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Nano Research 2024年第5期17卷 4006-4015页

作者： Xiaowei He Tianshuai Wang Lidong Tian Qiuyu Zhang School of Chemistry and Chemical Engineering Xi’an Key Laboratory of Functional Organic Porous MaterialsKey Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information TechnologyNorthwestern Polytechnical UniversityXi’an 710072China Chongqing Science and Technology Innovation Center of Northwestern Polytechnical University Chongqing 401135China College of materials Science and Engineering Xi’an University Science and TechnologyXi’an 710054China

Heterostructure engineering by coupling different nanocrystals has received extensive attention because it can enhance the reaction kinetics of the anode of sodium-ion batteries(SIBs).However,constructing high-quality heterostructure anode materials through green and environmentally friendly methods remains a challenge.Herein,we have proposed a simple one-step method by recycling the electronic waste metal materials to synthesize the Cu_(1.94)S/ZnS heterostructure materials.Combined with the experimental analysis and first principle calculations,we find that the synergistic effect of different components in heterostructure structures can significantly enhance the reversible capacity and rate performance of anode materials.Based on the constructed Cu_(1.94)S/ZnS anode,we obtain a superior reversible capacity of 440 mAh·g^(-1) at 100 mA·g^(-1) and 335 mAh·g^(-1) after 3000 cycles at 2000 mA·g^(-1).Our work sheds new light on designing high-rate and capacity anodes for SIBs through the greenness synthesis method.

关键词： sodium-ion batteries heterostructure reversible capacity environmentally synthesis process

Construction of biomimetic proton transport channels in metal-organic framework

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Chinese Chemical Letters 2024年第3期35卷 513-517页

作者： Xiao-Min Li Junchao Jia Danting Yang Jiali Jin Junkuo Gao School of materials Science and Engineering Institute of Functional Porous MaterialsZhejiang Sci-Tech UniversityHangzhou 310018China Zhejiang key laboratory of Pathophysiology School of Public HealthSchool of MedicineNingbo UniversityNingbo 315211China

Construction of proton transport channels in metal-organic frameworks(MOFs)with simple synthesis processes,high proton conductivities and good performance stabilities has been of great interest for proton exchange membrane fuel cell(PEMFC).Herein,we mimic the proton transport behavior of amino acid residues in bacteriorhodopsin,select UiO-66-COOH as the host,glycine and aspartic acid as the functional guest molecules,and then functionalize the MOF framework with amino acids to obtain biomimetic proton transport channels.This strategy endows UiO-66-COOH-Asp a high proton conductivity of 1.19×10^(-2)S/cm at 70℃and 98%RH,excellent cycle stability of performances and performance durability,which can be comparable to the reported MOFs-based proton conductors.Moreover,the proton conduction mechanism in UiO-66-COOH-Asp is elaborated in detail due to its visual structure,which is also one of the advantages of adopting MOFs as research platform,making it possible to optimize the structure-activity relationship of advanced materials.Notably,this strategy has clear objectives and simple synthesis,which has made certain contributions to both theoretical research and future industrial production of proton conductors.

关键词： MOF Amino acids Biomimetic proton transport channels Synergistic effect Proton conduction mechanism

MOF-derived Cu embedded into N-doped mesoporous carbon as a robust support of PdAu nanocatalysts for ethanol electrooxidation

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Rare Metals 2024年第3期43卷 1083-1094页

作者： Yu-Fu Huang Peng Wu Jun-Ping Tang Jian Yang Jing Li Shuai Chen Xue-Ling Zhao ChengChen Bin-Wei Zhang Yan-Yun Ma Wei-Heng Shi Dong-Hai Lin Shi-Gang Sun School of Energy and materials Shanghai Engineering Research Center of Advanced Thermal Functional MaterialsShanghai Key Laboratory of Engineering Materials Application and EvaluationShanghai Polytechnic UniversityShanghai201209China State key laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China School of Chemistry and Chemical Engineering Chongqing UniversityChongqing401331China Center of advanced Energy Technology and Electrochemistry Institute of Advanced Interdisciplinary StudiesChongqing UniversityChongqing400044China Institute of functional Nano&Soft materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou215123China Department of materials Science and Engineering Drexel UniversityPhiladelphiaPA19104USA

Metal-organic frameworks(MOFs)h ave attracted widespread attention due to their large surface area and porous structure.Rationally designing the nanostructures of MOFs to promote their application in ethanol electrooxidation is still a challenge.Here,a novel Cu-NCNs(Cu-nitrogen-doped carbon nanotubes)support was synthesized by pyrolysis of melamine(MEL)and Cu-ZIF-8 together,and then,Pd-Au nanoalloys were loaded by sodium borohydride reduction method to prepare PdAu@Cu-NCNs catalysts.The generating mesoporous carbon with high specific surface area and favorable electron and mass transport can be used as a potential excellent carrier for PdAu nanoparticles.In addition,the balance of catalyst composition and surface structure was tuned by controlling the content of Pd and Au.Thus,the best-performed Pd_(2)Au_(2)@Cu-NCN-1000-2(where 1000 means the carrier calcination temperature,and 2 means the calcination constant temperature time)catalyst exhibits better long-term stability and electrochemical activity for ethanol oxidation in alkaline media(4.80 A·mg^(-1)),which is 5.05 times higher than that of commercial Pd/C(0.95 A·mg^(-1)).Therefore,this work is beneficial to further promoting the application of MOFs in direct ethanol fuel cells(DEFCs)and can be used as inspiration for the design of more efficient catalyst support structures.

关键词： Metal-organic frameworks(MOFs) N-doped Mesoporous carbon PdAu Ethanol electrooxidation

Towards Ultrahigh Capacity and High Cycling Stability Lithium-Conducting Polymer Batteries by In Situ Construction of Nanostructured porous Cathodes

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CCS Chemistry 2024年第3期6卷 749-760页

作者： Junkai Yang Jixing Yang Yunhua Xu Yuesheng Li School of materials Science and Engineering Tianjin Key Laboratory of Composite and Functional MaterialsTianjin UniversityTianjin 300350

Conducting polymers(CPs)have long been studied as cathode materials for lithium-ion batteries,but the low doping level(maximum:30–50%or even lower)and poor cycling stability limit their applications.Herein,we have developed a method of nanoporeconfined in situ electropolymerization to prepare nanostructured polythiophene-type porous cathodes,achieving significantly improved doping availability and long cycle life.It was verified that the nanosized polymer formed in situ and loose porous structure are conducive to the doping reaction and maintain high electrochemical stability.The constructed thieno[3,2-b]thiophene(TtTP)/active carbon cathode delivers an ultrahigh reversible capacity of 309.2 mAh g^(−1)(doping level up to 80.9%)along with an ultrahigh energy density of 1252.3 Wh Kg^(−1),and an ultrahigh rate capability(172.4 mAh g^(−1) at 30 A g^(−1)),which far exceed all the CPs and even all the p-type organic cathode materials reported.Moreover,an excellent long cycle life of 2000 cycles at 5 A g^(−1) is also revealed,which is a new record for CPs-based cathode materials in nonaqueous lithium-ion batteries.Our method provides an effective strategy to improve the doping level and cycling stability of CP-based cathode materials.

关键词： organic cathode materials conducting polymers lithium-ion batteries porous carbon in situ electropolymerization

MOF-mediated synthesis of novel PtFeCoNiMn high-entropy nanoalloy as bifunctional oxygen electrocatalysts for zinc-air battery

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Nano Research 2024年第6期17卷 5288-5297页

作者： Mingkuan Xie Xin Xiao Duojie Wu Cheng Zhen Chunsheng Wu Wenjuan Wang Hao Nian Fayan Li Meng Danny Gu Qiang Xu Shenzhen key laboratory of Micro/Nano-porous functional materials(SKLPM) Shenzhen 518055China Department of Chemistry Southern University of Science and TechnologyShenzhen 518055China Department of materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055China SUSTech-Kyoto University advanced Energy materials Joint Innovation laboratory(SKAEM-JIL) Shenzhen 518055China key University laboratory of Highly Efficient Utilization of Solar Energy and Sustainable Development of Guangdong Southern University of Science and TechnologyShenzhen 518055China Eastern Institute for advanced Study Eastern Institute of TechnologyNingbo 315200China

High-entropy alloy(HEA)-based materials are expected to be promising oxygen electrocatalysts due to their exceptional properties.The electronic structure regulation of HEAs plays a pivotal role in enhancing their elctrocatalytic ability.Herein,PtFeCoNiMn nanoparticles(NPs)with subtle lattice distortions are constructed on metal-organic framework-derived nitrogen-doped carbon by an ultra-rapid Joule heating process.Thanks to the modulated electronic structure and the inherent cocktail effect of HEAs,the as-synthesized PtFeCoNiMn/NC exhibits superior bifunctional electrocatalytic performance with a positive half-wave potential of 0.863 V vs.reversible hydrogen electrode(RHE)for oxygen reduction reaction and a low overpotential of 357 mV at 10 mA·cm^(-2)for oxygen evolution reaction.The assembled quasi-solid-state zinc-air battery using PtFeCoNiMn/NC as air electrode shows a high peak power density of 192.16 mW·cm^(-2),low charge−discharge voltage gap,and excellent durability over 500 cycles at 5 mA·cm^(-2).This work demonstrates an effective route for rational design of bifunctional nanostructured HEA electrocatalysts with favorable electronic structures,and opens up a fascinating directions for energy storage and conversion,and beyond.

关键词： oxygen reduction reaction oxygen evolution reaction high-entropy nano-alloy zinc-air battery

Janus Quasi‑Solid Electrolyte Membranes with Asymmetric porous Structure for High‑Performance Lithium‑Metal Batteries

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Nano-Micro Letters 2024年第6期16卷 221-232页

作者： Zerui Chen Wei Zhao Qian Liu Yifei Xu Qinghe Wang Jinmin Lin Hao Bin Wu Institute for Composites Science Innovation(InCSI)and State key laboratory of Silicon and advanced Semiconductor materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China

Quasi-solid electrolytes(QSEs)based on nanoporous materials are promising candidates to construct high-performance Limetal batteries(LMBs).However,simultaneously boosting the ionic conductivity(σ)and lithium-ion transference number(t^(+)) of liquid electrolyte confined in porous matrix remains challenging.Herein,we report a novel Janus MOFLi/MSLi QSEs with asymmetric porous structure to inherit the benefits of both mesoporous and microporous hosts.This Janus QSE composed of mesoporous silica and microporous MOF exhibits a neat Li^(+) conductivity of 1.5.10^(–4)S cm^(−1) with t^(+) of 0.71.A partially de-solvated structure and preference distribution of Li^(+)near the Lewis base O atoms were depicted by MD simulations.Meanwhile,the nanoporous structure enabled efficient ion flux regulation,promoting the homogenous deposition of Li^(+).When incorporated in Li||Cu cells,the MOFLi/MSLi QSEs demonstrated a high Coulombic efficiency of 98.1%,surpassing that of liquid electrolytes(96.3%).Additionally,NCM 622||Li batteries equipped with MOFLi/MSLi QSEs exhibited promising rate performance and could operate stably for over 200 cycles at 1 C.These results highlight the potential of Janus MOFLi/MSLi QSEs as promising candidates for next-generation LMBs.

关键词： Metal-organic frameworks Mesoporous silicas Quasi-solid electrolytes Janus structure Lithium-metal battery

Complementary multicolor electrochromic devices with excellent stability based on porous tin oxide nanosheet scaffold

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Nano Research 2024年第4期17卷 3035-3042页

作者： Chenchen Bian Jinhui Wang Huanhuan Liu Yin Yan Ping Zhang Weilong Yang Sensen Jia Xiaodan Guo Guofa Cai key laboratory for Special functional materials of Ministry of Education National&Local Joint Engineering Research Center for High-Efficiency Display and Lighting TechnologySchool of Materials and Engineeringand Collaborative Innovation Center of Nano Functional Materials and ApplicationsHenan UniversityKaifeng 475004China

Electrochromic devices(ECDs)have been extensively investigated as promising candidates in broad cutting-edge applications,such as smart windows,electronic labels,adaptive camouflage,etc.However,they have suffered from either inadequate color variations or poor cycling stability for a long time.Herein,we developed a general strategy to boost the cyclic stability and enrich the color variations of ECDs by scrupulous design of the composition and nanostructure of electrodes,in which porous tin oxide(SnO_(2))nanosheets serve as the scaffold and typical metal oxides or conducting polymers as the active electrochromic materials.Various electrochromic composite materials,including polyaniline(PANI)@SnO_(2),V2O5@SnO_(2),and WO_(3)@SnO_(2) heterostructured nanoarrays were prepared by the facile wet-chemical method.These composite electrodes exhibit remarkable electrochromic performances,e.g.,superior cycling stability(more than 2000 cycles),rich color variations(more than 5 colors for PANI@SnO_(2)),and enlarged optical modulation.These excellent performances account for the heterogenous porous nanoarrays,which not only facilitate the intercalation/extraction of ions but also relieve the stress generated during the electrochemical process.In addition,diverse prototypes of complementary multicolor ECD with excellent cycling stability(over thousands of cycles)and rich color variations(8 colors)were realized for the first time.We believe that our work put forward a general strategy for developing high-quality multicolor complementary electrochromic devices.

关键词： electrochromism tin oxide metal oxide cycling stability multicolor complementary device

MIL-100(V) derived porous vanadium oxide/carbon microspheres with oxygen defects and intercalated water molecules as high-performance cathode for aqueous zinc ion battery

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Journal of Energy Chemistry 2024年第3期90卷 578-589,I0013页

作者： Yuexin Liu Jian Huang Xiaoyu Li Jiajia Li Jinhu Yang Kefeng Cai Shanghai key laboratory of Development and Application for Metal-functional materials Key Laboratory of Advanced Civil Engineering MaterialsMinistry of EducationSchool of Materials Science&EngineeringTongji UniversityShanghai 201804China State key laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 201800China Research Center for Translational Medicine East HospitalTongji University School of MedicineShanghai 200092China

The development of aqueous zinc ion battery cathode materials with high capacity and high magnification is still a challenge.Herein,porous vanadium oxide/carbon(p-VO_(x)@C,mainly VO_(2) with a small amount of V_(2)O_(3)) core/shell microspheres with oxygen vacancies are facilely fabricated by using a vanadium-based metal-organic framework(MIL-100(V)) as a sacrificial template.This unique structure can improve the conductivity of the VO_(x),accelerate electrolyte diffusion,and suppress structural collapse during circulation.Subsequently,H_(2)O molecules are introduced into the interlayer of VO_(x) through a highly efficient in-situ electrochemical activation process,facilitating the intercalation and diffusion of zinc ions.After the activation,an optimal sample exhibits a high specific capacity of 464.3 mA h g^(-1) at0.2 A g^(-1) and 395.2 mA h g^(-1) at 10 A g^(-1),indicating excellent rate performance.Moreover,the optimal sample maintains a capacity retention of about 89.3% after 2500 cycles at 10 A g^(-1).Density functional theory calculation demonstrates that the presence of oxygen vacancies and intercalated water molecules can significantly reduce the diffusion barrier for zinc ions.In addition,it is proved that the storage of zinc ions in the cathode is achieved by reversible intercalation/extraction during the charge and discharge process through various ex-situ analysis technologies.This work demonstrates that the p-VO_(x)@C has great potential for applications in aqueous ZIBs after electrochemical activation.

关键词： Metal-organic frameworks Vanadium oxide Carbon Zn-ion batteries Electrochemical activation

A high-sensitive and self-selective humanoid mechanoreceptor for spatiotemporal tactile stimuli cognition

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Nano Research 2024年第5期17卷 4400-4409页

作者： Shuxin Bi Xuan Zhao Fangfang Gao Xiaochen Xun Bin Zhao Liangxu Xu Tian Ouyang Qingliang Liao Yue Zhang Academy for advanced Interdisciplinary Science and Technology Beijing Advanced Innovation Center for Materials Genome EngineeringUniversity of Science and Technology(Beijing)Beijing 100083China key laboratory of advanced materials and Devices for Post-Moore Chips Ministry of EducationBeijing Key Laboratory for Advanced Energy Materials and TechnologiesSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China

The cognition of spatiotemporal tactile stimuli,including fine spatial stimuli and static/dynamic temporal stimuli,is paramount for intelligent robots to feel their surroundings and complete manipulation tasks.However,current tactile sensors have restrictions on simultaneously demonstrating high sensitivity and performing selective responses to static/dynamic stimuli,making it a challenge to effectively cognize spatiotemporal tactile stimuli.Here,we report a high-sensitive and self-selective humanoid mechanoreceptor(HMR)that can precisely respond to spatiotemporal tactile stimuli.The HMR with PDMS/chitosan@CNTs(PDMS:polydimethylsiloxane;CNT:carbon nanotube)graded microstructures and polyurethane hierarchical porous spacer exhibits high sensitivity of 3790.8 kPa^(-1).The HMR demonstrates self-selective responses to static and dynamic stimuli with mono signal through the hybrid of piezoresistive and triboelectric mechanisms.Consequently,it can respond to spatiotemporal tactile stimuli and generate distinguishable and multi-type characteristic signals.With the assistance of the convolutional neural network,multiple target objects can be easily identified with a high accuracy of 99.1%.This work shows great potential in object precise identification and dexterous manipulation,which is the basis of intelligent robots and natural human-machine interactions.

关键词： mechanoreceptors self-selective high-sensitive spatiotemporal tactile stimuli cognition sensors

Integration of urchin-like MnCo_(2)O_(4)@C core–shell nanowire arrays within porous copper current collector for superior performance Li-ion battery anodes

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Rare Metals 2024年第2期43卷 599-611页

作者： Xue-Ru Zhang Qiong Wu Yong Zhang Xi-Fei Li Ting Xie Yu-Cheng Wu Instrumental Analysis Center Hefei University of TechnologyHefei230009China key laboratory of advanced functional materials and Devices of Anhui Province Hefei230009China School of materials Science and Engineering Hefei University of TechnologyHefei230009China Institute of advanced Electrochemical Energy Xi’an University of TechnologyXi’an710048China

Spinel MnCo_(2)O_(4) is a promising energy storage candidate as anode materials in lithium-ion batteries owing to synergistic effects of two intrinsic solid-state redox couples.However,low conductivity,poor rate capacity and rapid capacity fading have seriously impaired its practical applications.To overcome the inferiorities,urchin-like MnCo_(2)O_(4)@C core–shell nanowire arrays have been fabricated directly within a porous copper current collector via a facile hydrothermal method followed by a chemical vapor deposition carbonization process.In a typical nanowire,the core is composed of interconnected MnCo_(2)O_(4)nanoparticles and the shell shows as a thin amorphous carbon layer.The integrated MnCo_(2)O_(4)@C/Cu structure could act as working anodes without using additives or polymer binders.While MnCo_(2)O_(4)@C/Cu possesses slightly longer Li-ion insertion/desertion pathway than that of MnCo_(2)O_(4)/Cu,the carbon shell could effectively prevent the pulverization of MnCo_(2)O_(4) and lower down charge transfer resistance and actively participate in Li-ion cycles.The rearrangement of carbon atoms during lithiation/delithiation cycling could inhibit the formation of passive solid electrolyte interphase films.As a result,the MnCo_(2)O_(4)@C/Cu electrode presents superior rate capacity(600 mAh·g^(−1) at 1 A·g^(−1)) and better stability(797 mAh·g^(−1) after 200 cycles at 100 mA·g^(−1)).The excellent reversible Li ion storage capacity,cycling stability and rate capacity endow MnCo_(2)O_(4)@C/Cu great potential as stable and high output integrated anode materials in Li-ion batteries.

关键词： MnCo_(2)O_(4)@C Urchin-like nanowire arrays Core-shell Integrated anode materials Lithium-ion batteries