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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 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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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 Pr-doped CoOOH catalytic sites for efficient electrooxidation of 5-hydroxymethylfurfural

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Journal of Energy Chemistry 2025年第1期100卷 234-244页

作者： Botao Fan Hao Zhang Bang Gu Feng Qiu Qiue Cao Wenhao Fang School of Chemical science and Technology Yunnan UniversityKunming 650091YunnanChina National center for International research on Photoelectric and Energy materials School of Materials and EnergyYunnan UniversityKunming 650091YunnanChina

Electrocatalytic conversion of renewable biomass is emerging as a promising route for sustainable chemical production;hence it urgently calls for developing efficient electrocatalysts with low potentials and high current ***,a Pr-doped Co(OH)_(2)hexagonal sheet(Pr/Co=1/9,in mole)is synthesized by electrodeposition as highly performant catalyst for 5-hydroxymethylfurfural(HMF)oxidation reaction(HMFOR)to produce 2,5-furandicarboxylic acid(FDCA).This novel and low-cost catalyst possesses a rather low onset potential of 1.05 V(***)and requires only 1.10 V(***)to reach a current density of 10 mA cm^(-2)for HMFOR,significantly outperforming Co(OH)_(2)benchmark(i.e.,210 mV higher to reach10 m A cm^(-2)).The origin of Pr promotion effect as well as the evolution of CoOOH catalytic sites and HMFOR process has been deeply elucidated by physical characterizations,kinetic experiments,in situ electrochemical techniques,and theoretical *** unique Pr-ameliorated CoOOH active centers enable 100%conversion of HMF,99.6%selectivity of FDCA,and 99.7%Faraday efficiency,with a superior cycling durability toward *** can be one of the most outstanding results for Co-based HMFOR catalysts to date in the *** this work can help open up new horizons for constructing novel and efficient Co-based electrocatalysts by the utilization of lanthanide elements.

关键词： Biomass conversion Electrocatalysis 2,5-Furandicarboxylic acid Doped Co catalyst Co3+active sites Charge transfer rate

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Decoupling the roles of grain boundary strength and grain size hidden in grain-level electro-chemo-mechanical failure of solid-state electrolyte

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Journal of Energy Chemistry 2025年第2期101卷 685-691页

作者： Ming Xu Xuyang Wang Zhengqian Jin Xingxing Jiao Ya Gao Zhongxiao Song Xieyu Xu Kai Xi Yangyang Liu School of Chemistry Engineering Research Center of Energy Storage Materials and Devices Ministry of Education Xi'an Jiaotong University State Key Laboratory for Mechanical Behavior of materials Xi'an Jiaotong University research Institute of Frontier science Southwest Jiaotong University School of Instrument science and Technology Xi'an Jiaotong University

Garnet lithium lanthanum zirconium oxide(Li7La3Zr2O12,LLZO) is a benchmark solid-state electrolyte（SSE） material receiving considerable attention owing to its high conductivity and chemical stability against Li *** its electro-chemo-mechanical failure mechanisms have been much investigated,the equivocal roles of grain boundary strength and grain size of LLZO remain under-explored,hindering further performance *** we decoupled the effects of grain size and grain boundary strength of polycrystalline LLZO via the combination of electrochemical kinetics and the cohesive zone *** discovered that the disintegration of LLZO is initiated by the accumulation of local displacements,which strongly relates to the changes in both grain size and grain boundary ***,variations in grain boundary strength affect the diffusion and propagation pathways of damage,while the failure of LLZO is determined by the grain *** LLZO grains facilitate transgranular damage under low grain boundary strength,which can alter local chemo-mechanics within the bulk of LLZO,leading to more extensive damage *** results showcase the structure optimization pathways by preferentially controlling the growth of lithium dendrites at grain boundaries and their penetration in garnet-type SSE.

关键词： Electro-chemo-mechanics Grain boundary Growth of lithium metal Solid-state electrolyte

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Na_(2)B_(6)SO_(13) with unprecedented [B_(6)SO_(13)]_(∞) double chains and largest birefringence among borosulfates induced by the uniform arrangement of [B_(3)O_(7)] units

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science China Chemistry 2025年第2期68卷 475-480页

作者： Jinbin Fan Ziting Yan Zilong Chen Huimin Li Zhihua Yang Fangfang Zhang Shilie Pan research center for Crystal materials State Key Laboratory of Functional Materials and Devices for Special Environmental ConditionsXinjiang Key Laboratory of Functional Crystal MaterialsXinjiang Technical Institute of Physics and ChemistryChinese Academy of SciencesUrumqi 830011China center of materials science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Birefringence is crucial for birefringent crystals to modulate polarized light and nonlinear optical crystals to enable *** is closely related to the arrangement of advantageous functional groups with large microcosmic polarizability anisotropy in the ***,designing crystals with large birefringence by modulating the arrangement of advantageous functional groups is still a *** this work,the arrangement of the advantageous[B_(3)O_(7)]groups is optimized by introducing rigid tetrahedral[SO_(4)]groups,resulting in a novel boron-rich borosulfate,Na_(2)B_(6)SO_(13) ,which exhibits unprecedented[B_(6)SO_(13)]_(∞)double chain and an enhanced birefringence(Δn=0.07 at 589.3 nm)against the borate parent *** calculations confirm that the birefringence is mainly attributable to the uniform alignment of[B_(3)O_(7)]***_(2)B_(6)SO_(13) also possesses a deep ultraviolet(DUV)cutoff edge(λ<185 nm).This work provides a feasible method to design DUV birefringent crystals with large birefringence by inducing the arrangement of advantageous functional groups.

关键词： borosulfate deep ultraviolet birefringence modulated groups

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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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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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