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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li department of chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University State Key Laboratory of Surface physics and department of physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable challenge.Herein,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as templates.The key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon matrix.The mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion lengths.This method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

Nanofluidic memristor based on the elastic deformation of nanopores with nanoparticle adsorption

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National Science Review 2024年第4期11卷 46-54页

作者： Xi Zhou Yuanyuan Zong Yongchang Wang Miao Sun Deli Shi Wei Wang Guanghua Du Yanbo Xie department of chemistry and Chemical engineering Northwestern Polytechnical University school of Physical Science and Technology Northwestern Polytechnical University school of Aeronautics and Institute of Extreme Mechanics Northwestern Polytechnical University Institute of Modern physics Chinese Academy of Sciences

The memristor is the building block of neuromorphic computing. We report a new type of nanofluidic memristor based on the principle of elastic strain on polymer nanopores. With nanoparticles absorbed at the wall of a single conical polymer nanopore, we find a pinched hysteresis of the current within a scanning frequency range of 0.01–0.1 Hz, switching to a diode below 0.01 Hz and a resistor above 0.1 Hz. We attribute the current hysteresis to the elastic strain at the tip side of the nanopore, caused by electrical force on the particles adsorbed at the inner wall surface. Our simulation and analytical equations match well with experimental results, with a phase diagram for predicting the system transitions. We demonstrate the plasticity of our nanofluidic memristor to be similar to a biological synapse. Our findings pave a new way for ionic neuromorphic computing using nanofluidic memristors.

关键词： nanofluidics memristor neurocomputing elastic deformation

Deciphering the controlling factors for phase transitions in zeolitic imidazolate frameworks

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National Science Review 2024年第4期11卷 151-163页

作者： Tao Du Shanwu Li Sudheer Ganisetti Mathieu Bauchy Yuanzheng Yue Morten M.Smedskjaer department of chemistry and Bioscience Aalborg University department of Mechanical engineering-engineering Mechanics Michigan Technological University physics of Amo Rphous and Inorganic Solids Laboratory(PARISlab) Department of Civil and Environmental EngineeringUniversity of CaliforniaLos Angeles

Zeolitic imidazolate frameworks（ZIFs） feature complex phase transitions, including polymorphism,melting, vitrification, and polyamorphism. Experimentally probing their structural evolution during transitions involving amorphous phases is a significant challenge, especially at the medium-range length scale. To overcome this challenge, here we first train a deep learning-based force field to identify the structural characteristics of both crystalline and non-crystalline ZIF phases. This allows us to reproduce the structural evolution trend during the melting of crystals and formation of ZIF glasses at various length scales with an accuracy comparable to that of ab initio molecular dynamics, yet at a much lower computational cost. Based on this approach, we propose a new structural descriptor, namely, the ring orientation index, to capture the propensity for crystallization of ZIF-4(Zn（Im）2, Im = C3H3N2-) glasses, as well as for the formation of ZIF-zni(Zn（Im）2) out of the high-density amorphous phase. This crystal formation process is a result of the reorientation of imidazole rings by sacrificing the order of the structure around the zinc-centered tetrahedra. The outcomes of this work are useful for studying phase transitions in other metal-organic frameworks（MOFs） and may thus guide the development of MOF glasses.

关键词： metal-organic frameworks phase transitions melting glass formation transferable deep learning force field ring orientation

Structural transformation from Waugh-type to Keggin-type polyoxomolybdate-based crystalline material for photo/electrocatalysis

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Rare Metals 2024年第5期43卷 2241-2250页

作者： Pei-Sen Wang Zi-Tong Wang Ya-Ya Tan Peng Chen Xue-Cheng Zhang Lu-Nan Zhang Yong-Ge Wei Lu-Bin Ni school of chemistry and Chemical engineering Yangzhou University State Key Laboratory of Natural and Biomimetic Drugs Peking University Key Lab of Organic Optoelectronics and molecular engineering of Ministry of Education Department of Chemistry Tsinghua University

An inorganicDorganic hybrid crystalline material (Si Mo12O40)[Cu（2,2'-bipy）2]2·2H2O （Complex 1,2,2'-bipy=2,2'-bipyridine） was synthesized for the first time by using 2,2'-bipy and transition metal copper to convert Waugh-type polyoxometalate[Mn Mo9O32]6-into a Keggin polyoxometalate structure[Si Mo12O40]4-under hydrothermal conditions in glass vials.Single crystal tests and a series of characterizations were carried out on Complex 1.The structure of Complex 1 is composed of[Si Mo12O40]4-and[CuII（2,2'-bipy）2]2+.The five-coordinated Cu is connected to two 2,2'-bipy through CuDN bonds,forming an approximately square structure.Astonishingly,Complex 1 exhibited good photocatalytic performance for methylene blue degradation and electrocatalytic nitrite reduction properties simultaneously.

关键词： Polyoxometalates Inorganic–organic hybrid materials Photocatalytic Electrocatalytic

Iron-Catalyzed Reductive C(aryl)—Si Cross-Coupling of Diaryl Ethers with Chlorosilanes

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Chinese Journal of chemistry 2024年第6期42卷 578-584页

作者： Pei Liu Baowei Wu Xuefeng Cong Jie Kong school of chemistry and Chemical engineering Northwestern Polytechnical UniversityXi'anShaanxi710072 China Institute of molecular Plus Department of Chemistry and Haihe Laboratory of Sustainable Chemical TransformationsTianjin University92 Weijin RoadTianjin300072 China

The reductive cross-coupling between C(aryl)—O and Si—Cl bonds is of much importance as a valuable strategy for the construction of C(aryl)—Si bonds but has remained a great challenge.Herein,we report a reductive cross-coupling of diaryl ethers and chlorosilanes via strong electrophilic C(aryl)—O and Si—Cl bonds cleavage by iron catalysis,which constitutes an efficient protocol for the synthesis of a range of functionalized arylsilanes.The combination of low cost FeCl2 as the precatalyst and iPrMgCl as the reductant shows high activity in the successive cleavage of unactivated C(aryl)—O bonds of diaryl ethers and strong electrophilic Si—Cl bonds of chlorosilanes,allowing their cross-coupling in a reductive fashion.The low-valent iron species generated in situ by reduction of FeCl2 with iPrMgCl was proposed,which prefers to initially cleavage the C(aryl)—O bond of diaryl ethers with the chelation help of an o-amide auxiliary.

关键词： Cross-coupling Diaryl ethers Chlorosilanes C—O bond cleavage Iron catalyst 3d transition metals Selectivity Regioselectivity

Combining cisplatin and a STING agonist into one molecule for metalloimmunotherapy of cancer

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National Science Review 2024年第1期11卷 107-119页

作者： Shuren Zhang Dongfan Song Wenhao Yu Ji Li Xiaoyu Wang Yachao Li Zihan Zhao Qi Xue Jing Zhao Jie P.Li Zijian Guo State Key Laboratory of Coordination chemistry School of Chemistry and Chemical EngineeringChemistry and Biomedicine Innovation Center (ChemBIC) Nanjing University department of Urology Afflliated Drum Tower HospitalMedical SchoolNanjing University Nanchuang (Jiangsu)Institute of chemistry and Health

Mounting evidence suggests that strategies combining DNA-damaging agents and stimulator of interferon genes(STING) agonists are promising cancer therapeutic regimens because they can amplify STING activation and remodel the immunosuppressive tumor microenvironment. However, a single molecular entity comprising both agents has not yet been developed. Herein, we designed two PtIV-MSA-2 conjugates(Ⅰand Ⅱ) containing the DNA-damaging chemotherapeutic drug cisplatin and the innate immuneactivating STING agonist MSA-2; these conjugates showed great potential as multispecific small-molecule drugs against pancreatic cancer. Mechanistic studies revealed that conjugate Ⅰ upregulated the expression of transcripts associated with innate immunity and metabolism in cancer cells, significantly differing from cisplatin and MSA-2. An analysis of the tumor microenvironment demonstrated that conjugate I could enhance the infiltration of natural killer(NK) cells into tumors and promote the activation of T cells, NK cells and dendritic cells in tumor tissues. These findings indicated that conjugate I, which was created by incorporating a Pt chemotherapeutic drug and STING agonist into one molecule, is a promising and potent anticancer drug candidate, opening new avenues for small-molecule-based cancer metalloimmunotherapy.

关键词： platinum drug STING agonist single-molecule multitarget metalloimmunology

Designing metal-organic framework fiber network reinforced polymer electrolytes to provide continuous ion transport in solid state lithium metal batteries

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Nano Research 2024年第4期17卷 2719-2727页

作者： Wanqing Fan Ying Huang Meng Yu Kaihang She Jingren Gou Zheng Zhang MOE Key Laboratory of Material physics and chemistry Under Extraordinary Conditions School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Beijing Key Laboratory of Membrane Materials and engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Polyethylene oxide(PEO)-based solid-state electrolytes are considered ideal for electrolyte materials in solid-state lithium metal batteries(SSLMBs).However,practical applications are hindered by the lower conductivity and poor interfacial stability.Here,we propose a strategy to construct a three-dimensional(3D)fiber network of metal-organic frameworks(MOFs).Composite solid electrolytes(CSEs)with continuous ion transport pathways were fabricated by filling a PEO polymer matrix in fibers containing interconnected MOFs.This 3D fiber network provides a fast Li+transport path and effectively improves the ionic conductivity(1.36×10^(-4) S·cm^(-1),30℃).In addition,the network of interconnected MOFs not only effectively traps the anions,but also provides sufficient mechanical strength to prevent the growth of Li dendrites.Benefiting from the advantages of structural design,the CSEs stabilize the Li/electrolyte interface and extend the cycle life of the Li-symmetric cells to 3000 h.The assembled SSLMBs exhibit excellent cycling performance at both room and high temperatures.In addition,the constructed pouch cells can provide an areal capacity of 0.62 mA·h·cm^(-2),which can still operate under extreme conditions.This work provides a new strategy for the design of CSEs with continuous structure and stable operation of SSLMBs.

关键词： polyethylene oxide(PEO) solid-state lithium metal batteries(SSLMBs) three-dimensional fiber network composite solid electrolytes(CSEs)

Liquid metal biomaterials: translational medicines,challenges and perspectives

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National Science Review 2024年第2期11卷 264-284页

作者： Hanchi Xu Jincheng Lu Yikuang Xi Xuelin Wang Jing Liu department of Biomedical engineering School of Medicine Tsinghua University Beijing Tsinghua Changgung Hospital School of Clinical Medicine Tsinghua University Shanghai World Foreign Language Academy Beijing Advanced Innovation Center for Biomedical engineering School of Engineering MedicineBeihang University Beijing Key Lab of Cryo-Biomedical engineering and Key Lab of Cryogenics Technical Institute of Physics and Chemistry Chinese Academy of Sciences

Until now, significant healthcare challenges and growing urgent clinical requirements remain incompletely addressed by presently available biomedical materials. This is due to their inadequate mechanical compatibility, suboptimal physical and chemical properties, susceptibility to immune rejection, and concerns about long-term biological safety. As an alternative, liquid metal(LM) opens up a promising class of biomaterials with unique advantages like biocompatibility, flexibility, excellent electrical conductivity,and ease of functionalization. However, despite the unique advantages and successful explorations of LM in biomedical fields, widespread clinical translations and applications of LM-based medical products remain limited. This article summarizes the current status and future prospects of LM biomaterials, interprets their applications in healthcare, medical imaging, bone repair, nerve interface, and tumor therapy, etc.Opportunities to translate LM materials into medicine and obstacles encountered in practices are discussed.Following that, we outline a blueprint for LM clinics, emphasizing their potential in making new-generation artificial organs. Last, the core challenges of LM biomaterials in clinical translation, including bio-safety,material stability, and ethical concerns are also discussed. Overall, the current progress, translational medicine bottlenecks, and perspectives of LM biomaterials signify their immense potential to drive future medical breakthroughs and thus open up novel avenues for upcoming clinical practices.

关键词： liquid metal biomaterials translational medicine clinical device healthcare therapeutics

Open-Shell Oligomers and Polymers: Theory, Characterization Methods, molecular Design, and Applications

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Chinese Journal of Polymer Science 2024年第4期42卷 417-436页

作者： Xue-Qing Wang Cheng Song Ting Lei Key Laboratory of Polymer chemistry and physics(Ministry of Education) School of Materials Science and EngineeringPeking UniversityBeijing100871China

Open-shell oligomers and polymers have exhibited intriguing electronic and magnetic properties, making them highly desirable for a wide range of applications, including ambipolar organic field-effect transistors (OFETs), photodetectors, organic thermoelectrics, and spintronics. Although open-shell ground states have been observed in certain small molecules and doped organic semiconductors, the exploration of open-shell ground-state conjugated polymers is still limited, and the strategies for designing these polymers remain obscure. This review aims to briefly introduce the theory and characterization methods of open-shell conjugated polymers, along with an overview of recent progress and applications. The objective is to stimulate further advancements and investigations in this promising area by shedding light on the potential of open-shell conjugated polymers and the challenges that lie ahead.

关键词： Conjugated polymers Open-shell molecules High-spin ground state Donor-acceptor(D-A)polymers Optoelectronic and magnetic properties

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Electrochemical CO_(2)reduction to C_(2+)products over Cu/Zn intermetallic catalysts synthesized by electrodeposition

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Frontiers in Energy 2024年第1期18卷 80-88页

作者： Ting DENG Shuaiqiang JIA Shitao HAN Jianxin ZHAI Jiapeng JIAO Xiao CHEN Cheng XUE Xueqing XING Wei XIA Haihong WU Mingyuan HE Buxing HAN school of chemistry and molecular engineering East China Normal UniversityShanghai 200062China Institute of Eco-Chongming Shanghai 202162China Institute of High Energy physics Chinese Academy of SciencesBeijing 100049China Institute of chemistry Chinese Academy of SciencesBeijing 100190China

Electrocatalytic CO_(2)reduction(ECR)offers an attractive approach to realizing carbon neutrality and producing valuable chemicals and fuels using CO_(2)as the feedstock.However,the lack of cost-effective electrocatalysts with better performances has seriously hindered its application.Herein,a one-step co-electrodeposition method was used to introduce Zn,a metal with weak^(*)CO binding energy,into Cu to form Cu/Zn intermetallic catalysts(Cu/Zn IMCs).It was shown that,using an H-cell,the high Faradaic efficiency of C_(2+)hydrocarbons/alcohols()could be achieved in ECR by adjusting the surface metal components and the applied potential.In suitable conditions,FEC_(2+)and current density could be as high as 75%and 40 mA/cm^(2),respectively.Compared with the Cu catalyst,the Cu/Zn IMCs have a lower interfacial charge transfer resistance and a larger electrochemically active surface area(ECSA),which accelerate the reaction.Moreover,the^(*)CO formed on Zn sites can move to Cu sites due to its weak binding with*CO,and thus enhance the C–C coupling on the Cu surface to form C_(2+)products.

关键词： carbon dioxide electroreduction electrochemistry co-electrodeposition intermetallic catalysts value-added chemicals