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From blocker to booster:Harnessing garnet surface chemistry for advanced solid-state electrolytes

Nano Research 2025年第1期18卷 323-331页

作者： Jun Cheng Xuan Zhou Hongqiang Zhang Zhen Zeng Yuanyuan Li Yulong Zhu Yingsheng Liao Lijie Ci Deping Li State Key Laboratory of Precision Welding and Joining of Materials and Structures School of Materials Science and EngineeringHarbin Institute of Technology(Shenzhen)Shenzhen 518055China

Garnet electrolytes with high ionic conductivity and electrochemical stability are widely used as fillers to fabricate composite solid electrolytes(CPEs)within polymer ***,the performance of CPEs is significantly influenced by the surface characteristics of the garnet ***,the impact of garnet surface characteristics on CPEs was systematically investigated and a conversion from a typically unstable and Lewis basic surface to a more stable Lewis acidic surface was realized,which is shown to be more conductive to the improved performance of *** simultaneously removing the Li_(2)CO_(3)layer and applying a Li-Al-O coating,the influence of surface characteristics on CPEs was *** Lewis acid Li-Al-O surface coating not only promotes lithium salt dissociation,improving the ionic conductivity and ionic transfer number,but also prevents the reformation of the passive Lewis basic Li_(2)CO_(3)*** to garnet with a Lewis basic Li_(2)CO_(3)surface,the garnet modified with a Lewis acid Li-Al-O coating enhances CPEs,which exhibit an improved critical current density of 1.0 mA·cm^(-2)and highly stable lithium symmetric cell cycling for 400 h at 0.2 mA·cm^(-2).This research highlights the importance of surface chemistry in the design of high-performance solid-state batteries and presents a strategic modification approach for garnetbased CPEs.

关键词： garnet electrolyte composite solid electrolyte surface chemistry all-solid-state batteries

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Controllable photooxidation of 1-phenylethanol integrated with hydrogen evolution by a polyoxometalate/ZnIn_(2)S_(4)/WO_(3)catalytic system

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Nano Research 2025年第4期18卷 116-124页

作者： Jiaxin Yang Yongkang Liu Yun Qin Zhenheng Diao Yuanyuan Dong Hongjin Lv School of Chemical Engineering Advanced Institute of Materials ScienceChangchun University of TechnologyChangchun 130012China MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectric/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488China

The photocatalytic oxidation of 1-phenylethanol coupling with hydrogen evolution represents a promising strategy for the full utilization of the photogenerated electrons and holes to accomplish the maximum conversion of solar energy into chemical *** date,however,the controllable of reaction path and product distribution has yet not to be ***,we report an efficient coupled catalytic system composed of ZnIn_(2)S_(4)/WO_(3)S-scheme heterojunction and Ni-containing polyoxometalate([Ni_(4)(H_(2)O)_(2)(PW_(9)O_(34))_(2)]^(10-)(Ni_(4)P_(2))),which exhibited excellent photocatalytic activities towards the oxidation valorization of 1-phenylethanol coupling with hydrogen *** addition of Ni_(4)P_(2)can efficiently control the product ***,1-phenylethanol was preferentially converted to pinacol(86.0% selectivity)via C-C coupling over ZnIn_(2)S_(4)/WO_(3)S-scheme heterojunction accompanied by hydrogen production(202.4μmol),whereas it would be converted to acetophenone(93.8% selectivity)by photogenerated holes with concomitant hydrogen formation(183.1μmol)over the coupled Ni_(4)P_(2)/ZnIn_(2)S_(4)/WO_(3) catalytic *** studies revealed that the hydrogen evolution cocatalyst Ni4P2,with its excellent electron storage capacity,can compete with the oxidation product acetophenone for electrons,and thus its addition can significantly inhibit the reduction of acetophenone,resulting in the inability to generate the coupling product pinacol.

关键词： S-scheme heterojunction ZnIn_(2)S_(4) polyoxometalates dehydrocoupling hydrogen evolution photocatalysis

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Improving the reliability of classical molecular dynamics simulations in battery electrolyte design

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Journal of Energy Chemistry 2025年第2期101卷 34-41,I0002页

作者： Xin He Yujie Zhang Haomiao Li Min Zhou Wei Wang Ruxing Wang Kai Jiang Kangli Wang State Key Laboratory of Advanced Electromagnetic Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina State Key Laboratory of Materials Processing and Die&Mould Technology College of Materials Science and EngineeringHuazhong University of Science and Technology Wuhan 430074HubeiChina Hubei Collaborative Innovation Center for High-efficiency Utilization of Solar Energy Hubei University of TechnologyWuhan 430068HubeiChina

Explorations into new electrolytes have highlighted the critical impact of solvation structure on battery performance,Classical molecular dynamics(CMD)using semi-empirical force fields has become an essential tool for simulating solvation ***,mainstream force fields often lack accuracy in describing strong ion-solvent interactions,causing disparities between CMD simulations and experimental *** some empirical methods have been employed in some of the studies to address this issue,their effectiveness has been *** CMD research,supported by quantum chemical calculations and experimental data,reveals that the solvation structure is influenced not only by the charge model but also by the polarization *** empirical approaches that focused solely on adjusting ion-solvent interaction strengths overlooked the importance of polarization *** on this insight,we propose integrating the Drude polarization model into mainstream force fields and verify its feasibility in carbonate,ether,and nitrile *** experimental results demonstrate that this approach significantly enhances the accuracy of CMD-simulated solvation *** work is expected to provide a more reliable CMD method for electrolyte design,shielding researchers from the pitfalls of erroneous simulation outcomes.

关键词： Electrolyte Classical molecular dynamics Solvation structure Simulations

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Highly electrically conductive MOF/conducting polymer nanocomposites toward tunable electromagnetic wave absorption

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材料科学技术（英文版） 2025年第2期205卷 258-269页

作者： Xin Wu Peiyuan Kang Yinghan Zhang Haocheng Guo Shuoying Yang Qi Zheng Lianjun Wang Wan Jiang State Key Laboratory for Modification of Chemical Fibers and Polymer Materials & College of Materials Science and Engineering Donghua UniversityShanghai 201620China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials & College of Materials Science and Engineering Donghua UniversityShanghai 201620China Engineering Research Center of Advanced Glasses Manufacturing Technology Ministry of EducationDonghua UniversityShanghai 201620China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials & College of Materials Science and Engineering Donghua UniversityShanghai 201620China Institute of Functional Materials Donghua UniversityShanghai 201620China

Metal-organic frameworks(MOFs)have attracted significant interest as self-templates and precursors for the synthesis of carbon-based composites aimed at electromagnetic wave(EMW)***,the utilization of high-temperature treatments has introduced uncertainties regarding the compositions and microstructures of resulting ***,complete carbonization has led to diminished yields of the produced carbon composites,significantly limiting their practical ***,the exploration of pristine MOF-based EMW absorbers presents an intriguing yet challenging endeavor,primarily due to inherently low electrical *** this study,we showcase the utilization of struc-turally robust Zr-MOFs as scaffolds to build highly conductive Zr-MOF/PPy composites via an inner-outer dual-modification approach,which involves the production of conducting polypyrrole(PPy)both within the confined nanoporous channels and the external surface of Zr-MOFs via post-synthetic *** interconnection of confined PPy and surface-lined PPy together leads to a consecutive and extensive conducting network to the maximum *** therefore entails outstanding conductivity up to～14.3 S cm-1 in Zr-MOF/PPy composites,which is approximately 1-2 orders of magnitude higher than that for conductive MOF nanocomposites constructed from either inner or outer *** from the strong and tunable conduction loss,as well as the induced dielectric polarization originated from the porous structures and MOF-polymer interfaces,Zr-MOF/PPy exhibits excellent microwave attenuation capabilities and a tunable absorption frequency ***,with only 15 wt.％loading,the mini-mum reflection loss(RLmin)can reach up to-67.4 dB,accompanied by an effective absorption bandwidth(EAB)extending to 6.74 ***,the microwave absorption characteristics can be tailored from the C-band to the Ku-band by adjusting the loading of *** work provide

关键词： Conductive mof nanocomposites Electromagnetic wave absorption MOF/conducting polymer Electrical conductivity Zr-MOF/PPy

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Precipitation Behavior of MnS Inclusion in Unidirectionally-solidified Fe–18Mn–1Al–0.3C Steels

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Tetsu-To-Hagane/Journal of the Iron and Steel Institute of Japan 2025年第3期111卷 122-130页

作者： Fan, Yuewen Kameda, Kouki Hu, Xiaojun Matsuura, Hiroyuki State Key Laboratory of Advanced Metallurgy University of Science and Technology Beijing China Department of Materials Engineering Graduate School of Engineering The University of Tokyo Japan

In order to reasonably control the precipitation of inclusions during solidification in TWIP steels, the precipitation behavior of typical MnS inclusions in high manganese steel was investigated by unidirectional solidification experiments. Through the combined analyses using ASEM-EDS, optical microscope, and thermodynamic calculation, it was found that Mn concentration in the liquid metal region were higher than those in the solid metal region. Furthermore, closer to the inclusion the liquid phase was, higher its Mn content was. In Fe–18mass%Mn–1Al–0.3C, MnS inclusions can precipitate at the positions located in the junction of dendrites at the end of the solidification (solid fraction fS = 0.96), Mn content reaching 34.88 mass%. Already existing Al2O3 particles could become the core of MnS to form composite inclusions to promote the MnS precipitation during the solidification process. When fS achieved 0.7 leading the Mn segregation in the liquid phase to 25 mass%, MnS starts to precipitate to attach the Al2O3 surface to form composite inclusion. © 2025 The Iron and Steel Institute of Japan.

关键词： Manganese steel

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Elastic properties of Cu–6wt% Ag alloy wires for pulsed magnets investigated by ultrasonic techniques

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Chinese Physics B 2025年第2期34卷 90-95页

作者： Ziyu Li Tianyi Gu Wenqi Wei Yang Yuan Zhuo Wang Kangjian Luo Yupeng Pan Jianfeng Xie Shaozhe Zhang Tao Peng Lin Liu Qi Chen Xiaotao Han Yongkang Luo Liang Li Wuhan National High Magnetic Field Center Huazhong University of Science and TechnologyWuhan 430074China School of Physics Huazhong University of Science and TechnologyWuhan 430074China State Key Laboratory of Advanced Electromagnetic Engineering and Technology Huazhong University of Science and TechnologyWuhan 430074China School of Materials Science and Engineering State Key Laboratory for Materials Processing and Die&Mold TechnologyHuazhong University of Science and TechnologyWuhan 430074China

Conductor materials with good mechanical performance as well as high electrical and thermal conductivities are particularly important to break through the current bottle-neck limit(~ 100 T) of pulsed magnets. Here, we perform systematic studies on the elastic properties of the Cu–6wt% Ag alloy wire, which is a promising candidate material for the new-generation pulsed magnets, by employing two independent ultrasonic techniques, i.e., resonant ultrasound spectroscopy(RUS) and ultrasound pulse-echo experiments. Our RUS measurements manifest that the elastic properties of the Cu–6wt% Ag alloy wires can be improved by an electroplastic drawing procedure as compared with the conventional cold drawing. We also take this opportunity to test the availability of our newly-built ultrasound pulse-echo facility at the Wuhan National High Magnetic Field Center(WHMFC, China), and the results suggest that the elastic performance of the electroplastically-drawn Cu–6wt% Ag alloy wire remains excellent without anomalous softening under extreme conditions,e.g., in ultra-high magnetic field up to 50 T and nitrogen or helium cryogenic liquids.

关键词： high-field magnet Cu–Ag alloy ultrasonic techniques elastic constants

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Metal-organic polyhedra as dynamic cross-linker for recyclable mixed matrix membranes with promising dimension stability

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Science China Chemistry 2025年第2期68卷 705-713页

作者： Linjie Lan Mingxin Zhang Haiyan Xiao Wei Liu-Fu Yuyan Lai Jiadong Chen Jia-Fu Yin Panchao Yin State Key Laboratory of Luminescent Materials and Devices&South China Advanced Institute for Soft Matter Science and Technology Guangdong Basic Research Center of Excellence for Energy and Information Polymer MaterialsSouth China University of TechnologyGuangzhou 510641China State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikou 570228China

Mixed matrix membranes(MMMs)are designed by incorporating microporous inorganic fillers into polymer matrix for the integration of inorganics’excellent gas separation performance with polymers’promising ***,due to the complex interphase interaction,the prevention of long-term aging is still challenging and the poor processability/recyclability of MMMs hinders their extensive ***,a coordination assembly protocol is developed for the fabrication of MMMs with both excellent processability/recyclability upon thermal annealing and promising dimension stability even under high gas *** bearing isophthalic acid(IPA)as side chains are applied to coordinate with Cu^(2+)and the assembled 2.5 nm microporous metal-organic polyhedra(MOP),{Cu_(24)IPA_(24)},serves as multi-functional cross-linkers for the polymer network *** MOPs’well-defined microporosity grants MMMs the capability for O_(2)/N_(2) separation while their activated dynamics at high temperatures(>120℃)endows polymer networks with excellent *** contrast to conventional supramolecular units,the MOPs possess unique logarithmic ligand-exchange kinetics and they show nearly frozen bonding dynamics at room temperature,ensuring promising dimensional stability to overcome the long-term aging and high gas pressure *** work not only provides fundamental understanding of the unique relaxation dynamics of complex systems with intertwined dynamics of supramolecular bonds and polymer chains,but also paves new avenues for the fabrication of robust and recyclable MMMs and elastomers.

关键词： dynamic bonding metal-organic polyhedra mixed matrix membrane polymer recycling gas separation

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Sulfur poisoned PtNi/C catalysts toward two-electron oxygen reduction reaction for acidic electrosynthesis of hydrogen peroxide

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材料科学技术（英文版） 2025年第1期204卷 268-275页

作者： Xin Yang Lijie Zhong Songxin Ye Dequan He Shuxian Yuan Huixin Li Yuting Ma Xiaocheng Mo Shiyu Gan Li Niu Center for Advanced Analytical Science Guangzhou Key Laboratory of Sensing Materials & DevicesGuangdong Engineering Technology Research Center for Photoelectric Sensing Materials & DevicesKey Laboratory of Optoelectronic Materials and Sensors in Guangdong Provincial UniversitiesSchool of Chemistry and Chemical EngineeringGuangzhou UniversityGuangzhou 510006China Center for Advanced Analytical Science Guangzhou Key Laboratory of Sensing Materials & DevicesGuangdong Engineering Technology Research Center for Photoelectric Sensing Materials & DevicesKey Laboratory of Optoelectronic Materials and Sensors in Guangdong Provincial UniversitiesSchool of Chemistry and Chemical EngineeringGuangzhou UniversityGuangzhou 510006China School of Chemical Engineering and Technology Sun Yat-Sen UniversityZhuhai 519082China

Selective electrocatalysis of two-electron oxygen reduction reaction(2e-ORR)has been recognized as a sustainable and on-site process for hydrogen peroxide(H2O2)*** progress has been achieved for 2e-ORR in alkaline ***,it is challenged by insufficient activity and selectiv-ity of the catalysts in acidic ***,we report sulfur-poisoned PtNi/C catalysts(PtNiSx/C)that could regulate ORR from the 4e-to *** identified PtNiS0.6/C offers high activity in terms of onset potential of～0.69 V(***)and～80％*** mass activity is also compara-ble and outperforms representative Pt-based precious and transition-metal-based *** addition,it is interestingly found that the Faradaic efficiency further increased to 95％during the long-term elec-trolysis test due to Ni atom surface *** electrochemical production of the H2O2 system was applied to the electro-Fenton process,which has realized the effective degradation of organic *** work offers a strategy by sulfur poisoning PtNi/C catalyst to realize Pt-based 2e-ORR active catalysts to electrolysis of H2O2 in acidic media.

关键词： Oxygen reduction reaction Hydrogen peroxide Acidic media Electrocatalysis

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Regulation of solvation structure and electrochemical performance optimization in Zn(NH_(2)SO_(3))_(2)-based electrolytes

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Journal of Energy Chemistry 2025年第5期104卷 644-654页

作者： Lei Liu Ruxue Yan Songyan Jiang Xiao Liu Zhonghua Zhang Xiaosong Guo Xingguang Liu Jun Zheng Guicun Li College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials Anhui University of TechnologyMa’anshan 243002AnhuiChina

Monovalent anions,with relatively low charge density,exhibit weak bond energy with Zn^(2+)ions,which facilitates the solubility of Zn salts and the regulation of solvation *** this study,zinc bis(aminosulfate)(Zn(NH_(2)SO_(3))_(2))with a monovalent anion,NH_(2)SO_(3)^(-),was synthesized and dissolved in different ratios of dimethyl sulfoxide(DMSO)and H_(2)O as electrolytes for Zn-ion batteries(ZIBs).From the perspective of game theory,the influences of DMSO and H_(2)O on the solvation structure and electrochemical performance of the Zn(NH_(2)SO_(3))_(2)based electrolytes has been meticulously *** and spectra analysis indicate that DMSO molecules are reluctant to penetrate the primary solvation structure of Zn^(2+)***,increasing DMSO in electrolytes can induce a transition from solvent-separated ion pairs(SSIP)to contact ion pairs(CIP),resulting in an enrichment of anions in the primary solvation *** alteration can significantly suppress parasitic reactions,enhance nucleation density,and refine the deposition morphology during the Zn plating process,leading to superior cyclic stability and high coulombic efficiency(CE)of Zn//Cu and Zn//Zn ***,the enrichment of anions in the primary solvation structure also inhibits the activity of Zn^(2+)ions,amplifies the polarization effect,and engenders a sluggish ionization dynamics,resulting in the low energy conversion efficiency of the *** findings underscore the influence of the anion ratio within the primary solvation structure on electrochemical properties of electrolytes for ZIBs,which may be a pivotal determinant in the Zn deposition process.

关键词： Monovalent anion Primary solvation structure Impressed current cathodic protection Game theory CIP

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Hybrid conductive-lithophilic-fluoride triple protection interface engineering:Dendrite-free reverse lithium deposition for high-performance lithium metal batteries

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Journal of Energy Chemistry 2025年第2期101卷 416-428,I0009页

作者： Huiying Li Chang Hong Runming Tao Xiaolang Liu Jianxing Wang Jianyu Chen Shuhao Yao Jiazhi Geng Guang Zheng Jiyuan Liang Key Laboratory of Optoelectronic Chemical Materials and Devices of Ministry of Education School of Optoelectronic Materials&TechnologyJianghan UniversityWuhan 430056HubeiChina Applied Materials Division Argonne National LaboratoryLemontIL 60439USA State Key Laboratory of Organic Electronics and Information Displays&Institute of Advanced Materials(IAM) Nanjing University of Posts&TelecommunicationsNanjing 210023JiangsuChina

Lithium metal batteries(LMBs)with high energy density are impeded by the instability of solid electrolyte interface(SEI)and the uncontrolled growth of lithium(Li)*** mitigate these challenges,optimizing the SEI structure and Li deposition behavior is the key to stable *** study novelty proposes a facile synthesis of MgF_(2)/carbon(C)nanocomposite through the mechanochemical reaction between metallic Mg and polytetrafluoroethylene(PTFE)powders,and its modified polypropylene(PP)separator enhances LMB *** in-situ formed highly conductive fluorine-doped C species play a crucial role in facilitating ion/electron transport,thereby accelerating electrochemical kinetics and altering Li deposition *** cycling,the in-situ reaction between MgF_(2)and Li leads to the formation of LiMg alloy,along with a LiF-rich SEI layer,which reduces the nucleation overpotential and reinforces the interphase strength,leading to homogeneous Li deposition with dendrite-free *** from these merits,the Li metal is densely and uniformly deposited on the MgF_(2)/C@PP separator side rather than on the current collector ***,the symmetric cell with MgF_(2)/C@PP exhibits superb Li plating/stripping performance over 2800 h at 1 mA cm^(-2)and 2 mA h cm^(-2).More importantly,the assembled Li@MgF_(2)/C@PPILiFePO4full cell with a low negative/positive ratio of 3.6delivers an impressive cyclability with 82.7%capacity retention over 1400 cycles at 1 C.

关键词： Lithium metal batteries Separator modification MgF_(2) Reverse deposition Mechanochemical reaction

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