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

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

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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

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Gradient‑Layered MXene/Hollow Lignin Nanospheres Architecture Design for Flexible and Stretchable Supercapacitors

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Nano-Micro Letters 2025年第2期17卷 447-462页

作者： Haonan Zhang Cheng Hao Tongtong Fu Dian Yu Jane Howe Kaiwen Chen Ning Yan Hao Ren Huamin Zhai Jiangsu Provincial Key Lab of Sustainable Pulp and Paper Technology and Biomass Materials NanJing Forestry UniversityNanjing 210037People’s Republic of China Department of chemical engineering and Applied chemistry University of Toronto200 College StreetTorontoON M5S 3E5Canada Department of Materials Science and engineering University of Toronto184 College StreetTorontoON M5S 3E4Canada college of Materials Science and engineering Nanjing Forestry UniversityNanjing 210037People’s Republic of China

With the rapid development of flexible wearable electronics,the demand for stretchable energy storage devices has *** this work,a novel gradient-layered architecture was design based on single-pore hollow lignin nanospheres(HLNPs)-intercalated two-dimensional transition metal carbide(Ti_(3)C_(2)T_(x) MXene)for fabricating highly stretchable and durable *** depositing and inserting HLNPs in the MXene layers with a bottom-up decreasing gradient,a multilayered porous MXene structure with smooth ion channels was constructed by reducing the overstacking of MXene ***,the micro-chamber architecture of thin-walled lignin nanospheres effectively extended the contact area between lignin and MXene to improve ion and electron accessibility,thus better utilizing the pseudocapacitive property of *** these strategies effectively enhanced the capacitive performance of the *** addition,HLNPs,which acted as a protective phase for MXene layer,enhanced mechanical properties of the wrinkled stretchable electrodes by releasing stress through slip and deformation during the stretch-release cycling and greatly improved the structural integrity and capacitive stability of the *** electrodes and symmetric flexible all-solid-state supercapacitors capable of enduring 600%uniaxial tensile strain were developed with high specific capacitances of 1273 mF cm^(−2)(241 F g^(−1))and 514 mF cm^(−2)(95 F g^(−1)),***,their capacitances were well preserved after 1000 times of 600%stretch-release *** study showcased new possibilities of incorporating biobased lignin nanospheres in energy storage devices to fabricate stretchable devices leveraging synergies among various two-dimensional nanomaterials.

关键词： Hollow lignin nanospheres MXene Gradient-layered architecture Wrinkled electrodes Stretchable supercapacitors

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Catalytic atroposelective synthesis of indolyl quinazolinones bearing N-N/C-C diaxes

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Science China chemistry 2025年

作者： Ning-Yi Wang Shuo Gao Zhu-Di Shu Bei-Bei Cheng Chun Ma Yu-Chen Zhang Feng Shi Research Center of Chiral Functional Heterocycles School of Chemistry and Materials Science Jiangsu Normal University School of Petrochemical engineering Changzhou University School of chemistry and chemical engineering Henan Normal University

The first catalytic atroposelective synthesis of indole derivatives bearing N-N/C-C diaxes has been established by the strategy of de novo ring formation. By this strategy, various indolyl quinazolinones bearing vicinal N-N/C-C diaxes were synthesized in high yields with overall good diastereoselectivities and excellent enantioselectivities via chiral phosphoric acid-catalyzed onepot asymmetric formal (5+1) cycloaddition/oxidation reaction. Moreover, such indolyl quinazolinones bearing vicinal N-N/CC diaxes have good configurational stability and could be converted into new chiral ligands with applications in asymmetric catalysis. Therefore, this work not only offered a new member for the family of diaxial atropisomers, but also provided a powerful strategy for catalytic asymmetric synthesis of atropisomers bearing N-N/C-C diaxes.

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An Efficient Boron Source Activation Strategy for the Low‑Temperature Synthesis of Boron Nitride Nanotubes

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Nano-Micro Letters 2025年第1期17卷 548-558页

作者： Ying Wang Kai Zhang Liping Ding Liyun Wu Songfeng E Qian He Nanyang Wang Hui Zuo Zhengyang Zhou Feng Ding Yue Hu Jin Zhang Yagang Yao National Laboratory of Solid State Microstructures College of Engineering and Applied SciencesJiangsu Key Laboratory of Artificial Functional Materialsand Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210093People’s Republic of China School of Electronic Information and Artificial Intelligence Shaanxi University of Science&TechnologyXian 710000People’s Republic of China college of Bioresources chemical and Materials engineering Shaanxi University of Science&TechnologyXian 710000People’s Republic of China Key Laboratory of Carbon Materials of Zhejiang Province College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325000People’s Republic of China Shenzhen Institutes of Advanced Technology Chinese Academy of SciencesShenzhen 518000People’s Republic of China college of chemical and Molecular engineering Peking UniversityBeijing 100871People’s Republic of China

Lowering the synthesis temperature of boron nitride nanotubes(BNNTs)is crucial for their *** primary reason for adopting a high temperature is to enable the effective activation of highmelting-point solid *** this study,we developed a novel approach for efficiently activating boron by introducing alkali metal compounds into the conventional MgO–B *** approach can be adopted to form various low-melting-point AM–Mg–B–O growth *** growth systems have improved catalytic capability and reactivity even under low-temperature conditions,facilitating the synthesis of BNNTs at temperatures as low as 850℃.In addition,molecular dynamics simulations based on density functional theory theoretically demonstrate that the systems maintain a liquid state at low temperatures and interact with N atoms to form BN *** findings offer novel insights into the design of boron activation and are expected to facilitate research on the low-temperature synthesis of BNNTs.

关键词： Boron nitride nanotubes Low-temperature Boron activation Density functional theory

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Oxygen vacancies enriched Ir/WOx catalysts for the directly chem-catalytic conversion of cellulose to ethanol

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Tungsten 2025年第1期7卷 88-99页

作者： Yu-Jing Weng Zhao-Ying Ding Ying-Chao Li Yuan-Feng Wu Yuan-Yang Xu Rui Chen Xiao-Lei Zhao Hai-Yong Wang Da-Lei Zhang Yu-Long Zhang Henan Key Laboratory of Coal Green Conversion and International Joint Laboratory of Coal Clean Utilization College of Chemistry and Chemical Engineering Henan Polytechnic University Key Laboratory of Renewable Energy Guangzhou Institute of Energy Conversion Chinese Academy of Sciences Liaoning Institute of Energy Technology

Tungsten and its oxides are highly versatile catalysts with unique properties that hold great promise for a wide array of applications,including biological pathways and chemical *** chemo-catalysis of cellulose to ethanol presents a promising avenue for ethanol synthesis with the potential for enhanced efficiency compared to conventional methods,offering a sustainable and carbon-neutral alternative to existing petrochemical and biological ***,Ir/WOxcatalysts enriched with oxygen vacancies were meticulously prepared and demonstrated remarkable catalytic performance in converting cellulose to ethanol directly in the presence of tungstic *** catalyst achieved a high ethanol yield of 66.5%under optimal reaction conditions,approaching the theoretical yield limit of traditional ethanol *** results revealed the presence of oxygen defects,Bronsted/Lewis acidity,and Ir nanoclusters on the catalyst surface,working synergistically to facilitate the cascade catalysis of cellulose hydrolysis,sugar retro-aldol condensation reaction,and C2 intermediate hydrodeoxygenation to *** situ Fourier transform infrared spectrometer analysis confirmed the catalyst's ability to enhance the adsorption and activation of ethylene glycol for ethanol *** manipulating subtle structural features,this study offers a fresh perspective on tungsten group catalyst design and underscores the importance of synergistic effects among catalytic sites for the efficient production of ethanol from cellulose.

关键词： Cellulosic ethanol Chem-catalysis Hydrogenolysis Retro-aldol condensation Tungsten

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Electrochemical conversion of methane to bridge the gap in the artificial carbon cycle

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Journal of Energy chemistry 2025年第1期100卷 286-308页

作者： Yuhao Peng Yuefeng Song Ihar Razanau Juanxiu Xiao Wei Xiao Di Hu Guoxiong Wang college of chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University State Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics Chinese Academy of Sciences Laboratory of Physical-chemical Technologies SSPA Scientific and Practical Materials Research Centre of NAS of Belarus State Key Laboratory of Marine Resources Utilization in South China Sea Collaborative Innovation Center of Marine Science and Technology School of Marine Science and Engineering Hainan University Department of chemical and Environmental engineering University of Nottingham Ningbo China

Methane, an abundant one-carbon（C1） resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO2emissions and coke deposition. Electrochemical conversion of methane（ECM） using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO2emission.

关键词： Activation energy

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Polybenzimidazolium-reinforced polyimide separators to inhibit dendrites for high-security lithium-ion batteries

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Science China chemistry 2025年

作者： Guohua Sun Jiaqi Cui Qingsong Zhang Yisong Zhou Xinluo Li Yingying Zhang Zhanao Zhang Xin Zhang Jiantao Fan Pengpeng Li Lianlong Hou Nanjun Chen Hebei Key Laboratory of Flexible Functional Materials School of Materials Science and Engineering Hebei University of Science and Technology State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Academy for Advanced Interdisciplinary Studies Southern University of Science and Technology State Key Laboratory of Physical chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University

Lithium dendrite formation poses a significant safety hazard in lithium-ion batteries（LIBs）, severely impeding their widespread adoption and further technological advancements. Here, we present a novel quaternized polybenzimidazolium（q-PBI） to armor polyimide（PI） nanofiber separator（q-PBI@PI）, in which the q-PBI containing lithiophilicity and anionphilicity sites serves as the multifunctional nano-layers to suppress the Li dendrite and reinforce the mechanical properties of PI nanofiber ***, the q-PBI@PI separator displays an unprecedented mechanical strength of 82.8 MPa, significantly outperforming previously reported PI nanofiber membranes（typically below 50.0 MPa）. Besides, we demonstrate that the q-PBI@PI separator simultaneously possesses low nucleation overpotential（59 mV） and exceptional average coulombic efficiency due to the suppression of Li dendrite. Importantly, q-PBI@PI-based Li||Li battery enables a stable Li plating-stripping at 1.0 m A cm-2for600 h. Attributing to these exceptional merits, the armored PI separator-based LIBs display remarkable specific capability and capacity retention. The density function theory calculations reveal that q-PBI is conducive to the desolvation of Li+and can immobilize Li+and PF6-ions near affinity sites of PI nanofibers for inhibiting the formation of Li dendrites. Our work paves a new avenue for the design of next-generation high-performing separators in LIBs.

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Rise of β-furanosyl ribonucleosides as the extant RNA component facilitated by simple divalent transition-metal minerals

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Science China chemistry 2025年

作者： Qianqian Chen Haoxing Xu Bingyue Zhao Yeersen Patehebieke Zerun Zhao Xiao Wang School of chemistry and chemical engineering Nanjing University Frontiers Science Center for Critical Earth Material Cycling Nanjing University

The selective nucleoside synthesis through direct condensation between nucleobase and unactivated sugar in aqueous media has long been a formidable obstacle for the early chemical transformations hypothesized to construct the RNAWorld, due to product complexity and the low selectivity of the desired isomer. The preference of β-furanoside, the extant RNA component, has never been documented. Here we report an aqueous ribosylation mediated by divalent transition-metal ions, which unprecedentedly enhances the selectivity of furanosyl ribonucleosides as opposed to the traditionally predominating pyranosyl ones, with the furanoside/pyranoside ratio reaching up to 9/1. Furthermore, β-furanoside stands out for the first time as the most prevalent isomer in the presence of zinc and ammonium salts. The mechanism of this selectivity is elucidated with density functional theory calculations. The selectivity for β-furanoside can be further elevated via the adsorption on a zinc mineral. These findings exhibit as the first example that the selection of nucleosides with the desired, canonical configuration might be completed in the early stage of the RNA-forming process as opposed to later evolution, promoted by simple and widespread transition-metal minerals. The study may also find its value in synthetic chemistry as a guideline for developing a sustainable and selective glycosylation process.

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Manufacture the conducting polymer with light

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Science China chemistry 2025年第1期68卷 8-9页

作者： Yang Li Tianyu Li Yan Ji Baoguang Liu college of Electronic and Optical engineering & college of Flexible Electronics (Future Technology) Nanjing University of Posts & Telecommunications

Poly(3,4-ethylenedioxythiophene) (PEDOT), heralded as the “king” of conducting polymers, is esteemed in bioelectronics for its mixed electronic and ionic conductivity, mechanical properties compatible with biological tissues, tunable healing ability and stability in diverse environments [1]. Based on additive manufacturing of three-dimensional structures,PEDOT realizes the implementation in the efficient production of flexible bioelectronics, the construction of intricate electrode-neural implantations, and the development of smart brain-computer-interfaces [2].

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