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Journal of Environmental Sciences 2025年第3期149卷 374-385页

作者： Qian Ma Yinghao Xue Chuning Zhang Yanyan Chen Wei Teng Hua Zhang Jianwei Fan state Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China

Electrocatalytic reduction of nitrate to ammonia has been considered a promising and sustainable pathway for pollutant treatment and ammonia has significant potential as a clean ***,the method has received much *** this work,Cu/Fe 2D bimetallic metal-organic frameworks were synthesized by a facile method applied as cathode materials without high-temperature *** centers(Cu,Fe)with enhanced intrinsic activity demonstrated higher removal ***,the 2D nanosheet reduced themass transfer barrier between the catalyst and nitrate and increased the reaction ***,the catalysts with a 2D structure showed much better removal efficiency than other structures(3D MOFs and BulkMOFs).Under optimal conditions,Cu/Fe-2D MOF exhibited high nitrate removal efficiency(87.8%)and ammonium selectivity(89.3%)*** ammonium yielded up to significantly 907.2μg/(hr·mg_(cat))(7793.8μg/(hr·mg_(metal)))with Faradaic efficiency of 62.8%at an initial 100 mg N/*** catalyst was proved to have good stability and was recycled 15 times with excellent *** simulations confirm the reduced Gibbs free energy of Cu/Fe-2D *** study demonstrates the promising application of Cu/Fe-2D MOF in nitrate reduction to ammonia and provides new insights for the design of efficient electrode materials.

关键词： Metal-organic frameworks Electrochemical denitrification Ammonium selectivity 2D bimetal materials

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 EngineeringSichuan UniversityChengdu 610065SichuanChina

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： Safe liquid-state lithium-ion batteries In-situ separator technology Hybrid-sol physical crosslinking Electrode coating Inorganic nonflammable separator

Dual-phase interface engineering via parallel modulation strategy for highly reversible Zn metal batteries

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Journal of Energy Chemistry 2025年第2期101卷 163-174页

作者： Zhean Bao Yang Wang Kun Zhang Guosheng Duan Leilei Sun Sinan Zheng Bin Luo Zhizhen Ye Jingyun Huang School of Materials Science and Engineering State Key Laboratory of Silicon and Advanced Semiconductor Materials Zhejiang University Institute of Wenzhou Zhejiang University Institute of Thermal Science and Power Systems Zhejiang University Longmen Laboratory of Luoyang

The reversibility and stability of aqueous Zn metal batteries（AZMBs） are largely limited by Zn dendrites and interfacial parasitic ***,we propose a parallel modulation strategy to boost the reversibility of the Zn anode by introducing N,N,N',N'-tetramethylchloroformamidinium hexafluorophosphate（TCFH） as an additive in the *** is composed of PF6-and TN+with opposite ***6-can spontaneously induce the in-situ generation of ZnF2solid electrolyte interface（SEI） on the anode,which can improve the transport kinetics of Zn2+at the interface,thus promoting the rapid and uniform deposition of Zn as well as inhibiting the growth of *** addition,TN+is enriched at the anode surface during Zn deposition through the anchoring effect,which brings a reconfiguration of the ion/molecule *** anchored-TN+reduces the concentrations of H2O and SO42-,sufficiently restraining the parasitic *** to the dual-phase interface engineering constructed of PF6-and TN+in parallel,the symmetric cell with the proposed electrolyte survives long cycling stability over750 h at 20 mA cm-2,10 mAh *** study offers a distinct viewpoint to the multidimensional optimization of Zn anodes for high-performance AZMBs.

关键词： Anchoring effect Aqueous Zn metal batteries Electrolyte additive Solid electrolyte interface Zn anode

Catalytic detoxification of mitoxantrone by graphitic carbon nitride(g-C_(3)N_(4))supported Fe/Pd bimetallic nanoparticles

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Journal of Environmental Sciences 2025年第2期148卷 614-624页

作者： Qianyu Xu Haoyang Fu Jiyuan Gu Liyu Lei Lan Ling state Key Laboratory for Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China

The overuse of antibiotics and antitumor drugs has resulted in more and more extensive pollution of water bodies with organic drugs,causing detrimental ecological effects,which have attracted attention towards effective and sustainable methods for antibiotics and antitumor drug ***,the hybrid nanomaterial(g-C_(3)N_(4)@Fe/Pd)was synthesized and used to remove a kind of both an antibiotic and antitumor drug named mitoxantrone(MTX)with 92.0%removal efficiency,and the MTX removal capacity is 450 mg/*** exposing to the hybrid material the MTX aqueous solution changed color from dark blue to lighter progressively,and LC-UV results of residual solutions showthat a newpeak at 3.0min(MTX:13.2min)after removal by g-C_(3)N_(4)@Fe/Pd appears,with the simultaneous detection of intermediate products indicating that g-C_(3)N_(4)@Fe/Pd indeed degrades *** mass spectrometric analysis suggests that the nuclear mass ratio decreased from 445.2(M+1H)to 126.0(M+1H),169.1(M+1H),239.2(M+1H),267.3(M+1H),285.2(M+1H),371.4(M+1H)and 415.2(M+1H),and the maximum proportion(5.63%)substance of all degradation products(126.0(M+1H))is 40-100 times less toxic than MTX.A mechanism for the removal and degradation of mitoxantrone was ***,actual water experiments confirmed that the maximum removal capacity of MTX by g-C_(3)N_(4)@Fe/Pd is up to 492.4 mg/g(0.02 g/L,10 ppm).

关键词： Degradation LC-QTOF-MS Nanoparticles Mitoxantrone Aqueous solution

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

Microdynamic modulation through Pt–O–Ni proton and electron “superhighway” for pH-universal hydrogen evolution

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Journal of Energy Chemistry 2025年第2期101卷 808-815页

作者： Dewen Wang Yuting Chen Bohan Yao Tian Meng Yanchao Xu Dongxu Jiao Zhicai Xing Xiurong Yang state Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences university of Science and Technology of China Department of Chemistry Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Southern University of Science and Technology state Key Laboratory of Automotive Simulation and Control School of Materials Science and Engineering Jilin University

Optimizing the microdynamics in alkaline and neutral conditions is a significant but challenging task in developing pH-universal hydrogen evolution（HER） ***,a unique Pt-O-Ni bridge has been constructed to alter the coordination and electronic environment between Pt nanoparticles（Pt_n）and nickel metaphosphate（NPO） substrate（Pt-NPO）.Sufficient electron transfer from NPO to Pt_n to maintain an electron-rich environment and a low valence state of Pt_***,H*is produced from the H2O dissociation on Ni site and then spillover toward Pt sites to bind into H2,which makes up for the insufficient H2O dissociation ability of Pt in Volmer ***-NPO exhibits long-term stability and only need the overpotentials of 22.3,33.0 and 30.5 mV to attain 10 mA cm-2in alkaline,neutral and acidic media,*** anion-exchange membrane（AEM） water electrolyzer catalyzed by Pt-NPO shows high water electrolysis performance that a cell voltage of 1.73 V is needed to obtain the current density of500 mA cm-2in 1 M KOH at 80℃,at the same time maintains good stability for 350 *** regulation strategy proposed in this work is helpful for the design and synthesis of highly efficient pH-universal HER electrocatalysts.

关键词： Atomic and electronic regulation Hydrogen evolution reactions Metal-support interactions Microdynamics pH-universal HER electrocatalysts

Low-cost and fluoride-free synthesis of MFI zeolite nanosheets with enhanced stability for benzene alkylation with ethanol

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Journal of Energy Chemistry 2025年第1期100卷 458-468页

作者： Peng Zhu Cun Liu Yiren Yu Guoshu Gao Yumeng Zhao Xiongfu Zhang Guodong Liu Guohui Yang state Key Laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyDalian 116024 state Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented *** obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.

关键词： MFI zeolite ZSM-5 Nanosheets Scale-up synthesis Aromatic alkylation

Beyond the arylamine convention

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Science China Materials 2025年第2期68卷 685-686页

作者： Liyuan Han state Key Laboratory of Metal Matrix Composites Shanghai Jiao Tong UniversityShanghai 200240China

Inverted perovskite solar cells(PSCs)offer several advantages including superior durability,compatibility with tandem structures,and thus market-integration potentials[1-4].Research on inverted PSCs has gained momentum with the introduction of molecule-based hole-selective contacts,significantly enhancing device power conversion efficiencies(PCEs).These molecules,consisting of aπ-conjugation unit and an anchoring group,play a critical role in affecting the hole extraction at the interface between the perovskite layer and anode in inverted PSCs[5].

关键词： perovskite durability gained

In situ formed fluorescent gold nanoclusters inhibit hair follicle regeneration in oxidative stress microenvironment via suppressing NFκB signal pathway

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Chinese Chemical Letters 2025年第2期36卷 284-288页

作者： Xiangdong Lai Tengfei Liu Zengchao Guo Yihan Wang Jiang Xiao Qingxiu Xia Xiaohui Liu Hui Jiang Xuemei Wang state Key Laboratory of Digital Medical Engineering School of Biological Science and Medical Engineering Southeast University

Skins expose to kinds of risk factors for damage, such as the hormone drugs, skin care products and ultraviolet radiation, which is accompanied by the production of excessive reactive oxygen species(ROS)and eventually leads to hypertrichosis. This skin disease is not aesthetically pleasing and even causes psychological and spiritual problems such as inferiority, anxiety and irritability. Current therapies are limited and often unsatisfactory, such as pharmacological and physical therapies, which have adverse effects and cause the irreversible destruction of hair follicles. Gold nanoclusters have good biocompatibility and their biosynthesis in vivo is responsive to oxidative stress microenvironment(OSM), which could be a safe and effective drug for ROS-induced skin injury. In our study, we demonstrated that zero valence fluorescent gold nanoclusters(FGNCs) were in situ biosynthesized in the plucking-induced damaged skin but not in the normal skin after the administration of gold precursors(+3), while FGNCs inhibited hair follicle regeneration by negatively regulating nuclear transcription factor kappa B(NFκB)-mediated inflammatory response signaling pathway(NFκB/tumor necrosis factor-α(TNF-α) axis). This OSM-responsive in situ biosynthesis method is facile and safe and holds great promise for curing hypertrichosis associated with skin dermatitis and injury.

关键词： Fluorescent gold nanoclusters Hair follicle regeneration Oxidative stress microenvironment Reactive oxygen species Skin injury

An efficient quantum proactive incremental learning algorithm

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Science China(Physics,Mechanics & Astronomy) 2025年第1期68卷 45-53页

作者： Lingxiao Li Jing Li Yanqi Song Sujuan Qin Qiaoyan Wen Fei Gao state Key Laboratory of Networking and Switching Technology Beijing University of Posts and TelecommunicationsBeijing 100876China School of Cyberspace Security Beijing University of Posts and TelecommunicationsBeijing 100876China

In scenarios where a large amount of data needs to be learned,incremental learning can make full use of old knowledge,signif-icantly reduce the computational cost of the overall learning process,and maintain high *** this paper,taking the MaxCut problem as our example,we introduce the idea of incremental learning into quantum computing,and propose a Quantum Proactive Incremental Learning algorithm(QPIL).Instead of a one-off training of quantum circuit,QPIL contains a multi-phase training on gradually-increased subgraphs of all vertices,proactively reducing large-scale problems to smaller ones to solve in steps,providing an efficient solution for ***,some vertices and corresponding edges are randomly selected for training to obtain optimized parameters of the quantum circuit at ***,in each incremental phase,the remaining vertices and corresponding edges are gradually added and the parameters obtained from the previous phase are reused in the parameter initialization of the current *** perform experiments on 120 different small-scale graphs,and it shows that QPIL performs superior to prevalent quantum and classical baselines in terms of approximation ratio(AR),time cost,anti-forgetting,and solv-ing *** particular,QPIL’s AR surpasses 20%of mainstream quantum baselines,and the time cost is less than 1/5 of *** idea of QPIL is expected to inspire efficient and high-quality solutions in large-scale MaxCut and other combinatorial optimization problems.

关键词： variational quantum algorithm incremental learning multi-phase training MaxCut quantum computing