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Heterostructured Pt-Ni_(3)Mo_(3)N formed via ammonia-containing polyoxometalates for highly efficient electrocatalytic hydrogen evolution in acid medium

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Journal of Energy Chemistry 2024年第5期92卷 698-704页

作者： Bianqing Ren Xue Gong Jing Cao Dezheng Zhang Zizhun Wang Ping Song Ce Han Weilin Xu State key laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina key laboratory of Automobile Materials MOE School of Materials Science&EngineeringJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy Centerand International Center of Future ScienceJilin UniversityChangchun 130012JilinChina

Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4)]·5H_(2)O polyoxometalates(NiMo_(6))are adopted as the cluster precursors for simple fabrication of heterostructured Pt-Ni_(3)Mo_(3)N nanohybrids supported by carbon black(Pt-Ni_(3)Mo_(3)N/C)without using additional N *** improved porosity and enhanced electronic interaction of Pt-Ni_(3)Mo_(3)N/C should be attributed to the integration of Pt with NiMo_(6),which favors the mass transport,promotes the formation of exposed catalytic sites,and benefits the regulation of intrinsic ***,the as-obtained Pt-Ni_(3)Mo_(3)N/C exhibits impressive and durable HER performance as indicated by the low overpotential of 13.7 mV at the current density of 10 mA cm^(-2) and the stable overpotential during continuous working at 100 mA cm^(-2) for 100 *** work provides significant insights for the synthesis of new highly active heterostructured electrocatalysts for renewable energy devices.

关键词： Polyoxometalates Cluster precursors Heterostructured nanohybrids Hydrogen evolution reaction Electrocatalysis

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Degradation mechanisms and stabilization strategies of ruthenium-based catalysts for OER in the proton exchange membrane water electrolyzer

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Progress in Natural Science:Materials International 2024年第1期34卷 207-222页

作者： Ming Yang Hongxiang Wu Zhaoping Shi Yibo Wang Jiahao Yang Jing Ni Pengbo Wang Yuqing Cheng Ziang Wang Meiling Xiao Changpeng Liu Wei Xing laboratory of Advanced power Sources Changchun Institute of Applied Chemistry Chinese Academy of Sciences School of Applied Chemistry and Engineering University of Science and Technology of China jilin Province key laboratory of low carbon chemical power Sources State key laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Designing economical oxygen evolution reaction(OER) electrocatalysts with high activity and long-term stability is essential to promote the scale-up applications of proton exchange membrane water electrolyzer(PEMWE) for hydrogen production. Ruthenium(Ru)-based materials with high intrinsic activity are hailed as the most promising catalysts, but still infeasible for practical application considering their long unresolved poor stability(only dozens of lifespan). Thus, tremendous efforts have been devoted to uncovering the degradation mechanisms and developing stabilization strategies for the Ru-based catalysts. In this review, starting from summarizing the fundamental understanding of deactivation mechanisms, a picture of the stability issue of Ru-based catalysts is proposed, which is followed by a detailed discussion on the recently developed strategies and progress made on enhancing durability. Finally, insights on the prospects for the future development of stable and practical Rubased OER catalysts are provided.

关键词： OER Ru-based catalysts PEMWE Degradation mechanisms Stabilization strategies

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Building Fe atom–cluster composite sites using a site occupation strategy to boost electrochemical oxygen reduction

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carbon Energy 2024年第3期6卷 276-286页

作者： Tingyi Zhou Yi Guan Changjie He Lei Zhang Xueliang Sun Zhongxin Song Qianling Zhang Chuanxin He Xiantao Jiang Zhaoyan Luo Wei Xing Xiangzhong Ren College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdongChina Department of Mechanical and Materials Engineering University of Western OntarioLondonOntarioCanada State key laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesJilinChangchunChina

The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic clusters to ***,understanding the interactions among these components,especially the synergistic effects between single atomic sites and cluster sites,is crucial for improving the oxygen reduction reaction(ORR)activity of M–N–C ***,herein,we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation *** found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron-withdrawing–OH ligands and decreasing the d-band center of the Fe *** as-developed catalyst exhibits encouraging ORR activity with halfwave potentials(E1/2)of 0.831 and 0.905 V in acidic and alkaline media,***,the catalyst also represents excellent durability exceeding that of Fe–N–C SA *** practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metalair battery *** work exhibits the great potential of synergistic effects between multiphase metal species for improvements of singleatom site catalysts.

关键词： d-band center metal clusters oxygen reduction reaction single-atom catalyst site occupations strategy

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Molecule aging induced by electron attacking

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Journal of Energy Chemistry 2024年第6期93卷 519-525,I0013页

作者： Ping Song Yining Dong Xue Gong Mingbo Ruan Baoxin Ni Xuanhao Mei Kun Jiang Weilin Xu State key laboratory of Electroanalytical Chemistry and jilin Province key laboratory of low carbon chemical power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied Chemistry and Engineering University of Science and Technology of Chin1Hefei 230026AnhuiChina Shanghai key laboratory of Molecular Catalysis and Innovative Materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China

Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed *** further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)*** IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water *** facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule *** exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C *** density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water *** results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.

关键词： Aging of molecules Electron attacking Full width at half maxima Hydrogen 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 *** 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 *** 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 ***,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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A zincophilic molecular brush for a dendrite-free,corrosionresistant,zinc metal anode with a long life cycle

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Nano Research 2024年第1期17卷 390-396页

作者： Penggao Liu Jia Guo Xinyue Chen Ting Wang Yanping Huang Shasha Gao Tao Wang Dongling Wu Kaiyu Liu State key laboratory of Chemistry and Utilization of carbon based Energy Resources College of ChemistryXinjiang UniversityUrumqi 830017China Hunan provincial key laboratory of chemical power Sources College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China key laboratory of New low-carbon Green chemical Technology School of Chemistry and Chemical EngineeringEducation Department of Guangxi Zhuang Autonomous RegionGuangxi UniversityNanning 530004China key laboratory of Microelectronics and Energy of Henan Province Department of Physics and Electronic EngineeringXinyang Normal UniversityXinyang 464000China Interdisciplinary Research Center for Sustainable Energy Science and Engineering(IRC4SE2) School of Chemical EngineeringZhengzhou UniversityZhengzhou 450001China

Zinc-based aqueous rechargeable batteries have attracted extensive attention due to their low cost,safety,and environmental ***,dendrite growth and hydrogen evolution of Zn anodes limit their large-scale application.A new strategy to produce a polyacrylamide/reduced graphene oxide(PAM@rGO)molecular nanobrush coating and control Zn electrolyte interface engineering is proposed for use in highly reversible Zn plating/*** evolution is inhibited,and Zn deposition is consolidated using the rich zincophilic functional groups of the branched polyacrylamide chain and the high conductivity of *** to the synergistic effects of corrosion resistance and dendrite-free growth,PAM@rGO/Zn provides prolonged and reversible Zn plating/*** functional theory(DFT)calculations expand on homogenized *** PAM@rGO/Zn||activated carbon(AC)capacitor exhibits long cyclic stability,fast ion transfer,and minimal interfacial *** study provides experimental and theoretical bases for the structural design of Zn anode.

关键词： zincophilic nanobrush polyacrylamide/reduced graphene oxide(PAM@rGO)/Zn surface modification Zn based energy storage

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Direct Observation on H-Elimination Enhancement from C_(2)H_(4) through Non-Adiabatic Process by Femtosecond Laser Induced Coulomb Explosion

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Chinese Physics Letters 2024年第5期41卷 17-22页

作者：金无维王春成赵晓戈杨译章任殿相刘泽槿李孝开罗嗣佐丁大军 Institute of Atomic and Molecular Physics Jilin UniversityChangchun 130012China jilin provincial key laboratory of Applied Atomic and Molecular Spectroscopy Jilin UniversityChangchun 130012China

Ethylene, the simplest model of a carbon-carbon double bond system, is pivotal in numerous chemical and biological processes. By employing intense infrared laser pump-probe techniques alongside coincidence measurements, we investigate the ultrafast non-adiabatic dynamics involved in the breakage of carbon-carbon double bonds and hydrogen elimination in dissociation of ethylene. Our study entails analyzing the dynamic kinetic energy release spectra to assess three bond-breaking scenarios, movements of nuclei, and structural changes around the carbon atoms. This allows us to evaluate the relaxation dynamics and characteristics of various dissociative states. Notably, we observe a significant rise in the yield of fragments resulting from C–H bond breakage with the delay time extended, suggesting non-adiabatic coupling through conical intersections from C–C bond breakage as a probable cause.

关键词： pump Femto adiabatic

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

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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 *** 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 ***,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 *** we successfully construct a series of catalyst models with gradient conductivities by regulating molybdenum disulfide(MoS_(2))electronic bandgap via a simple solvothermal *** demonstrate that the conductivity of catalysts greatly affects the overall catalytic *** 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 *** 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 *** 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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Intermolecular Acid-Base-Pairs Containing Poly(p-Terphenyl-co-Isatin Piperidinium) for High Temperature Proton Exchange Membrane Fuel Cells

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Energy & Environmental Materials 2024年第3期7卷 410-418页

作者： Xiaofeng Hao Zhen Li Min Xiao Zhiheng Huang Dongmei Han Sheng Huang Wei Liu Shuanjin Wang Yuezhong Meng The key laboratory of low-carbon Chemistry & Energy Conservation of Guangdong Province State Key Laboratory of Optoelectronic Materials and TechnologiesSchool of Materials Science and EngineeringSun Yat-sen University School of chemical Engineering and Technology Sun Yat-sen University Institute of Chemistry Henan Provincial Academy of Sciences Research Center of Green Catalysts College of ChemistryZhengzhou University

How to optimize and regulate the distribution of phosphoric acid in matrix,and pursuing the improved electrochemical performance and service lifetime of high temperature proton exchange membrane （HT-PEMs） fuel cell are significant ***,bifunctional poly （p-terphenyl-co-isatin piperidinium） copolymer with tethered phosphonic acid （t-PA） and intrinsic tertiary amine base groups are firstly prepared and investigated as *** distinctive architecture of the copolymer provides a well-designed platform for rapid proton *** not only transports through the hydrogen bond network formed by the adsorbed free phosphoric acid （f-PA）anchored by the tertiary amine base groups,but also rely upon the proton channel constructed by the ionic cluster formed by the t-PA *** the design of the structure,the bifunctional copolymers with lower PA uptake level （power densities (99 mS cm-1,812 mW cm-2at 160℃),along with lower PA leaching and higher voltage stability,which is a top leading result in disclosed *** results demonstrate that the design of intermolecular acid-base-pairs can improve the proton conductivity without sacrificing the intrinsic chemical stability or mechanical property of the thin membrane,realizing win-win demands between the mechanical robustness and electrochemical properties of HT-PEMs.

关键词： bifunctional copolymer high temperature proton exchange membrane intermolecular acid–base-pairs phosphonic acid retention phosphonic acid uptake level

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Metal-organic framework-derived porous carbon for the advanced aqueous zinc-ion hybrid capacitor

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Journal of Central South University 2024年第7期31卷 2268-2279页

作者： LIU Wei-fang HU Zi-han ZHANG Qi School of Chemistry and chemical Engineering Hunan University of Science&TechnologyXiangtan 411201China Hunan provincial key laboratory of chemical power Sources College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China

Aqueous zinc ion hybrid capacitors(ZIHCs)are considered one of the most promising electrochemical energy storage systems due to their high safety,environmental friendliness,low cost,and high power ***,the low energy density and the lack of sustainable design strategies for the cathodes hinder the practical application of ***,we design the N and O co-doped porous carbon cathode by annealing metal-organic framework(ZIF-8).ZIF-8 retains the original dodecahedral structure with a high specific surface(2814.67 m^(2)/g)and I_(G)/I_(D) ratio of 1.0 during carbonization and achieves self-doping of N and O *** defect sites are introduced into the porous carbon to provide additional active sites for ion adsorption after the activation of carbonized ZIF-8 by KOH *** ZIHCs assembled with modified ZIF-8 as the cathode and commercial zinc foil as the anode show an energy density of 125 W∙h/kg and a power density of 79 W/*** addition,this ZIHCs device achieves capacity retention of 77.8%after 9000 electrochemical cycles,which is attributed to the diverse pore structure and plentiful defect sites of ZIF-8-800(KOH).The proposed strategy may be useful in developing high-performance metal-ion hybrid capacitors for large-scale energy storage.

关键词： zinc ion hybrid capacitor cathode metal-organic framework(ZIF-8) KOH activation

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