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Scalable synthesis of N-doped Si/G@voids@C with porous structures for high-performance anode of lithium-ion batteries

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Rare Metals 2023年第12期42卷 4091-4102页

作者： Lei Wang Yan Jiang Shao-Yuan li Xiu-Hua Chen Feng-Shuo Xi Xiao-Han Wan Wen-Hui Ma Rong Deng Faculty of Metallurgical and Energy Engineering State Key Laboratory of Complex Nonferrous Metal Resources Clean UtilizationKunming University of Science and TechnologyKunming 650093China School of Materials Science and Engineering Yunnan UniversityKunming 650091China School of Science and Technology Pu'erUniversityPu'er 665000China School of Photovoltaic and Renewable Energy Engineering(SPREE) University of New South WalesSydney 2052Australia

The co-utilization of silicon(Si) and graphite(G) has been considered as the preferred strategy to achieve high energy density anode materials,but the effective synergistic integration of Si and graphite is still a challenge and it is necessary to find a scheme to accommodate the large-scale production of Si/graphite *** this work,silicon cutting waste from the photovoltaic industry was used as raw material,mixed with graphite,pitch,and polyvinylpyrrolidone,and subjected to high-energy ball *** mixture was then heated in an Ar atmosphere for the carbon coating,and the resulting Si/graphite/carbon(Si/G/C) composite was etched to remove the thicker SiOx layer formed on the Si surface to allow the pores between the Si and the carbon matrix to obtain Si@voids/G@*** from the integrated structural design and the significantly enhanced electronic conductivity,the Si/G@voids@C composite exhibited the first dischargespecific capacity of 2530 mAh·g^(-1) with an initial coulombic efficiency(ICE) of 86.7%,and the remaining capacity exceeded 1000 mAh·g^(-1) after 550 cycles at 1.5A·g^(-1).Notably,full lithium-ion batteries with a Si/G@voids@C anode and liFePO_4 cathode delivered a stable capacity of 140 mAh·g^(-1).The synthesis method is facile and cost-effective,providing an integration strategy for Si and G with a potential scheme for large-scale commercial applications.

关键词： Silicon/graphite anodes Surface coating Integration strategy Silicon cutting waste High-energy ball milling lithium-ion battery(liB)

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Interface-modulated approach toward multilevel metal oxide nanotubes for lithium-ion batteries and oxygen reduction reaction

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Nano Research 2016年第8期9卷 2445-2457页

作者： Jiashen Meng Chaojiang Niu Xiong liu Ziang liu Hongliang Chen Xuanpeng Wang Jiantao li Wei Chen Xuefeng Guo liqiang Mai state key laboratory of Advcrnced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Center for Nanochemistry Beijing National Laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Unstable and Stable Species College of Chemistry and Molecular Engineering Peking University Beijing 100871 China

Metal oxide hollow structures with multilevel interiors are of great interest for potential applications such as catalysis, chemical sensing, drug delivery, and energy storage. However, the controlled synthesis of multilevel nanotubes remains a great challenge. Here we develop a facile interface-modulated approach toward the synthesis of complex metal oxide multilevel nanotubes with tunable interior structures through electrospinning followed by controlled heat treatment. This versatile strategy can be effectively applied to fabricate wire-in-tube and tube- in-tube nanotubes of various metal oxides. These multilevel nanotubes possess a large specific surface area, fast mass transport, good strain accommodation, and high packing density, which are advantageous for lithium-ion batteries （liBs） and the oxygen reduction reaction （ORR）. Specifically, shrinkable CoMn204 tube-in-tube nanotubes as a lithium-ion battery anode deliver a high discharge capacity of -565 mAh-g-1 at a high rate of 2 A.g-~, maintaining 89% of the latter after 500 cycles. Further, as an oxygen reduction reaction catalyst, these nanotubes also exhibit excellent stability with about 92% current retention after 30,000 s, which is higher than that of commercial Pt/C （81%）. Therefore, this feasible method may push the rapid development of one-dimensional （1D） nanomaterials. These multifunctional nanotubes have great potential in many frontier fields.

关键词： interface-modulatedapproach multilevel nanotubes metal oxide lithium-ion battery (liB~ ~ oxygen reduction reaction(ORR)

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Metal-mediated catalysis in the gas phase: A review

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Chinese Journal of Catalysis 2017年第9期38卷 1515-1527页

作者： Xiao‐Na li Xiu‐Ping Zou Sheng‐Gui He Beijing National laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China School of chemistry and Chemical Engineering South China University of Technology Guangzhou 510641 Guangdong China

This review summarizes a variety of experimentally identified gas‐phase catalytic cycles,all of which are mediated by atomic metal ions,bare metal clusters,metal oxide clusters or metal *** is placed on the latest advances in the unique catalytic reactivity of cluster‐confined single noble metal *** cycles discussed in this paper cover a wide range of inorganic and organic *** use of start‐of‐the‐art mass spectrometric instrumentation in conjunction with quantum chemistry calculations is also reported,as these techniques have determined the mechanistic details of the elementary steps of such catalytic *** important role of gas‐phase data in guiding the rational design of better‐performing catalysts in related condensed phase reactions is also *** particular,this review focuses on the following three topics:(1)the catalytic oxidation of carbon monoxide,(2)the catalytic functionalization of methane,and(3)catalytic decarboxylation.

关键词： Metal catalysis Clusters Single atom catalysts Carbon monoxide Methane

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An important functional group, benzo[1,3]dioxole, of alkaloids induces the formation of the human telomeric DNA G-quadruplex

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Chinese Science Bulletin 2011年第7期56卷 613-617页

作者： YANG Shu XIANG JunFeng YANG QianFan ZHOU QiuJu ZHANG XiuFeng li Qian TANG Yalin XU GuangZhi Beijing National laboratory for Molecular Sciences Centre for Molecular SciencesState Key Laboratory for Structural Chemistry for Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China Graduate University of Chinese Academy of Sciences Beijing 100049China

Over the past few decades, numerous molecules have been discovered or designed to interact efficiently and selectively with a peculiar DNA structure named G-quadruplex. Some of these molecules have been developed as anticancer agents. To aid the design of anticancer agents, the ability of alkaloids possessing Protoberberine and Benzophenanthridine groups to induce the formation of G-quadruplexes were studied using CD spectroscopy. By careful examination of their structures, we found that a benzo[1,3]dioxole group plays an important role in influencing their inductive properties. The more functional groups the alkaloids have, the stronger their G-quadruplex inductive ability.

关键词：端粒DNA 生物碱诱导职能人类四链苯抗癌药物

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In-situ generation and global property profiling of metal nanoclusters by ultraviolet laser dissociation-mass spectrometry

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Science China chemistry 2022年第6期65卷 1196-1203页

作者： Zheyi liu Zhaoxian Qin Chaonan Cui Zhixun Luo Bing Yang You Jiang Can Lai Zhipeng Wang Xiaolei Wang Xiang Fang Gao li Fangjun Wang Chunlei Xiao Xueming Yang state key laboratory of Molecular Reaction Dynamics Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China CAS key laboratory of Separation Sciences for Analytical chemistry Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China state key laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China state key laboratory for structural chemistry of unstable and stable species Institute of ChemistryChinese Academy of SciencesBeijing100190China Dalian National laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China National Institute of Metrology Beijing100013China University of Chinese Academy of Sciences Beijing100049China

Metal nanoclusters are promising nanomaterials with unique properties, but only a few ones with specific numbers of metal atoms can be obtained and studied up to now. In this study, we establish a new paradigm of in-situ generation and global study of metal nanoclusters with different sizes, constitutions, and charge states, including both accurate constitution characterization and global activity profiling. The complex mixtures of metal nanoclusters are produced by employing single-pulsed 193-nm laser dissociation of monolayer-protected cluster(MPC) precursors within a high-resolution mass spectrometry(HRMS). More than400 types of bare gold nanoclusters including novel multiply charged(2+ and 3+), S-/P-doped, and silver alloy ones can be efficiently generated and accurately characterized. A distinct size(1 to 142 atoms)-and charge(1+ to 3+)-hierarchy reactivity is clearly observed for the first time. This global cluster study might greatly promote the developments and applications of novel metal nanoclusters.

关键词： metal nanocluster ultraviolet laser dissociation mass spectrometry global property profiling size-and charge-hierarchy

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Magnetic Nanoparticles for the Quantification of Cell Mechanics Using Force-Induced Remnant Magnetization Spectroscopy

Magnetic Nanoparticles for the Quantification of Cell Mechan...

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第十一届全国化学生物学学术会议

作者： Min Xu li Yao state key laboratory for structural chemistry of unstable and stable species Institute of ChemistryChinese Academy of Science University of Chinese Academy of Sciences

Magnetic nanoparticles（MNPs） have emerged as powerful tools for MRI, drug delivery, synergistic chemotherapy and so on1. Recently, a MNPs-based force-induced remnant magnetization spectroscopy（FIRMS） have been used to identify molecular interactions of antigen-antibody, DNA-DNA, aptamer-protein and so on2. Here we use FIRMS to measure cell mechanics. We first investigeted the MNPs-cell interactions from cell mechanics perspective and then use MNPs to label cells, subsequently applied an external centrifugal force with increasing amplitude to the labeled cells. When the applied force exceeds the cell adhesion force, cell detached from substrates, resulting in the decrease of the remanence signal. Therefore, a curve of force-dependent signal change is recorded by FIRMS and the cell adhesion force is obtained.

关键词： Magnetic Nanopaticles Biocompatibility Cell Mechanics FIRMS

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Mechanism on protection of *** outer membrane proteins by periplasmic chaperones SurA and Skp

Mechanism on protection of *** outer membrane proteins by pe...

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第十届全国化学生物学学术会议

作者： geng li Xin Sheng Zhao Beijing National laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesDepartment of Chemical BiologyCollege of Chemistry and Molecular Engineeringand Biodynamic Optical Imaging Center （BIOPIC）Peking University

SurA and Skp are both periplasmic chaperones in the biogenesis of E. coli β–barrel outer membrane proteins（OMPs）. It is commonly assumed that SurA plays a major role, whereas Skp is a minor factor. However, there is no molecular evidence whether their roles are redundant or not. By using different dilution methods, we obtained monodispersed and aggregated OMPs and studied their interactions with Skp and SurA by single–molecule fluorescence resonance energy transfer（smFRET） and fluorescence correlation spectroscopy（FCS）. We found that Skp has the ability to dissolve the aggregated OMPs, while SurA can hardly convert the aggregated OMPs into a monodispersed form, and OMPs protected by the two chaperones possess different conformations and stoichiometries. Our study demonstrates the functional distinctions between Skp and SurA. Especially, Skp is not redundant and will be more significant under stressed conditions. On the other hand, by using FRET technique, we studied the molecular interaction between SurA and outer membrane protein C（OmpC） from conformations to kinetics. Our results show that after binding to OmpC, SurA basically maintains its structure but somewhat expanded, in which the distance between the N and P1 domains is most stretched, and OmpC behaves like an extended random coil in the SurA-OmpC complex. Based on our conformational and kinetic information and previous works, we propose that OMPs anchors on the crevice in SurA’s core module first, then is wrapped around SurA, and finally one of its terminals settles down on the P2 *** manner of interaction may be essential for SurA to convey OMPs to BAM system for the folding and assembling.

关键词： Outer membrane proteins Chaperone smFRET FCS

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Co13O8—metalloxocubes:a new class of perovskite-like neutral clusters with cubic aromaticity

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National Science Review 2021年第1期8卷 89-97页

作者： lijun geng Mouyi Weng Cong-Qiao Xu Hanyu Zhang Chaonan Cui Haiming Wu Xin Chen Mingyu Hu Hai lin Zhen-Dong Sun Xi Wang Han-Shi Hu Jun li Jiaxin Zheng Zhixun Luo Feng Pan Jiannian Yao Beijing National laboratory for Molecular Sciences (BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences School of Physics Shandong University School of Advanced Materials Peking University Shenzhen Graduate School Department of chemistry Southern University of Science and Technology University of Chinese Academy of Sciences School of Physics and Electrical Engineering Kashi University College of Science Beijing Jiaotong University Department of chemistry and key laboratory of Organic Optoelectronics and Molecular Engineering of Ministry of Education Tsinghua University

Exploring stable clusters to understand structural evolution from atoms to macroscopic matter and to construct new materials is interesting yet challenging in chemistry. Utilizing our newly developed deep-ultraviolet laser ionization mass spectrometry technique, here we observe the reactions of neutral cobalt clusters with oxygen and find a very stable cluster species of Co13O8that dominates the mass distribution in the presence of a large flow rate of oxygen gas. The results of global-minimum structural search reveal a unique cubic structure and distinctive stability of the neutral Co13O8cluster that forms a new class of metal oxides that we named as ‘metalloxocubes’. Thermodynamics and kinetics calculations illustrate the structural evolution from icosahedral Co13to the metalloxocube Co13O8with decreased energy, enhanced stability and aromaticity. This class of neutral oxygen-passivated metal clusters may be an ideal candidate for genetic materials because of the cubic nature of the building blocks and the stability due to cubic aromaticity.

关键词： metalloxocube oxygen-passivated metal cluster cubic aromaticity cluster materials magnetic property

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镁铝复合氧化物负载铜催化剂上甘油选择性氢解合成丙二醇

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化学学报 2012年第18期70卷 1897-1903页

作者：王帅李洋刘海超北京分子科学国家实验室、分子动态与稳态结构国家重点实验室、北京大学化学与分子工程学院、绿色化学研究中心北京100871

我们通过乙醇溶液浸渍法合成出了具有高分散度金属Cu的Cu/MgO-Al2O3(Mg/Al原子比=1/1,3/1,4/1)、Cu/MgO和Cu/Al2O3等催化剂.在200℃,6.0 MPa H2和二氧六环溶剂中,这些催化剂高选择性地将甘油氢解为1,2-丙二醇(选择性>90%),而单位表面Cu... 详细信息

我们通过乙醇溶液浸渍法合成出了具有高分散度金属Cu的Cu/MgO-Al2O3(Mg/Al原子比=1/1,3/1,4/1)、Cu/MgO和Cu/Al2O3等催化剂.在200℃,6.0 MPa H2和二氧六环溶剂中,这些催化剂高选择性地将甘油氢解为1,2-丙二醇(选择性>90%),而单位表面Cu原子的甘油转化速率则随催化剂表面碱中心与Cu原子比例的提高而增大.N2O化学吸附-H2程序升温还原实验表明Cu粒子的本征氢解能力不随其负载量以及载体中的Mg/Al原子比发生明显改变,加之碱性MgO-Al2O3载体本身不催化甘油的转化,我们推测在甘油氢解反应中金属Cu粒子与载体界面处的碱中心辅助Cu粒子活化甘油分子的α位C—H键,从而加速甘油脱氢为甘油醛步骤以及甘油氢解反应的进行.CO2程序升温脱附实验以及对甘油氢解反应中Cu/MgO-Al2O3催化剂稳定性的考察结果暗示在甘油氢解反应中起主要作用的碱中心是载体表面上与Mg2+键连的羟基基团(即B碱OH-).这些对甘油氢解反应中金属中心与碱性中心协同作用的认识对进一步理性设计高效的甘油或其它多元醇分子氢解催化剂具有重要指导意义.

关键词：甘油选择性氢解丙二醇 Cu/MgO-Al2O3 载体效应

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An accurate,high-speed,portable bifunctional electrical detector for COVID-19

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Science China Materials 2021年第3期64卷 739-747页

作者： Guojun Ke Dingkai Su Yu li Yu Zhao Honggang Wang Wanjian liu Man li Zhiting Yang Fang Xiao Yao Yuan Fei Huang Fanyang Mo Peng Wang Xuefeng Guo Institute of Polymer Optoelectronic Materials and Devices State Key Laboratory of Luminescent Materials and DevicesSouth China University of TechnologyGuangzhou510640China Beijing National laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China Department of Energy and Resources Engineering College of EngineeringPeking UniversityBeijing100871China Qingdao Shuojing Biological Technology Co. Ltd.Qingdao266112China Department of Pathology Beijing Ditan Hospital Capital Medical UniversityBeijing100015China Institute of Digital Economy Industry Hangzhou310015China Beijing Sylincom Technology Co. Ltd.Beijing100081China

Coronavirus disease 2.19(COVID-19),caused by SARS-CoV-2,has rapidly spread and caused a severe global *** no specific drugs are available for COVID-19 and few vaccines are available for SARS-CoV-2,accurate and rapid diagnosis of COVID-19 has been the most crucial measure to control this ***,we developed a portable bifunctional electrical detector based on graphene fieldeffect transistors for SARS-CoV-2 through either nucleic acid hybridization or antigen-antibody protein interaction,with ultra-low limits of detection of~0.1 and~1 fg mL^(−1) in phosphate buffer saline,*** validated our method by assessment of RNA extracts from the oropharyngeal swabs of ten COVID-19 patients and eight healthy subjects,and the IgM/IgG antibodies from serum specimens of six COVID-19 patients and three healthy *** we show that the diagnostic results are in excellent agreement with the findings of polymerase chain reaction-based optical methods;they also exhibit rapid detection speed(~10 min for nucleic acid detection and~5 min for immunoassay).Therefore,our assay provides an efficient,accurate tool for high-throughput point-of-care testing.

关键词： COVID-19 biosensor nucleic acid detection immunoassay point-of-care testing

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