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

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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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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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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Applications of in-situ solid-state nuclear magnetic resonance in methanol to olefins reaction

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Science China Chemistry 2025年第1期68卷 134-151页

作者： Jing Niu Shutao Xu Yingxu Wei Zhongmin Liu national Engineering Research Center of Lower-Carbon Catalysis Technology Dalian Institute of Chemical PhysicsChinese Academy of Sciences state Key laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences

The methanol-to-olefins（MTO） reaction offers an alternative pathway for the production of low-carbon olefins from non-oil feedstocks. Fundamental research has been impeded by a lack of comprehensive understanding of its underlying mechanism,despite the significant progress made in industry. In-situ solid-state nuclear magnetic resonance（ss NMR） spectroscopy has emerged as a pivotal tool, offering crucial insights into key species under real-time operando conditions. Furthermore, the host–guest interaction between zeolites or surface species residing on zeolites and the reactant/active intermediates is revealed by the combination of in-situ13C MAS NMR and 2D correlation spectroscopy. Moreover, recent technological advancements in hyperpolarization（HP） methods, including HP129Xe NMR and dynamic nuclear polarization（DNP）, have significantly improved the sensitivity of ss NMR, enabling detailed structural and kinetic analysis as well as the detection of trace species. In this feature article, we summarized recent advancements in（in-situ） ss NMR spectroscopy applied to MTO reaction processes,encompassing mechanistic investigations at various stages and the intricate host–guest interactions. These theoretical insights into the dynamic evolution of MTO reactions lay a solid foundation for the optimization of catalytic processes and the development of efficient catalysts, thereby advancing the techniques towards more sustainable and economical production route for olefins.

关键词： MTO zeolites in-situ ssNMR reactive intermediates reaction mechanism

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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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Unraveling the impacts of intermolecular interaction on morphology evolution for highly efficient organic solar cells and modules

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Science China Chemistry 2025年第1期68卷 264-272页

作者： Xueqing Ma Yingying Cheng Yuqiang Liu Xinming Zheng Guangliu Ran Hongxiang Li Xinyue Cui Andong Zhang Wenkai Zhang Pei Cheng Wenchao Huang Zhishan Bo Beijing Key laboratory of Energy Conversion and Storage Materials College of Chemistry Beijing Normal University College of Textiles and Clothing State Key Laboratory of Bio-fibers and Eco-textiles Qingdao University Key state laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and EngineeringWuhan University of Technology department of physics and Applied Optics Beijing Area Major laboratory Center for Advanced Quantum Studies Beijing Normal University state Key laboratory of Polymer Materials Engineering College of Polymer Science and Engineering Sichuan University

Understanding the effect of intermolecular interaction on the growth dynamic of active layers is critical for advancing organic solar cells(OSCs). However, the diverse structure of donors and acceptors makes the research challenging. Additives with customizable structures and properties could simplify this complexity. Herein, we meticulously tailor two additives of 3,4-ethylenedioxythiophene(EDOT) and 2,5-dibromo-3,4-ethylenedioxythiophene(DBEDOT), possessing distinct intermolecular interaction features to elaborate the inherent relationship. It is found that varied interaction strengths can alter film formation processes. The enhanced intermolecular interaction between the DBEDOT and non-fullerene acceptor BTP-e C9-4F results in pre-aggregation and longer crystallization duration of BTP-e C9-4F, facilitating the formation of films with compact molecular packing and decent phase separation. Thus, exciton dissociation and charge transport become more efficient. Finally, devices processed with DBEDOT exhibit a remarkable power conversion efficiency of 19.35% in small-area OSCs and 14.11% in bladecoated 5 cm × 5 cm organic solar mini-modules. Especially, OSCs can maintain 80% of their initial efficiency after continuous annealing at 85 °C for over 2,100 h.

关键词： organic solar cell non-fullerene acceptor film growth molecular packing intermolecular interaction

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Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO2 in CO2 electroreduction

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Journal of Energy Chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia Key laboratory of Chemistry and physics of Rare Earth Materials School of Chemistry and Chemical Engineering Inner Mongolia University state Key laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Institute of Catalysis Department of Chemistry Zhejiang University national Key laboratory of Baiyunobo Rare Earth Resource Research and Comprehensive Utilization Baotou Research Institute of Rare Earths

Conversion of CO2back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO2nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79% catalytic current density to hydrocarbons （excluding CO）,with 49% faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO2utilization.

关键词： Nanorods

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Molecule‑Level Multiscale Design of Nonflammable Gel Polymer Electrolyte to Build Stable SEI/CEI for Lithium Metal Battery

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Nano-Micro Letters 2025年第1期17卷 404-423页

作者： Qiqi Sun Zelong Gong Tao Zhang Jiafeng Li Xianli Zhu Ruixiao Zhu Lingxu Wang Leyuan Ma Xuehui Li Miaofa Yuan Zhiwei Zhang Luyuan Zhang Zhao Qian Longwei Yin Rajeev Ahuja Chengxiang Wang Key laboratory for Liquid‑solid Structural Evolution and Processing of Materials(Ministry of Education) School of Materials Science and EngineeringShandong UniversityJinan 250061People’s Republic of China Condensed Matter Theory Department of Physics and AstronomyUppsala UniversityUppsala 75120Sweden

The risk of flammability is an unavoidable issue for gel polymer electrolytes(GPEs).Usually,flameretardant solvents are necessary to be used,but most of them would react with anode/cathode easily and cause serious interfacial instability,which is a big challenge for design and application of nonflammable ***,a nonflammable GPE(SGPE)is developed by in situ polymerizing trifluoroethyl methacrylate(TFMA)monomers with flame-retardant triethyl phosphate(TEP)solvents and LiTFSI–LiDFOB dual lithium *** is strongly anchored to PTFMA matrix via polarity interaction between-P=O and-CH_(2)CF_(3).It reduces free TEP molecules,which obviously mitigates interfacial reactions,and enhances flame-retardant performance of TEP *** TEP molecules are also inhibited in solvation of Li^(+),leading to anion-dominated solvation sheath,which creates inorganic-rich solid electrolyte interface/cathode electrolyte interface *** coordination structure changes Li^(+)transport from sluggish vehicular to fast structural transport,raising ionic conductivity to 1.03 mS cm^(-1) and transfer number to 0.41 at 30℃.The Li|SGPE|Li cell presents highly reversible Li stripping/plating performance for over 1000 h at 0.1 mA cm^(−2),and 4.2 V LiCoO_(2)|SGPE|Li battery delivers high average specific capacity>120 mAh g^(−1) over 200 *** study paves a new way to make nonflammable GPE that is compatible with Li metal anode.

关键词： Anchoring effect Nonflammable gel electrolyte In situ cross-linked Electrode-electrolyte interface Li metal battery

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Ca2+ cation-mediated microenvironment for electrochemical hydrodimerization of furfural

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Science China Chemistry 2025年

作者： Wei Du Shuangshuang Cha Can Lei Mengxin Qu Zhongqiang Deng Ming Gong Xinhe Bao department of Chemistry and Shanghai Key laboratory of Molecular Catalysis and Innovative Materials Fudan University state Key laboratory of Catalysis National Laboratory for Clean Energy Collaborative Innovation Center of Chemistry for Energy Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences

Furfural is one of the most important biomass-based platform molecules as sustainable precursors for chemicals and fuels. The electrochemical hydrodimerization of furfural can generate hydrofuroin, which is a promising precursor for gasoline or jet ***, steering the selectivity toward hydrodimerization under near-neutral conditions that suppress polymerization and disproportionation of furfural remains challenging. Herein, we discovered that tuning the electrolyte cations could be an effective and alternative strategy for modulating furfural reduction to the traditional electrocatalyst design. Under the optimal Ca2+cations,hydrofuroin yield could be much improved from other cations with hydrofuroin selectivity of 95.5%. The systematic characterization of the ion-centered double layer reflected the suitable sizes and charges of hydrated Ca2+for suppressing the hydrogen evolution reaction from activation of surrounding water molecules as well as encouraging furfural accumulation via non-covalent interaction for directing the electron transfer to furfurals. Ions with smaller or larger sizes can either activate local water molecules or form a crowded ionic interface that casts an adverse effect on furfural enrichment. This work not only presents an effective strategy for facilitating biomass valorization via hydrodimerization but also emphasizes the essential role of the ion-centered microenvironment for steering the electrocatalytic pathways.

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Crustal magma oxidation state and endowments in porphyry copper deposits

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Science China Earth Sciences 2025年第1期68卷 226-236页

作者： Yumin AI Massimo CHIARADIA Chao WU Huayong CHEN Key laboratory of Mineralogy and Metallogeny Guangzhou Institute of Geochemistry Chinese Academy of Sciences University of Chinese Academy of Sciences department of Earth Sciences University of Geneva Guangdong Provincial Key laboratory of Mineral physics and Materials

Porphyry copper deposits（PCDs） supply the majority of the world's copper（Cu） as well as significant amounts of molybdenum（Mo） and gold（Au）. The formation of these deposits is controlled by a variety of geological factors, among which the magmatic oxidation is one of the focuses of current research. This study investigates the redox characteristics of arc magmas by analyzing the ratio of vanadium（V） to scandium（Sc） and its correlation with the oxygen fugacity （fO2） of magmas from arcs of various crustal thicknesses globally. We compiled an extensive dataset of published V/Sc values and studied the partition coefficients of Vand Sc between minerals and silicate melts across various magmatic environments. The results demonstrate that fractional crystallization of magnetite markedly reduces V/Sc values of the residual melt. Furthermore, magnesium number（Mg#） at the onset of magnetite fractionation is strongly positively correlated with fO2of the equilibrium magma. Based on this,the oxidation of arc magmas from different crustal thicknesses can be evaluated. The result suggests that magmas generated in crusts thicker than 20 km tend to be more oxidized with increasing crust thickness. This trend is attributed to enhanced intracrustal differentiation processes involving garnet and amphibole, particularly in mature island and continental arcs. In contrast,magmas in thinner arc crusts（states than most of their thicker crust counterparts. These findings suggest that both subduction dynamics and crustal thickness play a vital role in determining the oxidation state of arc magmas and, consequently, their capacity to generate PCDs. Highly oxidized, primitive arc magmas are less favorable for PCD formation due to that they tend to experience magnetite fractionation and thus sulfide saturation in the early stage of magma evolution, a process leading to copper depletion. On the contra

关键词： Magma evolution V/Sc systematics Magnetite Oxygen fugacity Porphyry copper deposits

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