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A surface engineering strategy for the stabilization of zinc metal anodes with montmorillonite layers toward long-life rechargeable aqueous zinc ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 94-105页

作者： Wenbo Wang Ruifeng Xu Xu Zhang Peiyu Wang Bao Yang Bingjun Yang Juan Yang Kailimai Su Pengjun Ma Yanan Deng Xianfeng Fan Wanjun Chen key laboratory for Electronic Materials College of Electrical Engineering Northwest Minzu University Resource Chemistry and Energy Materials Research Center State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Institute for Materials and Processes School of Engineering University of Edinburgh

Rechargeable aqueous zinc-ion batteries （AZIBs） exhibit appreciable potential in the domain of electrochemical energy ***,there are serious challenges for AZIBs,for instance zinc dendrite growth,hydrogen evolution reaction （HER）,and corrosion side ***,we propose a surface engineering modification strategy for coating the montmorillonite （MMT） layer onto the surface of the Zn anode to tackle these issues,thereby achieving high cycling stability for rechargeable *** results reveal that the MMT layer on the surface of the Zn anode is able to provide ordered zincophilic channels for zinc ions migration,facilitating the reaction kinetics of zinc *** functional theory（DFT） calculations and water contact angle （CA） tests prove that MMT@Zn anode exhibits superior adsorption capacity for Zn2+and better hydrophobicity than the bare Zn anode,thereby achieving excellent cycling ***,the MMT@Zn||MMT@Zn symmetric cell holds the stable cycling over 5600 h at 0.5 mA cm-2and 0.125 m A h cm-2,even exceeding 1800 h long cycling under harsh conditions of 5 m A cm-2and 1.25 m A h *** MMT@Zn||V2O5full cell reaches over 3000 cycles at 2 A g-1with excellent rate ***,this surface engineering modification strategy for enhancing the electrochemical performance of AZIBs represents a promising application.

关键词： Hydrogen evolution reaction

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Bifunctional bridging capping layer enables 24.5% efficiency of perovskite solar cells with polymer-based hole transport materials

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Science China Chemistry 2025年第1期68卷 350-359页

作者： Can Zhu Yiyang Wang Lei Meng Beibei Qiu Jing Li Shucheng Qin Ke Hu Xin Jiang Wenbin Lai Minchao Liu Zhe Liu Chenxing Lu Jinyuan Zhang Yongfang Li Beijing National laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences School of Chemical Science University of Chinese Academy of Sciences key laboratory of solid state Optoelectronic Devices of Zhejiang Province College of Physics and Electronic Information Engineering Zhejiang Normal University key laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of Sciences laboratory of Advanced Optoelectronic Materials College of Chemistry Chemical Engineering and Materials ScienceSoochow University

Developing a bridge capping layer between perovskite and hole transport layer materials（HTMs） in the n-i-p perovskite solar cells（pero-SCs） is an effective approach to modify the morphology of HTMs and passivate the perovskite ***, we select the quinoxaline-based bifunctional passivation agent, quinoxalin-6-yl-methylamine hydrochloride（Qx MACl）,as the bridging layer, and a D-A copolymer PBQ12 containing the same quinoxaline unit as an HTM for the n-i-p pero-SCs. Due to the π-π stacking among the common quinoxaline units in the bridge layer and HTM, Qx MACl induces the π-π stacking of the PBQ12 film and improves the film morphology of HTMs with better conductivity. Additionally, Qx MACl can effectively passivate the perovskite surface, and PBQ12 possesses appropriate energy levels and high hole mobility. The pero-SCs based on FAPbI3with PBQ12/Qx MACl treatment showed a higher power conversion efficiency（PCE） of 24.05% and outstanding stability, maintaining 95.4% and 92.1% of its initial PCE after 750 h of storage and after over 800 h of thermal annealing at 85 °C, respectively. To further enhance the PCE of the PBQ12/Qx MACl-based devices, we developed a non-metal ion dopant for the PBQ12 HTM. Through trace doping of PBQ12 HTM by the non-metal ion dopant, the PCE of the PBQ12/Qx MACl-based devices reached 25.24%（the calibrated PCE of 24.55% by the National Institute of Metrology, China）.

关键词： D-A copolymer, hole transport materials, bifunctional bridge capping layer, passivation perovskite solar cells

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A self-adaptive inorganic in-situ separator by particle crosslinking for nonflammable lithium-ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 469-480页

作者： Jiarui Yang Jiuzhou Liu Wenrui Cai Ziyu Zhao Shan Wang Lu He Shanshan Lv Zhiwei Zhu Zhongfeng Ji Guojiang Wen Hua Li Yuanming Zhai Xuewei Fu Wei Yang Yu Wang College of Polymer Science and Engineering State Key Laboratory of Polymer Materials Engineering Sichuan University

All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.

关键词： Silica nanoparticles

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Substrate bias effects in p-channel GaN-on-Si transistors

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Science China(Information Sciences) 2025年第1期68卷 404-405页

作者： Mengyao ZHAO Jie MA Lanlan YANG Chuanqi PAN Denggui WANG Jianjun ZHOU Sheng LI Jiaxing WEI Long ZHANG Siyang LIU Weifeng SUN National ASIC System Engineering Research Center School of Integrated Circuits Southeast University National Center of Technology Innovation for Electronic Design Automation Southeast University National key laboratory of solid-state Microwave Devices and Circuits

The drain current （ID） of the n-channel GaN field-effecttransistor （n-FET） is influenced by the substrate-to-source bias voltage (VBS)（substrate bias effect）[1].Actually,nonzero VBSis also likely to occur in p-FET in real application,because the source electrode of p-FET is usually connected to high *** study reports the dependency between IDand VBSin p-FET for the first time,and analyzes the underlying mechanisms from the perspective of vertical electric field （EF） distribution.

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Efficient and Stable Photoassisted Lithium‑Ion Battery Enabled by Photocathode with Synergistically Boosted Carriers Dynamics

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Nano-Micro Letters 2025年第3期17卷 440-454页

作者： Zelin Ma Shiyao Wang Zhuangzhuang Ma Juan Li Luomeng Zhao Zhihuan Li Shiyuan Wang Yazhou Shuang Jiulong Wang Fang Wang Weiwei Xia Jie Jian Yibo He Junjie Wang Pengfei Guo Hongqiang Wang state key laboratory of solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Laboratory of Graphene(NPU)Xi’an 710072People’s Republic of China state key laboratory of solidification Processing School of Materials Science and Engineering DepartmentNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China state key laboratory of solidification Processing Center of Advanced Lubrication and Seal MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China Research and Development Institute of Northwestern Polytechnical University in Shenzhen Shenzhen 518063People’s Republic of China key laboratory of Applied Surface and Colloid Chemistry Shaanxi Key Laboratory for Advanced Energy DevicesShaanxi Engineering Lab for Advanced Energy TechnologySchool of Materials Science and EngineeringNational Ministry of EducationShaanxi Normal UniversityXi’an 710119People’s Republic of China

Efficient and stable photocathodes with versatility are of significance in photoassisted lithium-ion batteries(PLIBs),while there is always a request on fast carrier transport in electrochemical active *** work proposes a general approach of creating bulk heterojunction to boost the carrier mobility of photocathodes by simply laser assisted embedding of plasmonic *** employed in PLIBs,it was found effective for synchronously enhanced photocharge separation and transport in light charging ***,experimental photon spectroscopy,finite difference time domain method simulation and theoretical analyses demonstrate that the improved carrier dynamics are driven by the plasmonic-induced hot electron injection from metal to TiO_(2),as well as the enhanced conductivity in TiO2 matrix due to the formation of oxygen vacancies after Schottky *** from these merits,several benchmark values in performance of TiO2-based photocathode applied in PLIBs are set,including the capacity of 276 mAh g^(−1)at 0.2 A g^(−1)under illumination,photoconversion efficiency of 1.276%at 3 A g^(−1),less capacity and Columbic efficiency loss even through 200 *** results exemplify the potential of the bulk heterojunction strategy in developing highly efficient and stable photoassisted energy storage systems.

关键词： Photoassisted lithium-ion batteries Bulk heterojunction Carrier dynamics TiO2 nanofiber Plasmonic metal nanocrystals

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Unveiling the promotion role of ZnO on Zn-Al spinel oxide for CO2 hydrogenation

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Journal of Energy Chemistry 2025年第1期100卷 18-25页

作者： Tongyao Wang Xinlong Yao Lixin Liang Hongyu Chen Pan Gao Guangjin Hou state key laboratory of Catalysis Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences

The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO2hydrogenation. However, the structure–activity relationship of the reaction remains poorly understood due to challenges in atomic-level structural characterizations and analysis of reaction intermediates. In this study, we prepared two Zn-Al spinel oxide catalysts via coprecipitation（ZnAl-C）and hydrothermal（ZnAl-H） methods, and conducted a comparative investigation in the CO2hydrogenation reaction. Surprisingly, under similar conditions, ZnAl-C exhibited significantly higher selectivity towards methanol and DME compared to ZnAl-H. Comprehensive characterizations using X-ray diffraction（XRD）, Raman spectroscopy and electron paramagnetic resonance（EPR） unveiled that ZnAl-C catalyst had abundant ZnO species on its surface, and the interaction between the ZnO species and its ZnAl spinel oxide matrix led to the formation of oxygen vacancies, which are crucial for CO2adsorption and activation. Additionally, state-of-the-art solid-state nuclear magnetic resonance（NMR） techniques,including ex-situ and in-situ NMR analyses, confirmed that the surface ZnO facilitates the formation of unique highly reactive interfacial formate species, which was readily hydrogenated to methanol and DME. These insights elucidate the promotion effects of ZnO on the ZnAl spinel oxide in regulating active sites and reactive intermediates for CO2-to-methanol hydrogenation reaction, which is further evidenced by the significant enhancement in methanol and DME selectivity observed upon loading ZnO onto the ZnAl-H catalyst. These molecular-level mechanism understandings reinforce the idea of optimizing the ZnO-ZnAl interface through tailored synthesis methods to achieve activity-selectivity balance.

关键词： Reaction intermediates

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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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Wafer‑Scale Ag_(2)S‑Based Memristive Crossbar Arrays with Ultra‑Low Switching‑Energies Reaching Biological Synapses

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Nano-Micro Letters 2025年第3期17卷 328-339页

作者： Yuan Zhu Tomas Nyberg Leif Nyholm Daniel Primetzhofer Xun Shi Zhen Zhang Division of solid‑state Electronics Department of Electrical EngineeringUppsala University75121 UppsalaSweden Department of Chemistry Uppsala UniversityUppsalaSweden Department of Physics and Astronomy Uppsala UniversityUppsalaSweden state key laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050People’s Republic of China

Memristive crossbar arrays(MCAs)offer parallel data storage and processing for energy-efficient neuromorphic ***,most wafer-scale MCAs that are compatible with complementary metal-oxide-semiconductor(CMOS)technology still suffer from substantially larger energy consumption than biological synapses,due to the slow kinetics of forming conductive paths inside the memristive *** we report wafer-scale Ag_(2)S-based MCAs realized using CMOS-compatible processes at temperatures below 160℃.Ag_(2)S electrolytes supply highly mobile Ag+ions,and provide the Ag/Ag_(2)S interface with low silver nucleation barrier to form silver filaments at low energy *** further enhancing Ag+migration in Ag_(2)S electrolytes via microstructure modulation,the integrated memristors exhibit a record low threshold of approximately−0.1 V,and demonstrate ultra-low switching-energies reaching femtojoule values as observed in biological *** low-temperature process also enables MCA integration on polyimide substrates for applications in flexible ***,the intrinsic nonidealities of the memristive units for deep learning can be compensated by employing an advanced training *** impressive accuracy of 92.6%in image recognition simulations is demonstrated with the MCAs after the *** demonstrated MCAs provide a promising device option for neuromorphic computing with ultra-high energy-efficiency.

关键词： Wafer-scale Ag_(2)S films Reactive sputter Silver nucleation Ag^(+)migration Energy-efficient neuromorphic computing

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Tuning the porosity of {Co12IICo8III（μ3-OH）24（X）}11+ supramolecular frameworks by reaction time for D2/H2 separation

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Science China Chemistry 2025年

作者： Zhuozhou Xie Zhu Zhuo Zi-Ang Nan Qing Li Xiufang Li Zi-Xiu Lu Linzhe Lü Jin Liu Luyao Liu Wenjing Wang Wei Wang Daqiang Yuan You-Gui Huang state key laboratory of Structure Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences University of Chinese Academy of Sciences Xiamen key laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth Materials Haixi InstitutesChinese Academy of Sciences state key laboratory of Physical Chemistry of solid Surfaces Department of Chemistry College of Chemistry and Chemical EngineeringXiamen University

Systematicly tuning the porosities of porous materials is crucial for targeted gas mixture separation,yet it remains a longstanding *** a common strategy,altering the phenylene ring count in the organic building units has been exploited to adjust pore apertures in metal organic frameworks （MOFs） and covalent organic frameworks （COFs）,resulting in only a stepwise pore size variation of approximately 2.8?.Unlike MOFs and COFs,the porosities for supramolecular assembly frameworks are highly dependent on the packings of the molecular building units in the *** above strategy cannot be applied to supramolecular assembly frameworks and other strategies are required to adjust pore apertures in supramolecular frameworks,especially to achieve porous materials with the optimal pore size for D2/H2separation （～3?）.Here,we successfully modulate the porosity of supramolecular frameworks of[CoII1+12CoIII8L12（μ3-OH）24（X）]1clusters （L=mono-deprotonated 1-iminoisoindole-3-amine,X=ClO?4or Cl?） by controlling the duration of self-assembly *** simply adjusting the reaction time,we obtain three[CoII12CoIII8L12（μ3-OH）24（X）]11+supramolecular frameworks:[CoII12CoIII8（μ3-OH）24（ClO4）L12)]·（Cl）4·（HCO2）7（1）,[CoII12CoIII8L12（μ3-OH）24（Cl）]·（ClOI4）4·（Cl）6·（HCO2）·（H2O）10（2）,and[CoI12CoIII8L12（μ3-OH）24（Cl）]·（Cl）11·（H2O）12（3）.The different stacking patterns of the[CoII12CoIII8L12（μ3-OH）24（X）]11+clusters in these frameworks lead to significantly varied stabilities and *** 1 exhibits permanent porosity with interconnected channels and maintains stability under harsh *** contrast,compound 2 is nearly nonporous,and compound 3 becomes unstable upon *** pores of compound 1 show higher affinity to D2than H2,and the pore aperture diameter of compound 1 （～3.06?） meets the optimal porosity for D2/***,compound 1 demonstrates moderate D2/H2separation at 77 K (retention time:～7 min/g for D2/H2/Ne （10/10/80 vol%） in a flow of 5 mL

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Thermally triggered topological polymerization in diacetylene-functionalized covalent organic framework toward enhanced memristive properties

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Science China Chemistry 2025年

作者： Panke Zhou Yuxing Huang Ziyue Yu Cong Zhang Qian Chen Yiping Li Chao Lin Xiong Chen state key laboratory of Photocatalysis on Energy and Environment Key Laboratory of Advanced Carbon-Based Functional MaterialsCollege of Chemistry Fuzhou University

The development of stimuli-responsive switching memory devices and the elucidation of their switching mechanisms in specific environments are crucial for advancing the field of molecular electronics. Herein, we propose two distinct two-dimensional covalent organic frameworks (COFs), namely Py-EDA and Py-BDA, incorporating acetylene (-C≡C-) or diacetylene(-C≡C-C≡C-) moieties, respectively, targeting fabricate memory devices exhibiting stimuli-responsive switching *** findings demonstrate that the incorporation of acetylene units effectively modulates the electronic band structure and enhances the degree ofπ-conjugation, resulting in devices that exhibit typical bipolar nonvolatile memory performance. Notably,upon thermal treatment, the memory behavior of the ITO/Py-BDA/Ag device transitions to a write-once-read-many-times(WORM) mode, displaying decreased SET voltage, increased ON/OFF current ratio, and remarkable retention reliability and cycle stability. This switching behavior is attributed to the occurrence of interlayer solid-state topological polymerization at 350℃, leading to the transformation of diacetylene columnar arrays into enyne chains within Py-BDA, thereby further promoting interlayer charge transfer and separation.

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