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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 & Technology Jianghan University Applied materials Division Argonne National Laboratory State key laboratory of Organic Electronics and Information Displays & Institute of Advanced materials (IAM) Nanjing University of Posts & Telecommunications

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 MgF2/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 MgF2and 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 MgF2/C@PP separator side rather than on the current collector ***,the symmetric cell with MgF2/C@PP exhibits superb Li plating/stripping performance over 2800 h at 1 mA cm-2and 2 mA h *** importantly,the assembled Li@MgF2/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 Mechanochemical reaction MgF2 Reverse deposition Separator modification

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A low-cost wide bandgap polymer based on carboxylate substituted thiazole enables efficient organic solar cells with remarkable batch-to-batch reproducibility

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Science China Chemistry 2025年第2期68卷 733-744页

作者： Xiaodong Zhu Yuchen Lei Jianhong Gao Yanjun He Jinsicheng Liu Qian Guo Xiang Gao Liwei Xiong Xunchang Wang Renqiang Yang Zhitian Liu Hubei Engineering Technology Research Center of optoelectronic and New Energy materials Hubei Key Laboratory of Plasma Chemistry and Advanced MaterialsSchool of Materials Science and EngineeringWuhan Institute of TechnologyWuhan 430205China key laboratory of optoelectronic Chemical materials and Devices(Ministry of Education) School of Optoelectronic Materials&TechnologyJianghan UniversityWuhan 430056China

Constructing the low-cost,high-efficiency,and good batch-to-batch reproducibility polymer donor is vitally important for the application of organic solar ***,we develop a structurally simple carboxylate-substituted thiazole as an electronwithdrawing building block to construct a low-cost polymer,PBTTzE,containing a facilely prepared chlorinated benzo[1,2-b:4,5-b′]dithiophene(BDTCl)donor *** from synergistic electron deficient effects of chlorination and ester group and C=N,as well as the noncovalent interaction of S…O and S…N,PBTTzE exhibits a deep HOMO energy level(−5.59 eV),and a planar skeleton *** combined with the IT-4F acceptor,the polymer(54 kDa)demonstrated a champion PCE of 15.87%,which is the highest value in the IT-4F-based binary devices to ***,PBTTzE exhibits excellent batch-tobatch reproducibility due to its very similar PCEs within a range of 43–76 *** addition,an alloyed state and complementary absorption can be formed between PM6 and ***,in a ternary device with PBTTzE added to the PM6:BTP-eC9 blend,a top PCE of 18.76%is achieved due to the suppressed energy loss,prolonged exciton diffusion distance,and improved charge *** work demonstrates that the carboxylate-substituted thiazole is a highly promising acceptor unit for constructing low-cost and high-performance polymers.

关键词： carboxylate substituted thiazole polymer donor low-cost batch-to-batch reproducibility organic solar cells

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Controlled cationic ring-opening polymerization of L-lactide by organic ion pair:novel approach to isotactic-rich and crystalline polylactide

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Science China Chemistry 2025年第1期68卷 394-402页

作者： Zhiqiang Ding Mingqian Wang Zijing Zhou Bin Wang Yuesheng Li Tianjin key laboratory of Composite&functional materials School of Materials Science and EngineeringTianjin UniversityTianjin 300350China

Living/controlled cationic ring-opening polymerization(ROP)of L-lactide is a promising approach to isotactic-rich and crystalline poly(L-lactide).In contrast with the unsubstituted lactones,L-LA can not be polymerized by organic Lewis acids or carbenium ions,and the state of the art in this field is the cationic ROP of L-LA catalyzed by BrФnsted acid/alcohol system via activated monomer ***,we reported the first example of controlled cationic ROP of L-LA by using Meerweintype ion pair[Me_(3)O]^(+)[B(C_(6)F_(5))_(4)]^(-)as the catalyst.[Me_(3)O]^(+)[B(C_(6)F_(5))_(4)]^(-)promoted rapid L-LA cationic polymerization in the absence of alcohol,producing isotactic-rich and crystalline PLLA without transesterification and epimerization side *** activated chain end mechanism,involving twice S_(N)2 substitution and configuration-inversion(S→R→S)with the assistance of released Me_(2)O,was proposed and further verified by density functional theory and control *** work expands the catalytic toolbox of isotactic-rich and crystalline polylactide *** represents a unique example of cationic-controlled polymerization of L-LA catalyzed by an organic ion pair.

关键词： organic ion pair controlled cationic ring-opening polymerization activated chain end mechanism isotactic-rich poly-lactide

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Structuring MoO3-polyoxometalate hybrid superstructures to boost electrocatalytic hydrogen evolution reaction

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Chinese Chemical Letters 2025年第2期36卷 239-243页

作者： Bowen Li Ting Wang Ming Xu Yuqi Wang Zhaoxing Li Mei Liu Wenjing Zhang Ming Feng key laboratory of functional materials Physics and Chemistry of the Ministry of Education Jilin Normal University

Improving the surface atoms utilization efficiency of catalysts is extremely important for large-scale H2production by electrochemical water splitting,but it remains a great ***,we reported two kinds of Mo O3-polyoxometalate hybrid nanobelt superstructures (MoO3-POM HNSs,POM=PW12O40and Si W12O40) using a simple hydrothermal *** superstructure with highly uniform nanoparticles as building blocks can expose more surface atoms and emanate increased specific surface *** incorporated POMs generated abundant oxygen vacancies,improved the electronic mobility,and modulated the surface electronic structure of MoO3,allowing to optimize the H*adsorption/desorption and dehydrogenation kinetics of ***,the as-prepared MoO3-PW12O40HNSs electrodes not only displayed the low overpotentials of 108 mV at 10 mA/cm2current density in 0.5 mol/L H2SO4electrolyte but also displayed excellent long-term *** hydrogen evolution reaction （HER） performance of MoO3-POM superstructures is significantly better than that of corresponding bulk materials MoO3@PW12O40and Mo O3@Si W12O40,and the overpotentials are about 8.3 and 4.9 times lower than that of single Mo *** work opens an avenue for designing highly surface-exposed catalysts for electrocatalytic H2production and other electrochemical applications.

关键词： Electrocatalysis Hydrogen production Metal oxide Polyoxometalate Superstructure

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An electrically activable nanochip to intensify gas-ionic-immunotherapy

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Science Bulletin 2025年第3期70卷 390-406页

作者： Gang Wang Jingrui Li Shumin Sun Yuqi Yang Zhihui Han Zifan Pei Liang Cheng Institute of functional Nano&Soft materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China

Excess intracellular H_(2)S induces destructive mitochondrial toxicity,while overload of Zn^(2+)results in cell pyroptosis and potentiates the tumor immunogenicity for ***,the precise delivery of both therapeutics remains a great ***,an electrically activable ZnS nanochip for the controlled release of H_(2)S and Zn^(2+)was developed for enhanced gas-ionic-immunotherapy(GIIT).Under an electric field,a locality with particularly high concentrations of H_(2)S and Zn^(2+)was established by the voltage-controlled degradation of the ZnS nanoparticles(NPs).Consequently,the ZnS nanochip-mediated gas-ionic therapy(GIT)resulted in mitochondrial membrane potential depolarization,energy generation inhibition,and oxidative stress imbalance in tumor ***,the cyclic guanosine monophosphate-adenosine monophosphate synthase-stimulator of interferon genes(cGAS-STING)signaling pathway was activated due to the mitochondrial ***,the released Zn^(2+)resulted in the increase of the intracellular Zn levels and cell pyroptosis,which enhanced the immunogenicity via the release of damage-associated molecular patterns(DAMPs).In vitro and in vivo studies revealed that the ZnS nanochip-based GIT effectively eliminated the tumors under an electric field and mobilized the cytotoxic T lymphocytes for *** combination withαCTLA-4 further promoted the adaptive immune response and inhibited tumor metastasis and long-term tumor *** work presented an electrically activable ZnS nanochip for combined immunotherapy,which might inspire the development of electric stimulation therapy.

关键词： H_(2)S gas therapy lonic interference therapy Electrically controll eddelivery Cell pyroptosis CGAS-STING pathway

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Spin-selective and frequency-shift meta-holography based on reconfigurable origami chiral metasurface

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Science China(Physics,Mechanics & Astronomy) 2025年第2期68卷 121-131页

作者： Zhibiao Zhu Lixin Jiang Zhe Qin Yongfeng Li Jiafu Wang Yuxiang Jia Lin Zheng Shaobo Qu Shaanxi key laboratory of Artificially-Structured functional materials and Devices Air Force Engineering UniversityXi’an710051China

Origami-based reconfigurable metasurfaces have emerged as a versatile paradigm for dynamically manipulating electromagnetic(EM) waves due to their advantages, such as low manufacturing cost, lightweight, and structural deformability. Three-dimensional(3D) deformation can intensify asymmetry among structures, making origami metasurfaces particularly suitable for realizing reconfigurable chiral responses. However, previous studies have primarily focused on modulating spectral properties,such as chiral switching and resonant frequency shifting. There remains ample room for further exploration in complex wavefront manipulation and holographic imaging applications. This paper proposes a simple and efficient deformation method for origami metasurfaces that transforms a spin-insensitive planar metasurface into a 3D metasurface by folding. The breaking of mirror symmetry induces a pronounced chiral response. The binary amplitude is modulated within each pixel. When folded at angles of +θ and-θ, the designed origami metasurface generates distinct images under left-handed circularly polarized(LCP)wave incidence. Meanwhile, holographic encryption is achieved under right-handed circularly polarized(RCP) wave ***, by leveraging origami's reconfigurability, the holographic imaging's operating frequency can be shifted. The experimental results agree well with the numerical calculations and full-wave simulations, demonstrating the broad application potential of this method in areas such as multi-channel imaging, information encryption technologies, and stealth.

关键词： hologram origami metasurface chiral response

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Na_(2)B_(6)SO_(13) with unprecedented [B_(6)SO_(13)]_(∞) double chains and largest birefringence among borosulfates induced by the uniform arrangement of [B_(3)O_(7)] units

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Science China Chemistry 2025年第2期68卷 475-480页

作者： Jinbin Fan Ziting Yan Zilong Chen Huimin Li Zhihua Yang Fangfang Zhang Shilie Pan Research Center for Crystal materials State Key Laboratory of Functional Materials and Devices for Special Environmental ConditionsXinjiang Key Laboratory of Functional Crystal MaterialsXinjiang Technical Institute of Physics and ChemistryChinese Academy of SciencesUrumqi 830011China Center of materials Science and optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Birefringence is crucial for birefringent crystals to modulate polarized light and nonlinear optical crystals to enable *** is closely related to the arrangement of advantageous functional groups with large microcosmic polarizability anisotropy in the ***,designing crystals with large birefringence by modulating the arrangement of advantageous functional groups is still a *** this work,the arrangement of the advantageous[B_(3)O_(7)]groups is optimized by introducing rigid tetrahedral[SO_(4)]groups,resulting in a novel boron-rich borosulfate,Na_(2)B_(6)SO_(13) ,which exhibits unprecedented[B_(6)SO_(13)]_(∞)double chain and an enhanced birefringence(Δn=0.07 at 589.3 nm)against the borate parent *** calculations confirm that the birefringence is mainly attributable to the uniform alignment of[B_(3)O_(7)]***_(2)B_(6)SO_(13) also possesses a deep ultraviolet(DUV)cutoff edge(λfunctional groups.

关键词： borosulfate deep ultraviolet birefringence modulated groups

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Introducing strong metal–oxygen bonds to suppress the Jahn-Teller effect and enhance the structural stability of Ni/Co-free Mn-based layered oxide cathodes for potassium-ion batteries

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Journal of Energy Chemistry 2025年第2期101卷 713-722页

作者： Yicheng Lin Shaohua Luo Pengyu Li Jun Cong Wei Zhao Lixiong Qian Qi Sun Shengxue Yan School of materials Science and Engineering Northeastern University School of Resources and materials Northeastern University at Qinhuangdao key laboratory of Dielectric and Electrolyte functional Material Hebei Province

Mn-based layered oxides（KMO） have emerged as one of the promising low-cost cathodes for potassiumion batteries（PIBs）.However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the Jahn-Teller（JT） effect associated with Mn-ion,the cathode exhibits poor structural ***,we propose a strategy to enhance structural stability by introducing robust metal-oxygen（M-O） bonds,which can realize the pinning effect to constrain the distortion in the transition metal（TM） ***,all the elements employed have exceptionally high crustal *** a proof of concept,the designed K0.5Mn0.9Mg0.025Ti0.025Al0.05O2cathode exhibited a discharge capacity of approximately 100 mA h g-1at 20 mA g-1with 79% capacity retention over 50 cycles,and 73% capacity retention over 200 cycles at 200 mA g-1,showcased much better battery performance than the designed cathode with less robust M-O *** properties of the formed M-O bonds were investigated using theoretical *** enhanced dynamics,mitigated JT effect,and improved structural stability were elucidated through the in-situ X-ray diffractometer（XRD）,in-situ electrochemical impedance spectroscopy（EIS）(and distribution of relaxation times（DRT） method),and ex-situ X-ray absorption fine structure（XAFS） *** study holds substantial reference value for the future design of costeffective Mn-based layered cathodes for PIBs.

关键词： Jahn-Teller effect Layered oxide cathodes Low-cost Potassium-ion batteries Robust M–O bonds

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Defect Engineering with Rational Dopants Modulation for High‑Temperature Energy Harvesting in Lead‑Free Piezoceramics

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Nano-Micro Letters 2025年第3期17卷 87-101页

作者： Kaibiao Xi Jianzhe Guo Mupeng Zheng Mankang Zhu Yudong Hou key laboratory of Advanced functional materials Ministry of EducationCollege of Materials Science and EngineeringBeijing University of TechnologyBeijing 100124People’s Republic of China

High temperature piezoelectric energy harvester(HTPEH)is an important solution to replace chemical battery to achieve independent power supply of HT wireless ***,simultaneously excellent performances,including high figure of merit(FOM),insulation resistivity(ρ)and depolarization temperature(Td)are indispensable but hard to achieve in lead-free piezoceramics,especially operating at 250°C has not been reported ***,well-balanced performances are achieved in BiFeO3–BaTiO3 ceramics via innovative defect engineering with respect to delicate manganese *** to the synergistic effect of enhancing electrostrictive coefficient by polarization configuration optimization,regulating iron ion oxidation state by high valence manganese ion and stabilizing domain orientation by defect dipole,comprehensive excellent electrical performances(Td=340°C,ρ250°C>10^(7)Ωcm and FOM_(250°C)=4905×10^(–15)m^(2)N^(−1))are realized at the solid solubility limit of manganese *** HT-PEHs assembled using the rationally designed piezoceramic can allow for fast charging of commercial electrolytic capacitor at 250°C with high energy conversion efficiency(η=11.43%).These characteristics demonstrate that defect engineering tailored BF-BT can satisfy high-end HT-PEHs requirements,paving a new way in developing selfpowered wireless sensors working in HT environments.

关键词： Lead-free piezoceramic Defect engineering Dopants modulation High-temperature Piezoelectric energy harvester

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Methyl Groups Pendant on Triphenylmethane Toward Modulating Thermal Stability and Dielectric Properties of the Crosslinkable Fluorinated Polyimide Films with High Transparency

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Chinese Journal of Polymer Science 2025年第2期43卷 316-327页

作者： Wen Yang Liang Yuan Kai Gong Ruo-Han Zhang Lan Lei Hui Li School of Chemistry and Chemical Engineering Shandong Key Laboratory of Fluorine Chemistry and Chemical Engineering MaterialsUniversity of JinanJinan250022China School of materials Science and Engineering Tianjin Key Laboratory of Composite and Functional MaterialsTianjin UniversityTianjin300350China

It is urgent to develop high-performance polyimide(PI)films that simultaneously exhibit high transparency,exceptional thermal stability,mechanical robustness,and low dielectric to fulfil the requirements of flexible display ***,a series of fluorinated polyimide films(FPIs)were fabricated by the condensation of 5,5′-(perfluoropropane-2,2-diyl)bis(isobenzofuran-1,3-dione)(6FDA)and the fluorinated triphenylmethane diamine monomer(EDA,MEDA and DMEDA)with heat-crosslinkable tetrafluorostyrene side groups,which was incorporated by different numbers of methyl groups pendant in the ortho position of amino ***,the FPI films underwent heating to produce crosslinking FPIs(C-FPIs)through the self-crosslinking of double bonds in the *** transparency,solvent resistance,thermal stability,mechanical robustness and dielectric properties of FPI and C-FPI films can be tuned by the number of methyl groups and crosslinking,which were deeply investigated by virtue of molecular dynamics(MD)simulations and density functional theory(DFT).As a result,all the films exhibited exceptional optically colorless and transparent,with transmittance in the visible region of 450-700 nm exceeding 79.9%,and the cut-off wavelengths(λ_(off))were nearly 350 *** thermal decomposition temperatures at 5% weight loss(T_(d5%))for all samples exceeded 504℃.These films exhibited a wide range of tunable tensile strength(46.5-75.1 MPa).Significantly,they showed exceptional dielectric properties with the dielectric constant of 2.3-2.5 at full frequency(10^(7)-20 Hz).This study not only highlights the relationship between the polymer molecular structure and properties,but offer insights for balancing optical transparency,heat resistance and low dielectric constant in PI films.

关键词： Crosslinkable fluorinated polyimide Methyl group Triphenylmethane Transparency Thermal stability Low dielectric constant

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