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Key role of electron accessibility at the noble metal-free catalytic interface in hydrogen evolution reaction

Nano Research 2024年第4期17卷 2538-2545页

作者： Dongchen Han Nanxing Gao Yuyi Chu Zhaoping Shi Ying Wang Junjie Ge meiling xiao Changpeng Liu Wei Xing State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The reactant concentration at the catalytic interface holds the key to the activity of electrocatalytic hydrogen evolution reaction(HER),mainly referring to the capacity of adsorbing hydrogen and electron accessibility.With hydrogen adsorption free energy(ΔGH)as a reactivity descriptor,the volcano curve based on Sabatier principle is established to evaluate the hydrogen evolution activity of catalysts.However,the role of electron as reactant received insufficient attention,especially for noble metal-free compound catalysts with poor conductivity,leading to cognitive gap between electronic conductivity and apparent catalytic activity.Herein we successfully construct a series of catalyst models with gradient conductivities by regulating molybdenum disulfide(MoS_(2))electronic bandgap via a simple solvothermal method.We demonstrate that the conductivity of catalysts greatly affects the overall catalytic activity.We further elucidate the key role of intrinsic conductivity of catalyst towards water electrolysis,mainly concentrating on the electron transport from electrode to catalyst,the electron accumulation process at the catalyst layer,and the charge transfer progress from catalyst to reactant.Theoretical and experimental evidence demonstrates that,with the enhancement in electron accessibility at the catalytic interface,the dominant parameter governing overall HER activity gradually converts from electron accessibility to combination of electron accessibility and hydrogen adsorbing energy.Our results provide the insight from various perspective for developing noble metal-free catalysts in electrocatalysis beyond HER.

关键词： conductivity molybdenum disulfide catalytic interface electron accessibility hydrogen evolution charge transfer.

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Suppressing the lattice oxygen diffusion via high-entropy oxide construction towards stabilized acidic water oxidation

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Nano Research 2024年第3期17卷 1107-1113页

作者： Jing Ni Zhaoping Shi Yibo Wang Jiahao Yang Hongxiang Wu Pengbo Wang Kai Li meiling xiao Changpeng Liu Wei Xing State Key Laboratory of Electroanalytic Chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The scale-up deployment of ruthenium(Ru)-based oxygen evolution reaction(OER)electrocatalysts in proton exchange membrane water electrolysis(PEMWE)is greatly restricted by the poor stability.As the lattice-oxygen-mediated mechanism(LOM)has been identified as the major contributor to the fast performance degradation,impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative,yet remains challenging due to the lack of efficient approaches.Herein,we strategically regulate the bonding nature of Ru–O towards suppressed LOM via Ru-based high-entropy oxide(HEO)construction.The lattice disorder in HEOs is believed to increase migration energy barrier of lattice oxygen.As a result,the screened Ti_(23)Nb_(9)Hf_(13)W_(12)Ru_(43)O_(x) exhibits 11.7 times slower lattice oxygen diffusion rate,84%reduction in LOM ratio,and 29 times lifespan extension compared with the state-of-the-art RuO_(2) catalyst.Our work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.

关键词： ruthenium-based high-entropy oxide suppressing the lattice oxygen diffusion acidic oxygen evolution reaction

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Stabilizing high-efficiency iridium single atoms via lattice confinement for acidic oxygen evolution

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Nano Research 2024年第4期17卷 2492-2498页

作者： Yibo Wang Jiadong Jiang Zhaoping Shi Hongxiang Wu Jiahao Yang Pengbo Wang Shuai Hou meiling xiao Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026.China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province Key Laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Key Laboratory of Physics and Technology for Advanced Batteries Ministry of EducationCollege of PhysicsJilin UniversityChangchun 130012China

Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir doped in tetragonal PdO matrix(IrSAs-PdO)via a lattice-confined strategy.The optimized IrSAs-PdO-0.10 exhibited remarkable OER activity with an overpotential of 277 mV at 10 mA·cm^(-2) and long-term stability of 1000 h in 0.5 M H_(2)SO_(4).Furthermore,the turnover frequency attains 1.6 s^(-1) at an overpotential of 300 mV with a 24-fold increase in the intrinsic activity.The high activity originates from isolated iridium sites with low valence states and decreased Ir–O bonding covalency,and the excellent stability is a result of the effective confinement of iridium sites by Ir–O–Pd motifs.Moreover,we demonstrated for the first time that SACs have great potential in realizing ultralow loading of iridium(as low as microgram per square center meter level)in a practical water electrolyzer.

关键词： lattice confinement iridium single atoms ultralow iridium loading acidic oxygen evolution proton exchange membrane water electrolysis

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Atomically dispersed Fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

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Journal of Energy Chemistry 2024年第3期90卷 7-15,I0002页

作者： Ruixue Zheng Qinglei Meng Hao Zhang Teng Li Di Yang Li Zhang xiaolong Jia Changpeng Liu Jianbing Zhu xiaozheng Duan meiling xiao Wei Xing State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123JiangsuChina State Key Laboratory of Polymer Physics and Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina

Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air batteries.Although Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active sites.Motivated by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) sites.Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N precursors.Benefitting from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(vs.reversible hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 h.Molecular dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR performance.In situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C SAC-950.This work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.

关键词： Fe single atom catalysts Oxygen reduction reaction Mesoporous structure Active sites Zinc-air battery

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Catecholaminergic neurons orchestrate fasting-induced immune harmony

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Biophysics Reports 2024年第1期10卷 57-59页

作者： Mengdi Guo Weiyan Wang xiao Tu meiling Jiang Cun-Jin Zhang Department of Neurology Sichuan Provincial People's Hospital University of Electronic Science and Technology of China Department of Science and Technology Sichuan Provincial People's Hospital University of Electronic Science and Technology of China

Dietary fasting is a well-established intervention for immunosuppressive therapy, but the underlying mechanism remains elusive. Host fitness to nutritional stress has been confirmed to initiate a cascade of adaptive responses mediated by the central nervous system, shedding new light on a neural link between fasting and immunity(de Cabo and Mattson 2019).

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Microenvironment regulation of M-N-C single-atom catalysts towards oxygen reduction reaction

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Nano Research 2023年第4期16卷 4468-4487页

作者： Li Zhang Qinglei Meng Ruixue Zheng Liuqing Wang Wei Xing Weiwei Cai meiling xiao State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Sustainable Energy Laboratory Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430074China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

The development of cost-effective,robust,and durable electrocatalysts to replace the expensive Pt-based catalysts towards oxygen reduction reaction(ORR)is the trending frontier research topic in renewable energy and electrocatalysis.Particular attention has been paid to metal-nitrogen-carbon(M-N-C)single atom catalysts(SACs)due to their maximized atom utilization efficiency,biomimetic active site,and distinct electronic structure.More importantly,their catalytic properties can be further tailored by rationally regulating the microenvironment of active sites(i.e.,M-N coordination number,heteroatom doping and substitution.Herein,we present a comprehensive summary of the recent advancement in the microenvironment regulation of MN-C SACs towards improved ORR performance.The coordination environment manipulation regarding central metal and coordinated atoms is first discussed,focusing on the structure-function relationship.Apart from the near-range coordination,longrange substrate modulation including heteroatom doping,defect engineering is discussed as well.Besides,the synergy mechanism of nanoparticles and single atom sites to tune the electron cloud density at the active sites is summarized.Finally,we provide the challenges and outlook of the development of M-N-C SACs.

关键词： single-atom catalyst oxygen reduction reaction microenvironment regulation active site structure electronic structure

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Contemporary Asymmetric Genetic Introgression Between Two Pelophylax Species in Shanghai

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Asian Herpetological Research 2024年第1期15卷 1-11页

作者： Xu WEI Wenli LIU Gang WANG Rui MA meiling HUANG Jiaxin ZHENG Tingwei DONG Changqing YUAN Shunqi BO xiao YUAN Ben LI Shuo MA Qu YUE Youzhong DING Zhenghuan WANG School of Life Sciences East China Normal UniversityShanghai 200241China Shanghai Landscaping and City Appearance Administrative Bureau Shanghai 200041China State Key Laboratory of Estuarine and Coastal Research East China Normal UniversityShanghai 200241China Shanghai Key Lab for Urban Ecological Processes and Eco-Restoration East China Normal UniversityShanghai 200241China Yangtze Delta Estuarine Wetland Ecosystem Observation and Research Station Ministry of Education&Shanghai Science and Technology CommitteeShanghai 202162China

Human disturbances are considered to break reproduction barriers among species.Significant increases in hybridization events have been reported among a large number of taxonomic groups in anthropogenic environments,providing novel insights into species evolution mechanisms and conservation management in the Anthropocene.The Eastern Golden Frog(Pelophylax plancyi)and BlackSpotted Frog(P.nigromaculatus)are two sympatric anuran species with a long history of mitochondrial genome introgression in highly urbanized continental East Asia.However,there is only limited understanding of the pattern of their contemporary hybridization and factors influencing their interspecific relationship under anthropogenic disturbances.Here,interspecific hybridization between P.plancyi and P.nigromaculatus at the population level was investigated in Shanghai.All except two haplotypes obtained from both species in Shanghai were mixed together,and located in the introgression clade,implying multiple ancient mitochondrial introgression events occurred in the populations of our study area.Asymmetric genetic introgression was detected by microsatellite markers,with 0.7%of P.plancyi and 14.6%of P.nigromaculatus identified as contemporary admixed individuals.Consistent with the trend of population density,higher genetic diversity of neutral microsatellite loci was found in the more abundant P.plancyi;however,variation in mitochondrial(Cyt-b)and nuclear(POMC)genes was higher in relatively rare P.nigromaculatus.The population density of P.plancyi and number of water patches within local habitats were significantly positively correlated with both occurrences and proportions of admixed individuals in the populations of P.plancyi and P.nigromaculatus.Considering the prevalent transformation of habitats in urbanized areas,these results imply that a high population density in isolated artificially altered habitats is likely to increase interspecific hybridization.Thus,population monitoring and improvement of landscape connectivity between habitats wo

关键词： anthropogenic disturbances interspecific hybridization Pelophylax species abundance urban landscape urbanization

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Polymer-chelation approach to high-performance Fe-Nx-C catalyst towards oxygen reduction reaction

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Chinese Chemical Letters 2023年第4期34卷 349-352页

作者： Xue Wang Li Zhang meiling xiao Junjie Ge Wei Xing Changpeng Liu Jianbing Zhu Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Pyrolyzed Fe-Nx-C with atomically dispersed Fe-Nxsites are hailed as the most promising alternative to the noble metal Pt-based catalysts towards oxygen reduction reaction(ORR). However, the conventional micropore-confinement synthetic approach usually causes the insufficient utilization of active sites and mass transport resistance as the sites are located inside the micropore. We herein report a polymerchelation strategy to directly disperse the Fe-Nxactive sites onto the carbon surface. The N-rich monomer was in-situ polymerized on the carbon support and then chelated with Fe. The strong Fe-N chelating interaction is crucial to suppress Fe aggregation when undergoing the high-temperature pyrolysis. Due to the enriched surface sites, hierarchically porous structure and excellent conductivity of carbon support,the optimal catalyst(denoted as Fe-Nx-C@C-900) exhibits impressive ORR activity of onset and half-wave potential of 1.02 and 0.87 V, respectively, superior to the Pt/C benchmark.

关键词： Oxygen reduction reaction Electrocatalyst Active site Atomically dispersed metal Hierarchically porous

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Revealing the true origin of size-dependent Pd/C catalytic behavior towards formic acid decomposition

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Chinese Chemical Letters 2023年第1期34卷 457-460页

作者： Qinglei Meng Xian Wang meiling xiao Zhao Jin Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Formic acid decomposition(FAD)is considered a promising hydrogen production route to facilitate the ambient storage and on demand release of hydrogen energy.To optimize the catalysts for FAD,efforts have been paid to explore the underlying reason for the varied catalytic activity among catalysts with similar composition but differed structure.However,such endeavors are highly challenging due to the deeply intermingled effects of electronic structure,particle size,and facets,etc.Herein,to separately evaluate the respective effects of these factors,a series of catalysts with the same surface electronic structure and different particle size was prepared by cation dipole adjustment method.The performance and characterization results showed that the catalysts with different sizes and facets exhibited similar intrinsic activity with deviation of less than 5%.However,they showed 252%deviation of site stability,indicating that only the optimized electronic structure could enhance the intrinsic activity and a smaller particle size could extend the catalyst’s life.

关键词： Hydrogen production Formic acid Catalyst deactivation Size effect Facets effect

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Copper‑Based Catalysts for Electrochemical Carbon Dioxide Reduction to Multicarbon Products

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Electrochemical Energy Reviews 2022年第3期5卷 178-212页

作者： Fangfang Chang meiling xiao Ruifang Miao Yongpeng Liu Mengyun Ren Zhichao Jia Dandan Han Yang Yuan Zhengyu Bai Lin Yang Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals Key Laboratory of Green Chemical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007HenanChina Department of Chemical Engineering University of WaterlooWaterlooON N2L 3G1Canada

Electrochemical conversion of carbon dioxide into fuel and chemicals with added value represents an appealing approach to reduce the greenhouse effect and realize a carbon-neutral cycle,which has great potential in mitigating global warming and effectively storing renewable energy.The electrochemical CO_(2) reduction reaction(CO_(2)RR)usually involves multiproton coupling and multielectron transfer in aqueous electrolytes to form multicarbon products(C_(2+) products),but it competes with the hydrogen evolution reaction(HER),which results in intrinsically sluggish kinetics and a complex reaction mechanism and places higher requirements on the design of catalysts.In this review,the advantages of electrochemical CO_(2) reduction are briefly introduced,and then,different categories of Cu-based catalysts,including monometallic Cu catalysts,bimetallic catalysts,metal-organic frameworks(MOFs)along with MOF-derived catalysts and other catalysts,are summarized in terms of their synthesis method and conversion of CO_(2) to C2+products in aqueous solution.The catalytic mechanisms of these catalysts are subsequently discussed for rational design of more efficient catalysts.In response to the mechanisms,several material strategies to enhance the catalytic behaviors are proposed,including surface facet engineering,interface engineering,utilization of strong metal-support interactions and surface modification.Based on the above strategies,challenges and prospects are proposed for the future development of CO_(2)RR catalysts for industrial applications.

关键词： C_(2)products Carbon dioxide Nanocatalysts Electrochemical reduction Mechanism

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