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Electrochemical reconstruction: a new perspective on Sn metal-organic complex microbelts as robust anode for lithium storage

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Rare metals 2024年第1期43卷 76-86页

作者： Jin-Ke Shen Nai-Teng Wu Li-Yuan Wang Gang Jiang Dong-Lei Guo Jin Li Gui-Long Liu Hong-Yu Mi Huan Pang Xian-Ming Liu Key Laboratory of Function-oriented Porous Materials of Henan Province College of Chemistry and Chemical EngineeringLuoyang Normal UniversityLuoyang 471934China State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources School of Chemical Engineering and TechnologyXinjiang UniversityUrumqi 830046China School of Chemistry and Chemical Engineering Institute for Innovative Materials and EnergyYangzhou UniversityYangzhou 225009JiangsuChina

Tin-based materials with high theoretical capacity and suitable working voltage are ideal anode materials for lithium-ion batteries(LIBs). However, to overcome their shortcomings(volume expansion and inferior stability), the preparation processes are usually complicated and expensive. Herein, a tin-based metal-organic complex(tin 1,2-benzenedicarboxylic acid, Sn-BDC)with one-dimensional microbelt morphology is synthesized by a facile, rapid and low-cost co-precipitation method, and served as anode material for LIBs without any post-treatment. Sn-BDC exhibits a high reversible capacity with609/440 m Ah·g^(-1) at 50/2000 m A·g^(-1), and robust cycling stability of 856 m Ah·g^(-1) after 200 cycles at 200 m A·g^(-1),which are obviously superior to that of the Sn Ox/C counterparts. Moreover, an electrochemical reconstruction perspective on the lithium storage mechanism of Sn-BDC is proposed by systematic ex-situ characterizations. The reconstructed SnO_(2) replaces Sn-BDC and becomes the active material in the subsequent cycles. As the by-product of the lithiation reaction, the formed Li-based metal-organic complex(Li-BDC, wrapped around the reconstructed SnO_(2)) plays an important role in alleviating volume expansion and accelerating the charge transfer kinetics.This work is beneficial to design and construct the new electrode materials based on the electrochemical reconstruction for advanced LIBs.

关键词： Electrochemical reconstruction metal-organic complex Anode Lithium storage mechanism Lithium-ion batteries

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A bifunctional POM-based Cu-viologen complex with mixed octamolybdate clusters for rapid oxidation desulfurization and effective photogeneration of hydrogen

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Rare metals 2024年第1期43卷 236-246页

作者： Lin Yang Zhong Zhang Chao-Nan Zhang Xiu-Li Wang College of Chemistry and Materials Engineering Bohai UniversityJinzhou 121013China Professional Technology Innovation Center of Liaoning Province for Conversion Materials of Solar Cell Bohai UniversityJinzhou 121013China

The design and synthesis of catalysts for the oxidation desulfurization and production of hydrogen are extremely important for solving environmental pollution and energy shortage.Herein,a novel bifunctional [α-Mo_(8)O_(26)]^(4-)/[β-Mo_(8)O_(26)]^(4-)-based Cu-viologen complex H_(4)[Cu_(2)~ⅠCl_(2)(Hbcbpy)_(4)] [α-Mo_(8)O_(26)] [β-Mo8O_(26)]·H_(2)O(BHU-2,Hbcbpy=1-(4-carboxybenzyl)-4,4'-bipyridinium) was synthesized and characterized by single-crystal X-ray diffraction(XRD),infrared radiation spectra,powder X-ray diffraction(PXRD) and X-ray photoelectron spectroscopy(XPS) spectra.The structural characteristic of BHU-2 is the presence of two types of octamolybdate clusters [α-Mo_(8)O_(26)]^(4-)/[β-Mo_(8)O_(26)]^(4-)and a new binuclear Cu~Ⅰ-Hbcbpy complex linked by Cl-bridges[Cu_(2)ⅠCl_(2)(Hbcbpy)_(4)]^(4+).BHU-2 as a heterogeneous catalyst exhibits excellent activities to the oxidation desulfurization and photocatalytic hydrogen production.At room temperature,BHU-2 can catalyze 96% conversion of methyl phenyl sulfide with 98% selectivity,and the process obeys the pseudo-first-order reaction kinetic with the half-life of9.6 min.The notorious 2-chloroethyl ethyl sulfide can achieve 99% conversion with 98% selectivity within only1 min at the presence of BHU-2,and the turnover frequency(TOF) is up to 7400 h^(-1).BHU-2 also exhibits high catalytic activity for the oxidation of other aromatic and aliphatic thioethers within short time at room temperature.Furthermore,BHU-2 shows a high catalytic activity for visible-light-driven hydrogen evolution with an H_(2) evolution rate of 1677.85 μmol·g^(-1)·h^(-1) within 10 h.Moreover,the catalytic activities do not decrease evidently after three cycles,revealing the prominent structural stability and recyclability.

关键词： Polyoxometalate metal-organic complex Viologen Oxidation desulfurization Photocatalytic hydrogen production

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Altering elastic-plastic mechanical response of a series of isostructural metal-organic complex crystals

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Science China Chemistry 2022年第4期65卷 710-718页

作者： Zheng Tang Xiao-Peng Sun Shu-Dong Wang Xue-Yang Ji Yun Li Zi-Shuo Yao Jun Tao Key Laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Henan Key Laboratory of Polyoxometalate Chemistry College of Chemistry and Chemical EngineeringHenan UniversityKaifeng 475004China

The mechanically compliant single crystals have attracted massive attention.However,the related reports on the single crystals composed of metal-organic complexes remain scarce.In this study,we synthesized a series of isostructural single crystals of Zn^(Ⅱ) complexes that manifest mechanical bending in response to external stress.In these crystals,the mechanical responses can be shifted between elastic bending and plastic bending by the control of the intermolecular interactions through a rational structural modification in the substituent group of pyridine ligands.As the molecular reorientation corresponding to ligand variation elongates the interfacial distance between molecular slip planes,and the structural disorder of ligands disperses the interplanar intermolecular interactions,the shift from elastic bending to plastic bending of the metal-organic complex-based single crystal was realized.The different mechanical responses of single crystals were comprehensively investigated both experimentally and theoretically.

关键词： mechanical property flexible crystals crystal engineering metal-organic complex intermolecular interaction

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Interwoven nickel(II)-dimethylglyoxime nanowires in 3D nickel foam for dendrite-free lithium deposition

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Chinese Chemical Letters 2022年第4期33卷 2165-2170页

作者： Tianyi Zhou Yanlu Mu Jianyang Wu Bing Zhong Chengkai Yang Qian Wang Wen Liu Henghui Zhou Peng Jiang CAS Key Laboratory of Standardization and Measurement for Nanotechnology CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China College of Chemistry and Molecular Engineering Peking UniversityBeijing 100871China University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Chemical Resource Engineering College of ChemistryBeijing Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China College of Materials Science and Engineering Fuzhou UniversityFuzhou 350108China Institute of Energy Innovation College of Materials Science and EngineeringTaiyuan University of TechnologyTaiyuan 030024China

metal skeletons,such as Nickel Foam(NF) has attracted worldwide interests as stable host for lithium metal anode because of its high stability,large specific surface area and high conductivity.However,most metal skeletons have lithophobic surface and uneven current distribution that result in sporadic lithium nucleation and uncontrolled dendrites growth.Herein,we describe a sequential immersing strategy to generate interwoven Nickel(Ⅱ)-dimethylglyoxime(Ni-DMG) nanowires at NF to obtain composite skeleton(NDNF),which can be used as an stable host for Li metal storage.The Ni-DMG has proved effective to realize uniform lithium nucleation and dendrite-free lithium deposition.Combing with the three dimensional(3 D) hierarchical porous structure,the composite host shows a significantly improved coulombic efficiency(CE) than pristine commercial nickel foam.Moreover,the corresponding Li‖Li symmetrical cells can run more than 700 h with low voltage hysteresis 22 mV at 1.0 mA/cm^(2),and Li@NDNF‖LiFePO;full-cell exhibits a high capacity retention of 82.03% at 1.0 C during 630 cycles.These results proved the effectiveness of metal-organic complexes in governing Li metal growth and can be employed as a new strategy for dendrite-free Li metal anode and safe Li metal batteries(LMBs).

关键词： Nickel(II)-dimethylglyoxime Nickel foam metal-organic complex Uniform nucleation Dendrite-free

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