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Electronic interactions between neighboring functionalized guest Sb single atoms and Pt clusters enhance CO tolerance

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Journal of Energy Chemistry 2025年第2期101卷 733-743页

作者： Wenkang Miao Ronghui Hao Lu Gan Wanyin Xu Zihan Wang Wenxin Lin Heguang Liu Yinchun Lyu Qianqian Li Jinyang Xi Anmin Nie Jinsong Wu Hongtao Wang materials Genome Institute Shanghai University School of materials science and engineering Zhejiang Sci-Tech University School of materials science and engineering Xi'an University of Technology center for High Pressure science State Key Laboratory of Metastable Materials Science and Technology Yanshan University Nanostructure research center Wuhan University of Technology center for X-mechanics Zhejiang University

Platinum-based（Pt） catalysts are notoriously susceptible to deactivation in industrial chemical processes due to carbon monoxide（CO） *** this poisoning deactivation of Pt-based catalysts while enhancing their catalytic activity,selectivity,and durability remains a major ***,we propose a strategy to enhance the CO tolerance of Pt clusters（Pt_n） by introducing neighboring functionalized guest single atoms（such as Fe,Co,Ni,Cu,Sb,and Bi）.Among them,antimony（Sb） single atoms（SAs） exhibit significant performance enhancement,achieving 99% CO selectivity and 33.6% CO2conversion at 450℃,Experimental results and density functional theory（DFT） calculations indicate the optimization arises from the electronic interaction between neighboring functionalized Sb SAs and Pt clusters,leading to optimal 5d electron redistribution in Pt clusters compared to other functionalized guest single *** redistribution of 5d electrons weaken both the σ donation and π backdonation interactions,resulting in a weakened bond strength with CO and enhancing catalyst activity and *** situ environmental transmission electron microscopy（ETEM） further demonstrates the exception thermal stability of the catalyst,even under H2at 700℃.Notably,the functionalized Sb SAs also improve CO tolerance in various heterogenous catalysts,including Co/CeO2,Ni/CeO2,Pt/Al2O3,and Pt/*** finding provides an effective approach to overcome the primary challenge of CO poisoning in Pt-based catalysts,making their broader applications in various industrial catalysts.

关键词： CO tolerance Electronic effect Functionalized guest single atoms In-situ TEM Pt cluster

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Biomimetic proton pocket and effective interfacial modulation for zinc metal anodes

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science China Chemistry 2025年第2期68卷 526-535页

作者： Qi Dong Qingshun Nian Xuan Luo Jiajia Fan Jinyu Jiang Zhuangzhuang Cui Digen Ruan Xiaodi Ren Hefei National research center for Physical sciences at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Rechargeable aqueous zinc batteries(RAZBs)offer a promising solution for large-scale energy storage due to the abundance,low cost,and safety of ***,practical applications are hindered by Zn anode instability,dendrite growth,and hydrogen evolution reactions(HER).Chaotropic Zn(ClO_(4))2 electrolytes are favorable for low-temperature operations but exacerbate these issues due to their high acidity,leading to severe Zn corrosion and layered double hydroxide *** propose a biomimetic strategy using methylguanidoacetic acid(creatine)as a low-cost,eco-friendly additive to address these *** acts as a proton pocket to finely tune the pH of acidic Zn(ClO_(4))2 electrolytes for suppressing HER and stabilizing the Zn ***,the formed creatinine cations adsorb on the Zn surface,promoting highly controlled Zn deposition with a preferred(002)*** approach significantly enhances battery cycling performance,with Zn||Zn cells demonstrating extended cycling stability at both low and high current ***||Cu cells exhibited improved Coulombic efficiency over thousands of cycles,indicating highly reversible Zn plating/***,stable cell operations were realized at the temperature as low as−35℃ without electrolyte *** findings highlight the potential of biomimetic proton regulation and interfacial modulation for improving the stability and reversibility of Zn plating/stripping in RAZBs.

关键词： zinc metal anode dendrite suppression interfacial modulation proton-triggered cyclization Zn(ClO_(4))2 electrolyte

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A binary eutectic electrolyte design for high-temperature interface-compatible Zn-ion batteries

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Journal of Energy Chemistry 2025年第2期101卷 587-597页

作者： Guomin Li Wentao Wen Kefeng Ouyang Yanyi Wang Jianhui Zhu Ming Yang Hongwei Mi Ning Zhao Peixin Zhang Dingtao Ma College of Chemistry and Environmental engineering Shenzhen University School of materials science and engineering Harbin Institute of Technology (Shenzhen) School of materials and Environmental engineering Shenzhen Polytechnic Guangdong Flexible Wearable Energy and Tools engineering Technology research center

The deterioration of aqueous zinc-ion batteries（AZIBs） is confronted with challenges such as unregulated Zn2+diffusion,dendrite growth and severe decay in battery performance under harsh ***,a design concept of eutectic electrolyte is presented by mixing long chain polymer molecules,polyethylene glycol dimethyl ether（PEGDME）,with H2O based on zinc trifluoromethyl sulfonate(Zn（OTf）2),to reconstruct the Zn2+solvated structure and in situ modified the adsorption layer on Zn electrode *** dynamics simulations（MD）,density functional theory（DFT） calculations were combined with experiment to prove that the long-chain polymer-PEGDME could effectively reduce side reactions,change the solvation structure of the electrolyte and priority absorbed on Zn（002）,achieving a stable dendrite-free Zn *** to the comprehensive regulation of solvation structure and zinc deposition by PEGDME,it can stably cycle for over 3200 h at room temperature at 0.5 mA/cm2and 0.5 mAh/*** at high-temperature environments of 60℃,it can steadily work for more than 800 cycles（1600 h）.Improved cyclic stability and rate performance of aqueous Zn‖VO2batteries in modified electrolyte were also achieved at both room and high *** that,the demonstration of stable and high-capacity Zn‖VO2pouch cells also implies its practical application.

关键词： Dendrite suppression Eutectic electrolyte High temperature Solvation structure Zn anode

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Influence of laser shock peening on microstructure and high-temperature oxidation resistance of Ti45Al8Nb alloy fabricated via laser melting deposition

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Transactions of Nonferrous Metals Society of China 2025年第1期35卷 157-168页

作者： Lu-lu JIANG Liang LAN Cheng-yan BAI Ru-yi XIN Shuang GAO Hao-yu WANG Bo HE Chao-yue CHEN Guo-xin LU research center of High-Temperature Alloy Precision Forming School of Materials Science and EngineeringShanghai University of Engineering ScienceShanghai 201620China State Key Laboratory of Advanced Special Steels School of Materials Science and EngineeringShanghai UniversityShanghai 200444China School of materials science and engineering Shandong UniversityJinan 250061China

Laser shock peening(LSP)was used to enhance the high-temperature oxidation resistance of laser melting deposited Ti45Al8Nb *** microstructure and high-temperature oxidation behavior of the as-deposited Ti45Al8Nb alloy before and after LSP were investigated by scanning electron microscopy,X-ray diffraction,and electron backscatter *** results indicated that the rate of mass gain in the as-deposited sample after LSP exhibited a decrease when exposed to an oxidation temperature of 900℃,implying that LSP-treated samples exhibited superior oxidation resistance at high temperatures.A gradient structure with a fine-grain layer,a deformed-grain layer,and a coarse-grain layer was formed in the LSP-treated sample,which facilitated the diffusion of the Al atom during oxidation,leading to the formation of a dense Al_(2)O_(3)layer on the *** mechanism of improvement in the oxidation resistance of the as-deposited Ti45Al8Nb alloy via LSP was discussed.

关键词： TiAl alloy laser melting deposition laser shock peening additive manufacturing oxidation resistance

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A general stabilizing strategy based on vitamin C for n-type organic semiconductors

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science China materials 2025年第1期68卷 303-304页

作者： Hui Huang College of materials science and Opto-Electronic Technology Center of Materials Science and Optoelectronics EngineeringUniversity of Chinese Academy of SciencesBeijing 101408China

Organic semiconductors (OSCs), as an emerging next-generation semiconductor material, hold promising prospects in fields such as flexible displays, electronic skins, smart healthcare,and the Internet of Things, due to their excellent flexibility,solution processability, and tunable band structures [1,2]. These molecules are often classified into n-type and p-type, depending on whether the prevalent charge carriers are electrons or holes[3].

关键词： tunable semiconductors smart

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research progress of lignin-derived materials in lithium/sodium ion batteries

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Green Energy & Environment 2025年第2期10卷 322-344页

作者： Jingke Zhang Hengxue Xiang Zhiwei Cao Shichao Wang Meifang Zhu Institute of Hybrid materials National Center of International Research for Hybrid Materials TechnologyNational Base of International Science&Technology CooperationCollege of Materials Science and EngineeringQingdao UniversityQingdao266071China State Key Laboratory for Modification of Chemical Fibers and Polymer materials College of Materials Science and EngineeringDonghua UniversityShanghai201620China

With the increase of energy consumption,the shortage of fossil resource,and the aggravation of environmental pollution,the development of cost-effective and environmental friendly bio-based energy storage devices has become an urgent *** the second most abundant natural polymer found in nature,lignin is mainly produced as the by-product of paper pulping and bio-refining *** possesses several inherent advantages,such as low-cost,high carbon content,abundant functional groups,and bio-renewable,making it an attractive candidate for the rechargeable battery ***,there has been a surge of research interest in utilizing lignin or lignin-based carbon materials as the components of lithium-ion(LIBs)or sodium-ion batteries(SIBs),including the electrode,binder,separator,and *** review provides a comprehensive overview on the research progress of lignin-derived materials used in LIBs/SIBs,especially the application of lignin-based carbons as the anodes of LIBs/*** preparation methods and properties of lignin-derived materials with different dimensions are systemically discussed,which emphasizes on the relationship between the chemical/physical structures of lignin-derived materials and the performances of LIBs/*** current challenges and future prospects of lignin-derived materials in energy storage devices are also proposed.

关键词： Lignin-based carbons Lithium battery Sodium battery Chemical structure evolution

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Platinum modification of metallic cobalt defect sites for efficient electrocatalytic oxidation of 5-hydroxymethylfurfural

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Journal of Energy Chemistry 2025年第2期101卷 463-473页

作者： Haoyu Zhan Baixue Cheng Yankun Lu Danning Xing Xingshuai Lv Huining Huang Thomas Frauenheim Tao Wang Peng Zhou State Key Laboratory of Bio-fibers and Eco-textiles College of Materials Science and Engineering Collaborative Innovation Center of Shandong Marine Biobased Fibers and Ecological Textiles Institute of Marine Biobased Materials Qingdao University Shandong Institute of Advanced Technology College of Chemistry and Chemical engineering Ocean University of China Tianjin Key Laboratory of Advanced Functional Porous materials Institute for New Energy Materials & Low-Carbon Technologies School of Materials Science and EngineeringTianjin University of Technology School of science Constructor University Beijing Computational science research center College of Chemistry and Molecular engineering Qingdao University of Science and Technology

Co3O4possesses both direct and indirect oxidation effects and is considered as a promising catalyst for the oxidation of 5-hydroxymethylfurfural（HMF）.However,the enrichment and activation effects of Co3O4on OH-and HMF are weak,which limits its further *** defect engineering can regulate the electronic structure,optimize the adsorption of intermediates,and improve the catalytic activity by breaking the symmetry of the material,which is rarely involved in the upgrading of *** this work,we prepare Co3O4with metal defects and load the precious metal platinum at the defect sites（PtVco）.The results of in-situ characterizatio ns,electrochemical measurements,and theoretical calculations indicate that the reduction of Co-Co coordination number and the formation of Pt-Co bond induce the decrease of electron filling in the antibonding orbitals of Co *** resulting upward shift of the d-band center of Co combined with the characteristic adsorption of Pt species synergically enhances the enrichment and activation of organic molecules and OH species,thus exhibiting excellent HMF oxidation activity(including a lower onset potential（1.14 V） and 19 times higher current density than pure Co3O4at 1.35 V).In summary,this work explores the adsorption enhancement mechanism of metal defect sites modified by precious metal in detail,provides a new option for improving the HMF oxidation activity of cobalt-based materials,broadens the application field of metal defect based materials,and gives an innovative guidance for the functional utilization of metal defect sites in biomass conversion.

关键词： Adsorption enhancement Biomass upgrading Coordination environment Electrocatalysis Metallic defect

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Modification of polypropylene separator with multifunctional layers to achieve highly stable sodium metal anode

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Journal of Energy Chemistry 2025年第2期101卷 223-232页

作者： Aadil Nabi Chishti Sikandar Iqbal Muhammad Ali Moazzam Ali Samia Aman Hamid Hussain Muhammad Yousaf Yinzhu Jiang Future science research Institute ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang University School of materials science and engineering Zhejiang University School of Chemistry Zhejiang University

Separator modification is an effective approach to suppress dendrite growth to realize high-energy sodium metal batteries（SMBs） in practical applications,however,its success is mainly subject to surface ***,a separator with multifunctional layers composed of N-doped mesoporous hollow carbon spheres（HCS） as the inner layer and sodium fluoride（NaF） as the outer layer on commercial polypropylene separator（PP） is proposed（PP@HCS-NaF） to achieve stable cycling in *** the molecular level,the inner HCS layer with a high content of pyrrolic-N induces the uniform Na+flux as a potential Na+redistributor for homogenous deposition,whereas its hollow mesoporous structure offers nanoporous buffers and ion channels to regulate Na+ion distribution and uniform *** outer layer（NaF） constructs the NaF-enriched robust solid electrolyte interphase layer,significantly lowering the Na+ions diffusion *** from these merits,higher electrochemical performances are achieved with multifunctional double-layered PP@HCS-NaF separators compared with single-layered separators（***@HCS or PP@NaF） in *** Na‖Cu half-cell with PP@HCS-NaF offers stable cycling（280 cycles）with a high CE（99.6%）,and Na‖Na symmetric cells demonstrate extended lifespans for over 6000 h at 1 mA cm-2with a progressively stable overpotential of 9 ***,in Na‖NVP full-cells,the PP@HCS-NaF separator grants a stable capacity of ～81 mA h g-1after 3500 cycles at 1 C and an impressive rate capability performance(～70 mA h g-1at 15 C).

关键词： Enhanced cyclic stability Multifunctional layers NaF-enriched SEI layer Separator modification Sodium metal batteries

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Constructing electrochemically stable single crystal Ni-rich cathode material via modification with high valence metal oxides

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Journal of Energy Chemistry 2025年第02期101卷 392-401页

作者： Hancheng Shi Jiongzhi Zheng Tao Wan Hongqiang Wang Zeping Wen Fenghua Zheng Mingru Su Aichun Dou Yu Zhou Ahmad Naveed Panpan Zhang Hailong Wang Ruiqiang Guo Yunjian Liu Dewei Chu School of Material science and engineering Jiangsu University Thayer School of engineering Dartmouth College School of materials science and engineering The University of New South Wales School of Chemistry and Pharmaceutical sciences Guangxi Normal University School of materials and New Energy Ningxia University Thermal science research center Shandong Institute of Advanced Technology

Single crystal Ni-rich cathode materials（SCNCM） are a good supplement in the market of nickel-based materials due to their safety and excellent electrochemical ***,the challenges of cation mixing,phase change during charge/discharge,and low thermal stability remain unresolved in single crystal *** address these issues,SCNCM are rationally modified by incorporating transition metal（TM） oxides,and the influence of metal ions with different valence states on the electrochemical properties of SCNCM is methodically explored through experimental results and theoretical *** structural stability is demonstrated in SCNCM after the modifications,and the degree of improvement in the matrix materials varies depending on the valence state of doped TM *** highest structural stability is found in WO3-modified SCNCM,due to the smaller effective ion radii,higher electro-negativity,stronger W-O bond,and efficient suppression of oxygen vacancy *** a result,WO3-modified SCNCM have outstanding cycle performance,with a capacity retention rate of90.2% after 200 *** study provides an insight into the design of advanced SCNCM with enhanced reversibility and cyclability.

关键词： In-situ coating Ion doping Lithium-ion battery Single crystal Ni-rich material Strengthening mechanism analysis

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Unveiling solid-solid contact states in all-solid-state lithium batteries:An electrochemical impedance spectroscopy viewpoint

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Journal of Energy Chemistry 2025年第2期101卷 16-22页

作者： Jin-Liang Li Liang Shen Zi-Ning Cheng Jun-Dong Zhang Ling-Xuan Li Yu-Tong Zhang Yan-Bin Gao Chunli Guo Xiang Chen Chen-Zi Zhao Rui Zhang Qiang Zhang Tsinghua center for Green Chemical engineering Electrification Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical Engineering Tsinghua University College of materials science and engineering Taiyuan University of Technology Advanced research Institute of Multidisciplinary science School of Materials Science and Engineering Beijing Institute of Technology Beijing Huairou Laboratory Institute for Carbon Neutrality Tsinghua University Shanxi research Institute for Clean Energy Tsinghua University

All-solid-state lithium batteries（ASSLBs） are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic *** solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs,which is challenging to investigate quantitatively by experimental *** work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in *** the assistance of an equivalent circuit model and distribution of relaxation times,it is discovered that as the number of voids and the sharpness of cracks increase,the contact resistance Rcgrows and ultimately dominates the battery *** accurate fitting,inverse proportional relations between contact resistance Rcand（1-porosity） as well as crack angle was *** contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.

关键词： All-solid-state lithium batteries Distribution of relaxation times Electrochemical impedance spectroscopy Equivalent circuit model Finite element method Solid-solid contacts

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