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High‑Entropy Electrode Materials:Synthesis,Properties and Outlook

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Nano-Micro Letters 2025年第1期17卷 472-506页

作者： Dongxiao Li Chang Liu Shusheng Tao Jieming Cai Biao Zhong Jie Li Wentao Deng Hongshuai Hou Guoqiang Zou Xiaobo Ji College of chemistry and chemical engineering Central South UniversityChangsha 410083People’s Republic of China School of chemistry and chemical engineering Hunan Institute of EngineeringXiangtan 411104People’s Republic of China

High-entropy materials represent a new category of high-performance materials,first proposed in 2004 and extensively investigated by researchers over the past two *** definition of high-entropy materials has continuously *** the last ten years,the discovery of an increasing number of high-entropy materials has led to significant advancements in their utilization in energy storage,electrocatalysis,and related domains,accompanied by a rise in techniques for fabricating high-entropy electrode ***,the research emphasis has shifted from solely improving the performance of high-entropy materials toward exploring their reaction mechanisms and adopting cleaner preparation ***,the current definition of high-entropy materials remains relatively vague,and the preparation method of high-entropy materials is based on the preparation method of single metal/low-or medium-entropy *** should be noted that not all methods applicable to single metal/low-or medium-entropy materials can be directly applied to high-entropy *** this review,the definition and development of high-entropy materials are briefly ***,the classification of high-entropy electrode materials is presented,followed by a discussion of their applications in energy storage and catalysis from the perspective of synthesis ***,an evaluation of the advantages and disadvantages of various synthesis methods in the production process of different high-entropy materials is provided,along with a proposal for potential future development directions for high-entropy materials.

关键词： High-entropy Energy storage Electrode materials

Defect engineering:Can it Mitigate Strong Coulomb Effect of Mg^(2+)in Cathode Materials for Rechargeable Magnesium Batteries?

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Nano-Micro Letters 2025年第1期17卷 135-159页

作者： Zhengqing Fan Ruimin Li Xin Zhang Wanyu Zhao Zhenghui Pan Xiaowei Yang School of chemistry and chemical engineering Shanghai Jiao Tong UniversityShanghai 200240People’s Republic of China School of chemistry and chemical engineering Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China School of Materials Science and engineering Tongji UniversityShanghai 201804People’s Republic of China

Rechargeable magnesium batteries(RMBs)have been considered a promising“post lithium-ion battery”system to meet the rapidly increasing demand of the emerging electric vehicle and grid energy storage ***,the sluggish diffusion kinetics of bivalent Mg^(2+)in the host material,related to the strong Coulomb effect between Mg^(2+)and host anion lattices,hinders their further development toward practical *** engineering,regarded as an effective strategy to break through the slow migration puzzle,has been validated in various cathode materials for *** this review,we first thoroughly understand the intrinsic mechanism of Mg^(2+)diffusion in cathode materials,from which the key factors affecting ion diffusion are further ***,the positive effects of purposely introduced defects,including vacancy and doping,and the corresponding strategies for introducing various defects are *** applications of defect engineering in cathode materials for RMBs with advanced electrochemical properties are also ***,the existing challenges and future perspectives of defect engineering in cathode materials for the overall high-performance RMBs are described.

关键词： Rechargeable magnesium battery Sluggish diffusion kinetic Defect engineering Cathode materials Ion migration

In situ polymerization of poly(3,4-ethylenedioxythiophene)protective layer towards stable zinc anode

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Nano Research 2025年第1期18卷 382-394页

作者： Debin Luo Peng Zhou Xiaowei Lv Panpan Sun Xiaohua Sun Hewei Zhao College of Materials and chemical engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion MaterialsChina Three Gorges UniversityYichang 443002China Hubei Three Gorges Laboratory Yichang 443007China School of chemistry Beihang UniversityBeijing 100191China

Aqueous zinc-ion devices are considered promising candidates for energy storage due to their high safety,low cost and relatively high energy ***,the dendrite growth,hydrogen evolution reaction(HER)and corrosion of the zinc anode significantly limit the development of Zn-ion ***,an inexpensive poly(3,4-ethylenedioxythiophene)(PEDOT)protective layer was constructed in situ on the Zn surface using electropolymerization to suppress dendrite growth and side reactions,thereby enhancing the reversibility of *** and theoretical calculations revealed that this hydrophilic protective layer promotes the desolvation process of hydrated Zn^(2+)and facilitates the transport of zinc ions,thus improving the thermodynamic and kinetic properties of Zn^(2+)deposition and inhibiting interfacial side ***,the optimized PEDOT@Zn symmetric battery exhibited a cycling stability exceeding 1250 h at 0.5 mA·cm^(-2)and 0.25 mAh·cm^(-2),with a significantly reduced overpotential(from 91.8 to 35 mV).With the assistance of the PEDOT protective layer,the PEDOT@Zn//Cu battery maintained approximately 99.5%Coulombic efficiency after 450 ***-situ scanning electron microscopy(SEM)and in situ optical microscopy characterizations further confirmed that the PEDOT protective layer can effectively suppress the growth of zinc ***,the Zn-ion capacitors assembled by the PEDOT@Zn and activated carbon also demonstrated outstanding cycling stability.

关键词： zinc-ion devices zinc anode poly(3 4-ethylenedioxythiophene)(PEDOT) dendrite desolvation process

Trinuclear gold-catalyzed site-selective alkylation of peptides

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Science China chemistry 2025年第01期 249-256页

作者： Qing-Yun Fang Chengyihan Gu Yinghan Chen Wencheng Yan Yong Liang Weipeng Li Chengjian Zhu Jie Han Jin Xie State Key Laboratory of Coordination chemistry Jiangsu Key Laboratory of Advanced Organic Materials Chemistry and Biomedicine Innovation Center (Chem BIC) School of Chemistry and Chemical Engineering Nanjing University Green Catalysis Center College of Chemistry Zhengzhou University State Key Laboratory of Natural Medicines China Pharmaceutical University

Selective modification of peptides has always been a challenging issue. The selective alkylation of peptides can alter the biological activity and physical properties of molecules, and it has gained significant research interest. We herein disclose an intriguing gold-catalyzed alkylation of peptides using bench-stable unactivated alkyl bromides under photoredox catalysis. A wide range of structurally diverse primary, secondary and tertiary alkyl bromides serve as effective coupling partners to precisely connect with the α-C(sp3)–H in glycine residue of peptides. This protocol demonstrates an exceptionally broad scope for alkyl halides and excellent tolerance for a wide range of useful functional groups. A series of relay transformations to construct cyclic peptides, to proceed click reaction and to realize peptide fluorescence labeling further enhance its synthetic practicality. In addition, mechanistic studies and density functional theory(DFT) calculations reveal an inner-sphere and subsequent outersphere single electron transfer(SET) mechanism.

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Molecular Structure Tailoring of Organic Spacers for High‑Performance Ruddlesden–Popper Perovskite Solar Cells

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Nano-Micro Letters 2025年第2期17卷 314-357页

作者： Pengyun Liu Xuejin Li Tonghui Cai Wei Xing Naitao Yang Hamidreza Arandiyan Zongping Shao Shaobin Wang Shaomin Liu School of Materials Science and engineering State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum(East China)Qingdao 266580People’s Republic of China School of chemistry and chemical engineering Shandong University of TechnologyZibo 255049People’s Republic of China Centre for Applied Materials and Industrial chemistry(CAMIC) School of ScienceRMIT UniversityMelbourneVic 3000Australia WA School of Mines:Minerals Energy and Chemical Engineering(WASM‑MECE)Curtin UniversityPerthWA 6102Australia School of chemical engineering The University of AdelaideAdelaideSA 5005Australia School of engineering Great Bay UniversityDongguan 523000People’s Republic of China

Layer-structured Ruddlesden–Popper(RP)perovskites(RPPs)with decent stability have captured the imagination of the photovoltaic research community and bring hope for boosting the development of perovskite solar cell(PSC)***,two-dimensional(2D)or quasi-2D RP PSCs are encountered with some challenges of the large exciton binding energy,blocked charge transport and poor film quality,which restrict their photovoltaic ***,these issues can be readily resolved by rationally designing spacer cations of *** review mainly focuses on how to design the molecular structures of organic spacers and aims to endow RPPs with outstanding photovoltaic *** firstly elucidated the important roles of organic spacers in impacting crystallization kinetics,charge transporting ability and stability of *** we brought three aspects to attention for designing organic ***,we presented the specific molecular structure design strategies for organic spacers of RPPs aiming to improve photovoltaic performance of RP *** proposed strategies in this review will provide new avenues to develop novel organic spacers for RPPs and advance the development of RPP photovoltaic technology for future applications.

关键词： Ruddlesden-Popper perovskites Low-dimensional perovskite solar cells Organic spacers Molecular structure Design strategies

Low‑Temperature Oxidation Induced Phase Evolution with Gradient Magnetic Heterointerfaces for Superior Electromagnetic Wave Absorption

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Nano-Micro Letters 2025年第1期17卷 191-204页

作者： Zizhuang He Lingzi Shi Ran Sun Lianfei Ding Mukun He Jiaming Li Hua Guo Tiande Gao Panbo Liu School of chemistry and chemical engineering Northwestern Polytechnical UniversityXi’an 710129People’s Republic of China School of Marine Science and Technology Northwestern Polytechnical UniversityXi’an 710072People’s Republic of China

Gradient magnetic heterointerfaces have injected infinite vitality in optimizing impedance matching,adjusting dielectric/magnetic resonance and promoting electromagnetic(EM)wave absorption,but still exist a significant challenging in regulating local phase ***,accordion-shaped Co/Co_(3)O_(4)@N-doped carbon nanosheets(Co/Co_(3)O_(4)@NC)with gradient magnetic heterointerfaces have been fabricated via the cooperative high-temperature carbonization and lowtemperature oxidation *** results indicate that the surface epitaxial growth of crystal Co_(3)O_(4) domains on local Co nanoparticles realizes the adjustment of magnetic-heteroatomic components,which are beneficial for optimizing impedance matching and interfacial ***,gradient magnetic heterointerfaces simultaneously realize magnetic coupling,and long-range magnetic ***,the synthesized Co/Co_(3)O_(4)@NC absorbents display the strong electromagnetic wave attenuation capability of−53.5 dB at a thickness of 3.0 mm with an effective absorption bandwidth of 5.36 GHz,both are superior to those of single magnetic domains embedded in carbon *** design concept provides us an inspiration in optimizing interfacial polarization,regulating magnetic coupling and promoting electromagnetic wave absorption.

关键词： Magnetic heterointerfaces Phase evolution Interfacial polarization Magnetic coupling Electromagnetic wave absorption

CaH2-promoted activity of Ni-carbonate interface for CO2 methanation

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Journal of Energy chemistry 2025年第01期 522-532页

作者： Jin-Peng Wang Guo-Cui Mao Hui-Lin Jiang Bao-Xia Dong Yun-Lei Teng School of chemistry and chemical engineering Yangzhou University

Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic *** interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO2hydrogenation reaction,involving surface carbonate hydrogenation and ***,there have been few reports on engineering the activity of the interface between transition metal and alkaline earth metal carbonate for catalytic *** work demonstrated that the incorporation of CaH2in Ni/CaCO3enhances the CO2methanation activity of the *** CO2conversion for Ni/CaH2-CaCO3reached 68.5%at 400°C,which was much higher than that of the Ni/CaCO3（31.6%） and Ni/CaH2-CaO （42.4%） ***,the Ni/CaH2-CaCO3catalysts remained stable during the stability test for 24 h at 400°C and 8 *** research revealed that CaH2played a crucial role in promoting the activity of the Ni-carbonate interface for ***2could modify the electronic structure of Ni and tune the structural properties of CaCO3to generate medium basic sites （OH groups）,which are favorable for the activation of H2and ***-situ Fourier transform infrared spectroscopy （FTIR） analysis combined with density functional theory calculations demonstrated that CO2activation occurs at the hydroxyl group （OH） on the CaH2-modified Ni-carbonate surface,leading to the formation of CO3H****,our study has confirmed that CO2methanation over the Ni/CaH2-CaCO3catalysts proceeds via the formate pathway.

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Advancements and Challenges in Organic–Inorganic Composite Solid Electrolytes for All‑Solid‑State Lithium Batteries

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Nano-Micro Letters 2025年第1期17卷 46-97页

作者： Xueyan Zhang Shichao Cheng Chuankai Fu Geping Yin Liguang Wang Yongmin Wu Hua Huo State Key Laboratory of Space Power‑Sources School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001People’s Republic of China College of chemical and Biological engineering Zhejiang UniversityHangzhou 310058People’s Republic of China State Key Laboratory of Space Power-Sources 2965 Dongchuan RoadMinhang DistrictShanghai 200240People’s Republic of China

To address the limitations of contemporary lithium-ion batteries,particularly their low energy density and safety concerns,all-solid-state lithium batteries equipped with solid-state electrolytes have been identified as an up-and-coming *** the various SEs,organic–inorganic composite solid electrolytes(OICSEs)that combine the advantages of both polymer and inorganic materials demonstrate promising potential for large-scale ***,OICSEs still face many challenges in practical applications,such as low ionic conductivity and poor interfacial stability,which severely limit their *** review provides a comprehensive overview of recent research advancements in ***,the influence of inorganic fillers on the main functional parameters of OICSEs,including ionic conductivity,Li+transfer number,mechanical strength,electrochemical stability,electronic conductivity,and thermal stability are systematically *** lithium-ion conduction mechanism of OICSE is thoroughly analyzed and concluded from the microscopic ***,the classic inorganic filler types,including both inert and active fillers,are categorized with special emphasis on the relationship between inorganic filler structure design and the electrochemical performance of ***,the advanced characterization techniques relevant to OICSEs are summarized,and the challenges and perspectives on the future development of OICSEs are also highlighted for constructing superior ASSLBs.

关键词： Composite solid electrolytes Inorganic filler Interfacial stability Li-ion conduction mechanism Characterization techniques

基于共价有机框架的分子工程高效光催化CO2还原为CO（英文）

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Science China Materials 2025年第01期 165-172页

作者：赵文玲孙磊杨丽张瑞玲任国庆王森吴昊康欣晨邓伟侨刘乘乘 Institute of Frontier chemistry School of Chemistry and Chemical Engineering Shandong University Beijing National Laboratory for Molecular Sciences Key Laboratory of Colloid and Interface and Thermodynamics Institute of Chemistry Chinese Academy of Sciences College of chemistry Chemical Engineering and Resource Utilization Northeast Forestry University State Key Laboratory of Microbial Technology Shandong University

共价有机框架广泛应用于光催化CO2还原中.然而,它们在分离光生载流子方面的效率有限,且催化位点较少,因此其光催化性能有待提高.本文利用分子工程设计了一种芘基共价有机框架（PyTa-H COF）,并将钴单原子（Co SACs）负载在COF骨架中用...

共价有机框架广泛应用于光催化CO2还原中.然而,它们在分离光生载流子方面的效率有限,且催化位点较少,因此其光催化性能有待提高.本文利用分子工程设计了一种芘基共价有机框架（PyTa-H COF）,并将钴单原子（Co SACs）负载在COF骨架中用于二氧化碳还原.在COF中,芘基团可以增强可见光捕获能力和电荷分离能力, Co SACs可以加速光生载流子的迁移及降低决速步的反应能垒.在可见光照射下,PyTa-H@Co在4小时内的CO产率为18.36 mmol g-1h-1,选择性为94%,其性能与目前报道的COFs的最佳性能相当.密度泛函理论计算表明,Co SACs稳定了*COOH中间体,并大大降低了决定性步骤的能垒,从而获得了优异的光催化性能.本工作通过分子工程设计,突出了催化剂结构和功能在提高光催化效率方面的重要作用.

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