practical applications. 展开更多
关键词 Formic acid oxidation reactions Atomically dispersed catalysts Structure-activity relationship Reaction mechanisms
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Atomically dispersed tungsten enhances CO tolerance in electrocatalytic hydrogen oxidation by regulating the 5d-orbital electrons of platinum 认领 引用 被引量：1
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作者 Xu Zhang Peng Yu +4 位作者 Di Shen Bin Cai Tianyu Han Ying Xie Lei Wang 《Advanced Powder Materials》 EI CAS CSCD 2025年第3期67-77,共11页
The susceptibility of Pt catalyst surfaces to carbon monoxide(CO)poisoning in anodic hydrogen oxidation reaction(HOR)has been a critical constraint on the development of proton exchange membrane fuel cells(PEMFCs).Eff... The susceptibility of Pt catalyst surfaces to carbon monoxide(CO)poisoning in anodic hydrogen oxidation reaction(HOR)has been a critical constraint on the development of proton exchange membrane fuel cells(PEMFCs).Effectively regulating the electronic structure of Pt to enhance CO resistance is crucial for developing high-performance catalysts with robust anti-poisoning capabilities.Herein,the Pt/W@NCNF featured by Pt nanoparticles and atomical dispersed tungsten(W)sites on N-doped carbon nanofibers is developed for CO tolerance HOR catalyst.The presence of W enables the electron transfer from Pt,which promotes electron rearrangement in the Pt-5d orbitals.It not only optimizes the adsorption of H* and CO*on Pt,but also the OH* intermediates adsorbed on the W sites oxidize the CO*adsorbed on Pt,thereby retaining more active sites for H2 adsorption and oxidation.The HOR exchange current density of Pt/W@NCNF reaches 1.35 times that of commercial Pt/C,and the limiting current density decreases by only 3.4%after introducing 1000 ppm CO in H2.Notably,the Pt/W@NCNF-based PEMFCs deliver markedly superior performance across a range of CO concentrations.The present study demonstrates that electronic modulation of Pt is an effective strategy for simultaneously achieving resistance to CO and promoted HOR activity. 展开更多
关键词 Modulation electron structure Atomical dispersed W sites Pt 5d-orbital Hydrogen oxidation reaction Anti-CO poisoning
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Atomically dispersed cobalt in MFI zeolite framework for sustainable propane dehydrogenation 认领 引用
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作者 Xiang Fu Jun Yu Weili Dai 《Chinese Journal of Structural Chemistry》 SCIE CAS CSCD 2025年第10期9-10,共2页
Propylene,a pivotal chemical feedstock,is extensively used in synthesizing high-value derivatives such as polypropylene and acrylonitrile[1].Although propylene is predominantly produced via naphtha cracking,a persiste... Propylene,a pivotal chemical feedstock,is extensively used in synthesizing high-value derivatives such as polypropylene and acrylonitrile[1].Although propylene is predominantly produced via naphtha cracking,a persistent supply-demand gap exists[2].Non-oil routes,such as propane dehydrogenation(PDH),are increasingly attractive,particularly with the availability of shale gas[3].Modern non-oxidative PDH heavily relies on Pt nanoparticle catalysts promoted with SnOx(e.g.,PtSn/Al2O3 used in Honeywell UOP's Oleflex process)[4].However,these systems suffer from inherent limitations:high Pt costs,coke formation via deep dehydrogenation,and sintering during regeneration-necessitating environmentally detrimental oxychlorination treatments to restore activity[5]. 展开更多
关键词 naphtha crackinga sustainable propane dehydrogenation propane dehydrogenation pdh shale gas modern pt nanoparticle catalysts honeywell uops oleflex atomically dispersed cobalt chemical feedstockis
Atomically dispersed Ru on flower-like In2O3 to boost CO2 hydrogenation to methanol 认领 引用 被引量：1
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作者 Mengyao Xu Fei Liu +4 位作者 Shike Liu Jun Ma Mengqin Yao Xiaodan Wang Jianxin Cao 《Journal of Materials Science & Technology》 SCIE EI CAS CSCD 2025年第18期289-301,共13页
Metal-based catalysts are prevalent in the CO2 hydrogenation to methanol owing to their remarkable catalytic activity.Herein,Ru/In2O3 catalysts with different morphologies obtained by doping Ru into In2O_(... Metal-based catalysts are prevalent in the CO2 hydrogenation to methanol owing to their remarkable catalytic activity.Herein,Ru/In2O3 catalysts with different morphologies obtained by doping Ru into In2O3 with irregular,rod-like,and flower-like morphologies are used for catalytic CO2 hydrogenation to methanol.Results indicate that the flower-like Ru/In2O3(Ru/In2O3-F)exhibits higher catalytic performance than Ru/In2O3 with other morphologies,achieving a 12.9%CO2 conversion,74.02%methanol selectivity,and 671.36 mgMeOH h−1 gcat−1 methanol spatiotemporal yield.Furthermore,Ru/In2O3-F maintains its catalytic stability over 200 h at 5 MPa and 290℃.The promotional effect mainly stems from the fact that electronic structure of Ru can be effectively adjusted by modulating the morphology of In2O3.The strong interaction between atomically dispersed Ru and In2O3-F enhances the structural stability of Ru,inhibiting the agglomeration of the catalyst during the reaction process.Furthermore,density-functional theory calculations reveal that highly dispersed Ru atoms not only perform efficient and rapid electronic gain and loss processes,facilitating the catalytic activation of H2 into H intermediates.It also enables the generated reactive H to rapidly overflow to the surrounding In sites to participate in CO2 reduction.These findings provide a theoretical basis for the development of high-performance catalysts for CO2 hydrogenation. 展开更多
关键词 CO2hydrogenation Methanol Morphology Atomic dispersion Ruthenium
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Atomically Dispersed Transition Metal-Nitrogen-Carbon Bifunctional Oxygen Electrocatalysts for Zinc-Air Batteries:Recent Advances and Future Perspectives 认领 引用 被引量：37
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作者 Fang Dong Mingjie Wu +4 位作者 Zhangsen Chen Xianhu Liu Gaixia Zhang Jinli Qiao Shuhui Sun 《Nano-Micro Letters》 SCIE EI CAS CSCD 2022年第2期257-281,共25页
Rechargeable zinc-air batteries(ZABs)are currently receiving extensive attention because of their extremely high theoretical specific energy density,low manufacturing costs,and environmental friendliness.Exploring bif... Rechargeable zinc-air batteries(ZABs)are currently receiving extensive attention because of their extremely high theoretical specific energy density,low manufacturing costs,and environmental friendliness.Exploring bifunctional catalysts with high activity and stability to overcome sluggish kinetics of oxygen reduction reaction and oxygen evolution reaction is critical for the development of rechargeable ZABs.Atomically dispersed metal-nitrogen-carbon(M-N-C)catalysts possessing prominent advantages of high metal atom utilization and electrocatalytic activity are promising candidates to promote oxygen electrocatalysis.In this work,general principles for designing atomically dispersed M-N-C are reviewed.Then,strategies aiming at enhancing the bifunctional catalytic activity and stability are presented.Finally,the challenges and perspectives of M-N-C bifunctional oxygen catalysts for ZABs are outlined.It is expected that this review will provide insights into the targeted optimization of atomically dispersed M-N-C catalysts in rechargeable ZABs. 展开更多
关键词 Atomically dispersed metal-nitrogen-carbon Oxygen evolution reaction(OER) Oxygen reduction reaction(ORR) Bifunctional oxygen electrocatalysts Zinc-air batteries(ZABs)
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