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CCS Chemistry 2024年第3期6卷 749-760页

作者： Junkai Yang Jixing Yang Yunhua Xu Yuesheng Li School of materials Science and Engineering Tianjin Key Laboratory of Composite and Functional MaterialsTianjin UniversityTianjin 300350

Conducting polymers(CPs)have long been studied as cathode materials for lithium-ion batteries,but the low doping level(maximum:30–50%or even lower)and poor cycling stability limit their applications.Herein,we have developed a method of nanoporeconfined in situ electropolymerization to prepare nanostructured polythiophene-type porous cathodes,achieving significantly improved doping availability and long cycle life.It was verified that the nanosized polymer formed in situ and loose porous structure are conducive to the doping reaction and maintain high electrochemical stability.The constructed thieno[3,2-b]thiophene(TtTP)/active carbon cathode delivers an ultrahigh reversible capacity of 309.2 mAh g^(−1)(doping level up to 80.9%)along with an ultrahigh energy density of 1252.3 Wh Kg^(−1),and an ultrahigh rate capability(172.4 mAh g^(−1) at 30 A g^(−1)),which far exceed all the CPs and even all the p-type organic cathode materials reported.Moreover,an excellent long cycle life of 2000 cycles at 5 A g^(−1) is also revealed,which is a new record for CPs-based cathode materials in nonaqueous lithium-ion batteries.Our method provides an effective strategy to improve the doping level and cycling stability of CP-based cathode materials.

关键词： organic cathode materials conducting polymers lithium-ion batteries porous carbon in situ electropolymerization

porous metal oxides in the role of electrochemical CO_(2) reduction reaction

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Journal of Energy Chemistry 2024年第1期88卷 373-398,I0009页

作者： Ziqi Zhang Jinyun Xu Yu Zhang Liping Zhao Ming Li Guoqiang Zhong Di Zhao Minjing Li Xudong Hu Wenju Zhu Chunming Zheng Xiaohong Sun School of Chemical Engineering and Technology Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringState Key Laboratory of Separation Membrane and Membrane ProcessesTiangong UniversityTianjin 300387China School of materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining TechnologyMinistry of EducationTianjin UniversityTianjin 300072China

The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous metal oxide materials in the electrocatalytic reduction of CO_(2)(CO_(2)RR).The focus is on the development of robust and selective catalysts,particularly metal and metal-oxide-based materials.porous metal oxides offer high surface area,enhancing the accessibility to active sites and improving reaction kinetics.The tunability of these materials allows for tailored catalytic behavior,targeting optimized reaction mechanisms for CO_(2)RR.The work also discusses the various synthesis strategies and identifies key structural and compositional features,addressing challenges like high overpotential,poor selectivity,and low stability.Based on these insights,we suggest avenues for future research on porous metal oxide materials for electrochemical CO_(2) reduction.

关键词： CO_(2)reduction Carbon dioxide Transformation porous metal oxides Electrocatalysis

Recent advances in the electrocatalytic oxidative upgrading of lignocellulosic biomass

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ChemPhysMater

ChemPhysMater 2024年第2期3卷 157-186页

作者： Yufeng Qi Hairui Guo Junting Li Li Ma Yang Xu Huiling Liu Cheng Wanga Zhicheng Zhang Institute for New Energy materials and Low-Carbon Technologies School of Materials Science and EngineeringTianjin Key Laboratory of Advanced Functional Porous MaterialsTianjinUniversityof TechnologyTianjin 300384China key laboratory of Organic Integrated Circuit Minitry of Education&Tianjin Key Laboratoryof Molecular Optoelectronic Sciencespartment of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering(tianjin) Tianjin 300072China

Lignocellulosic biomass is a critical renewable carbon resource,but most of its utilization is inefficient,and elec-trocatalytic oxidation is a promising method of upgrading lignocellulose into value-added fuels and chemicals under mild operating conditions.Recently,efforts to enable conversion with a high efficiency and low energy con-sumption have been reported,but understanding the reaction mechanisms and realizing scaled-up applications of the electrooxidation of lignocellulosic biomass are still in their early stages.A timely overview of recently reported general reaction mechanisms,particularly the strategies developed for use in improving the reaction efficiencies,is necessary to inspire research regarding the highly efficient utilization of lignocellulose.Herein,we summa-rize the strategies developed to improve electrocatalytic performance in oxidative lignocellulose conversion.The organized summary includes strategies ranging from designing efficient electrocatalysts and adding functional co-catalysts or electrolytes to employing advanced electrolyzers.A comprehensive overview of representative examples should provide universal principles to yield insight into the reaction processes and guide the design of efficient electrocatalytic systems.Finally,the challenges and opportunities in developing the electrocatalytic oxidative upgrading of lignocellulosic biomass in the near future are proposed.

关键词： Biomass conversion Lignocellulose Electrocatalysis Oxidative upgrading Electrocatalyst

∼2.5 nm pores in carbon-based cathode promise better zinc-iodine batteries

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Chinese Chemical Letters 2024年第5期35卷 471-476页

作者： Yajun Hou Chuanzheng Zhu Qiang Wang Xiaomeng Zhao Kun Luo Zongshuai Gong Zhihao Yuan School of materials Science and Engineering Tianjin Key Laboratory of Photoelectric Materials&DevicesTianjin University of TechnologyTianjin 300384China

The relationship mechanism between the material pore structures and cathodic iodine chemistry plays a vital role in efficient Zn-I_(2) batteries,but is unclear,retarding further advances.This work innovatively indicates a great contribution of∼2.5nm pore structure of nanocarbons to efficient iodine adsorption,rapid I^(−)↔I_(2) conversion,and polyiodide inhibition,via scrupulously designing catalysts with controllable pore sizes systematically.The I_(2)-loading within the designed nitrogen-doped nanocarbons can reach up to as high as 60.8 wt%.The batteries based on the cathode deliver impressive performances with a large capacity of 178.8 mAh/g and long-term cycling stability more than 4000 h at 5.0 C.Notably,these is no polyiodide such as I_(3)−and I_(5)−detected during the charge-discharge processes from comprehensive electrochemical cyclic voltammetry,X-ray photoelectron spectroscopy,and Raman technique.This work provides a novel knowledge-guided concept for rational pore design,promising better Zn-I_(2) batteries,which is also hoped to benefit other advanced energy technologies,such as Li-S,Li-ion,and Al-I_(2) batteries.

关键词： Zinc-iodine batteries Structure-performance relationship Iodine conversion chemistry Cathode materials porous carbon

Recycling the spent electronic materials to construct a highperformance Cu_(1.94)S/ZnS heterostructure anode of sodium-ion batteries

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Nano Research 2024年第5期17卷 4006-4015页

作者： Xiaowei He Tianshuai Wang Lidong Tian Qiuyu Zhang School of Chemistry and Chemical Engineering Xi’an Key Laboratory of Functional Organic Porous MaterialsKey Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information TechnologyNorthwestern Polytechnical UniversityXi’an 710072China Chongqing Science and Technology Innovation Center of Northwestern Polytechnical University Chongqing 401135China College of materials Science and Engineering Xi’an University Science and TechnologyXi’an 710054China

Heterostructure engineering by coupling different nanocrystals has received extensive attention because it can enhance the reaction kinetics of the anode of sodium-ion batteries(SIBs).However,constructing high-quality heterostructure anode materials through green and environmentally friendly methods remains a challenge.Herein,we have proposed a simple one-step method by recycling the electronic waste metal materials to synthesize the Cu_(1.94)S/ZnS heterostructure materials.Combined with the experimental analysis and first principle calculations,we find that the synergistic effect of different components in heterostructure structures can significantly enhance the reversible capacity and rate performance of anode materials.Based on the constructed Cu_(1.94)S/ZnS anode,we obtain a superior reversible capacity of 440 mAh·g^(-1) at 100 mA·g^(-1) and 335 mAh·g^(-1) after 3000 cycles at 2000 mA·g^(-1).Our work sheds new light on designing high-rate and capacity anodes for SIBs through the greenness synthesis method.

关键词： sodium-ion batteries heterostructure reversible capacity environmentally synthesis process

Construction of biomimetic proton transport channels in metal-organic framework

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Chinese Chemical Letters 2024年第3期35卷 513-517页

作者： Xiao-Min Li Junchao Jia Danting Yang Jiali Jin Junkuo Gao School of materials Science and Engineering Institute of Functional Porous MaterialsZhejiang Sci-Tech UniversityHangzhou 310018China Zhejiang key laboratory of Pathophysiology School of Public HealthSchool of MedicineNingbo UniversityNingbo 315211China

Construction of proton transport channels in metal-organic frameworks(MOFs)with simple synthesis processes,high proton conductivities and good performance stabilities has been of great interest for proton exchange membrane fuel cell(PEMFC).Herein,we mimic the proton transport behavior of amino acid residues in bacteriorhodopsin,select UiO-66-COOH as the host,glycine and aspartic acid as the functional guest molecules,and then functionalize the MOF framework with amino acids to obtain biomimetic proton transport channels.This strategy endows UiO-66-COOH-Asp a high proton conductivity of 1.19×10^(-2)S/cm at 70℃and 98%RH,excellent cycle stability of performances and performance durability,which can be comparable to the reported MOFs-based proton conductors.Moreover,the proton conduction mechanism in UiO-66-COOH-Asp is elaborated in detail due to its visual structure,which is also one of the advantages of adopting MOFs as research platform,making it possible to optimize the structure-activity relationship of advanced materials.Notably,this strategy has clear objectives and simple synthesis,which has made certain contributions to both theoretical research and future industrial production of proton conductors.

关键词： MOF Amino acids Biomimetic proton transport channels Synergistic effect Proton conduction mechanism

MOF-derived Cu embedded into N-doped mesoporous carbon as a robust support of PdAu nanocatalysts for ethanol electrooxidation

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Rare Metals 2024年第3期43卷 1083-1094页

作者： Yu-Fu Huang Peng Wu Jun-Ping Tang Jian Yang Jing Li Shuai Chen Xue-Ling Zhao ChengChen Bin-Wei Zhang Yan-Yun Ma Wei-Heng Shi Dong-Hai Lin Shi-Gang Sun School of Energy and materials Shanghai Engineering Research Center of Advanced Thermal Functional MaterialsShanghai Key Laboratory of Engineering Materials Application and EvaluationShanghai Polytechnic UniversityShanghai201209China State key laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China School of Chemistry and Chemical Engineering Chongqing UniversityChongqing401331China Center of advanced Energy Technology and Electrochemistry Institute of Advanced Interdisciplinary StudiesChongqing UniversityChongqing400044China Institute of functional Nano&Soft materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou215123China Department of materials Science and Engineering Drexel UniversityPhiladelphiaPA19104USA

Metal-organic frameworks(MOFs)h ave attracted widespread attention due to their large surface area and porous structure.Rationally designing the nanostructures of MOFs to promote their application in ethanol electrooxidation is still a challenge.Here,a novel Cu-NCNs(Cu-nitrogen-doped carbon nanotubes)support was synthesized by pyrolysis of melamine(MEL)and Cu-ZIF-8 together,and then,Pd-Au nanoalloys were loaded by sodium borohydride reduction method to prepare PdAu@Cu-NCNs catalysts.The generating mesoporous carbon with high specific surface area and favorable electron and mass transport can be used as a potential excellent carrier for PdAu nanoparticles.In addition,the balance of catalyst composition and surface structure was tuned by controlling the content of Pd and Au.Thus,the best-performed Pd_(2)Au_(2)@Cu-NCN-1000-2(where 1000 means the carrier calcination temperature,and 2 means the calcination constant temperature time)catalyst exhibits better long-term stability and electrochemical activity for ethanol oxidation in alkaline media(4.80 A·mg^(-1)),which is 5.05 times higher than that of commercial Pd/C(0.95 A·mg^(-1)).Therefore,this work is beneficial to further promoting the application of MOFs in direct ethanol fuel cells(DEFCs)and can be used as inspiration for the design of more efficient catalyst support structures.

关键词： Metal-organic frameworks(MOFs) N-doped Mesoporous carbon PdAu Ethanol electrooxidation

Boosting Fischer-Tropsch Synthesis via Tuning of N Dopants in TiO_(2)@CN-Supported Ru Catalysts

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Transactions of tianjin University 2024年第1期30卷 90-102页

作者： Xincheng Li Yunhao Liu Dejian Zhao Shuaishuai Lyu Jingwei Ye Xiaoshen Li Peipei Wu Ye Tian Yingtian Zhang Tong Ding Song Song Qingpeng Cheng Xingang Li State key laboratory of Chemical Engineering Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Haihe Laboratory of Sustainable Chemical TransformationsTianjin Key Laboratory of Applied Catalysis Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Zhejiang Institute of tianjin University Shaoxing 312300China Sinopec Research Institute of Petroleum Processing Co. LTDBeijing 100083China Physical Sciences and Engineering Division Advanced Membranes and Porous Materials(AMPM)CenterKing Abdullah University of Science and Technology(KAUST)23955-6900 ThuwalSaudi Arabia

Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted signifi cant attention,but the eff ect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such as Fischer-Tropsch synthesis(FTS).Herein,we engineered ruthenium(Ru)FTS catalysts supported on N-doped carbon overlayers on TiO_(2)nanoparticles.By regulating the carbonization temperatures,we successfully controlled the types and contents of N dopants to identify their impacts on metal-support interactions(MSI).Our fi ndings revealed that N dopants establish a favorable surface environment for electron transfer from the support to the Ru species.Moreover,pyridinic N demonstrates the highest electron-donating ability,followed by pyrrolic N and graphitic N.In addition to realizing excellent catalytic stability,strengthening the interaction between Ru sites and N dopants increases the Ru^(0)/Ru^(δ+)ratios to enlarge the active site numbers and surface electron density of Ru species to enhance the strength of adsorbed CO.Consequently,it improves the catalyst’s overall performance,encompassing intrinsic and apparent activities,as well as its ability for carbon chain growth.Accordingly,the as-synthesized Ru/TiO_(2)@CN-700 catalyst with abundant pyridine N dopants exhibits a superhigh C_(5+)time yield of 219.4 mol CO/(mol Ru·h)and C_(5+)selectivity of 85.5%.

关键词： Fischer-Tropsch synthesis N-doped carbon materials Ruthenium catalyst Pyridinic N Metal-N interaction

MOF-mediated synthesis of novel PtFeCoNiMn high-entropy nanoalloy as bifunctional oxygen electrocatalysts for zinc-air battery

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Nano Research 2024年第6期17卷 5288-5297页

作者： Mingkuan Xie Xin Xiao Duojie Wu Cheng Zhen Chunsheng Wu Wenjuan Wang Hao Nian Fayan Li Meng Danny Gu Qiang Xu Shenzhen key laboratory of Micro/Nano-porous functional materials(SKLPM) Shenzhen 518055China Department of Chemistry Southern University of Science and TechnologyShenzhen 518055China Department of materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055China SUSTech-Kyoto University advanced Energy materials Joint Innovation laboratory(SKAEM-JIL) Shenzhen 518055China key University laboratory of Highly Efficient Utilization of Solar Energy and Sustainable Development of Guangdong Southern University of Science and TechnologyShenzhen 518055China Eastern Institute for advanced Study Eastern Institute of TechnologyNingbo 315200China

High-entropy alloy(HEA)-based materials are expected to be promising oxygen electrocatalysts due to their exceptional properties.The electronic structure regulation of HEAs plays a pivotal role in enhancing their elctrocatalytic ability.Herein,PtFeCoNiMn nanoparticles(NPs)with subtle lattice distortions are constructed on metal-organic framework-derived nitrogen-doped carbon by an ultra-rapid Joule heating process.Thanks to the modulated electronic structure and the inherent cocktail effect of HEAs,the as-synthesized PtFeCoNiMn/NC exhibits superior bifunctional electrocatalytic performance with a positive half-wave potential of 0.863 V vs.reversible hydrogen electrode(RHE)for oxygen reduction reaction and a low overpotential of 357 mV at 10 mA·cm^(-2)for oxygen evolution reaction.The assembled quasi-solid-state zinc-air battery using PtFeCoNiMn/NC as air electrode shows a high peak power density of 192.16 mW·cm^(-2),low charge−discharge voltage gap,and excellent durability over 500 cycles at 5 mA·cm^(-2).This work demonstrates an effective route for rational design of bifunctional nanostructured HEA electrocatalysts with favorable electronic structures,and opens up a fascinating directions for energy storage and conversion,and beyond.

关键词： oxygen reduction reaction oxygen evolution reaction high-entropy nano-alloy zinc-air battery

Janus Quasi‑Solid Electrolyte Membranes with Asymmetric porous Structure for High‑Performance Lithium‑Metal Batteries

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Nano-Micro Letters 2024年第6期16卷 221-232页

作者： Zerui Chen Wei Zhao Qian Liu Yifei Xu Qinghe Wang Jinmin Lin Hao Bin Wu Institute for Composites Science Innovation(InCSI)and State key laboratory of Silicon and advanced Semiconductor materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China

Quasi-solid electrolytes(QSEs)based on nanoporous materials are promising candidates to construct high-performance Limetal batteries(LMBs).However,simultaneously boosting the ionic conductivity(σ)and lithium-ion transference number(t^(+)) of liquid electrolyte confined in porous matrix remains challenging.Herein,we report a novel Janus MOFLi/MSLi QSEs with asymmetric porous structure to inherit the benefits of both mesoporous and microporous hosts.This Janus QSE composed of mesoporous silica and microporous MOF exhibits a neat Li^(+) conductivity of 1.5.10^(–4)S cm^(−1) with t^(+) of 0.71.A partially de-solvated structure and preference distribution of Li^(+)near the Lewis base O atoms were depicted by MD simulations.Meanwhile,the nanoporous structure enabled efficient ion flux regulation,promoting the homogenous deposition of Li^(+).When incorporated in Li||Cu cells,the MOFLi/MSLi QSEs demonstrated a high Coulombic efficiency of 98.1%,surpassing that of liquid electrolytes(96.3%).Additionally,NCM 622||Li batteries equipped with MOFLi/MSLi QSEs exhibited promising rate performance and could operate stably for over 200 cycles at 1 C.These results highlight the potential of Janus MOFLi/MSLi QSEs as promising candidates for next-generation LMBs.

关键词： Metal-organic frameworks Mesoporous silicas Quasi-solid electrolytes Janus structure Lithium-metal battery