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Two-dimensional polymer nanosheets for efficient energy storage and conversion

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Nano Research 2021年第6期14卷 2023-2036页

作者： Yumei Ren Chengbing Yu Zhonghui Chen yuxi xu School of Materials Science and Engineering Shanghai UniversityShanghai201800China School of Materials Science and Engineering Zhengzhou University of AeronauticsZhengzhou450046China School of Engineering Westlake UniversityHangzhou310024China Key Lab for Special Functional Materials of Ministry of Education School of Materials Science and EngineeringHenan UniversityKaifeng475004China

As a promising graphene analogue,two-dimensional(2D)polymer nanosheets with unique 2D features,diversified topological structures and as well as tunable electronic properties,have received extensive attention in recent *** in this review,we summarized the recent research progress in the preparation methods of 2D polymer nanosheets,mainly including interfacial polymerization and solution *** also discussed the recent research advancements of 2D polymer nanosheets in the fields of energy storage and conversion applications,such as batteries,supercapacitors,electrocatalysis and ***,on the basis of their current development,we put forward the existing challenges and some personal perspectives.

关键词： two-dimensional(2D)polymer nanosheets 2D polymerization batteries supercapacitors photo(electro)catalysis

Covalent organic framework-based solid-state electrolytes for advanced batteries

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Science China Chemistry 2024年第12期67卷 4037-4062页

作者： Desheng Feng Zhen Qin Yumei Ren yuxi xu School of Materials Science and Engineering Zhengzhou University of AeronauticsZhengzhou 450046China School of Engineering Westlake UniversityHangzhou 310024China

The emergence of solid-state batteries(SSBs)has generated significant interest in the field of energy storage,primarily due to their advantages such as high safety,high energy density and long *** state electrolytes(SSEs)play a crucial role in SSBs,which not only affects the ion transport efficiency,but also relates to the overall performance and stability of the *** recent years,SSEs based on covalent organic frameworks(COFs)have become a research focus in the battery field because of their unique structural characteristics and excellent *** review aims to provide an overview of the application and latest progress of COF-based SSEs in the field of advanced ***,the structural features of COFs and their advantages as SSEs are briefly introduced,followed by a summary of the types of COF-based SSEs(including neutral COF-based SSEs and ionic COF-based SSEs).The latest research progress in lithium ion batteries(LIBs),lithium metal batteries(LMBs),proton exchange membrane fuel cells(PEMFCs)and other advanced batteries recently is also ***,we summarize and outlook the current research status,the challenges faced in practical application,the future research directions and application prospects of COF-based SSEs.

关键词： covalent organic framework solid-state electrolytes advanced batteries

Highly crystalline vinylene-linked covalent organic frameworks enhanced solid polycarbonate electrolyte for dendrite-free solid lithium metal batteries

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Nano Research 2022年第9期15卷 8083-8090页

作者： Kaige Zhang Chaoqun Niu Chengbing Yu Li Zhang yuxi xu School of Materials and Engineering Zhengzhou UniversityZhengzhou 450001China School of Engineering Westlake UniversityHangzhou 310024China School of Materials Science and Engineering Shanghai UniversityShanghai 201800China

The development of solid-state electrolytes(SSEs)with high ionic conductivity,outstanding electrochemical window,and promising mechanical strength is a key factor in realizing the commercialization of high energy density solid-state lithium metal batteries(LMBs).Covalent organic frameworks(COFs)are a functional crystalline material with highly customizable molecular networks and one-dimensional channel structures,thus showing great potential applications in ***,we design flexible COF-poly(vinyl ethylene carbonate)(PVEC)(abbreviated as COF-PVEC)composite electrolyte films with excellent ionic conductivity and high mechanical strength,enabling dendrite-free and long-term running solid-state *** to the lithiumphilic triazine and carbon–carbon double bonds groups in the COF skeleton,the obtained flexible COF-PVEC shows high ionic conductivity up to 1.11×10^(−4)S·cm^(−1)at 40℃,and enlarged electrochemical window up to 4.6 V(***^(+)/Li)compared with pure PVEC *** the same time,the lithium dendrites are efficiently inhibited after discharge–charging cycles,due to the improved Young’s modulus(150 MPa)and ordered channels of *** the various features of COF-PVEC,we assembled a solid-state full battery with LiFePO4 cathode,which showed superior rate capacity(151.8,146.2,139.2,128.1,113.7,and 100.8 mAh·g^(−1)at 0.1,0.2,0.5,1,1.5,and 2 C,respectively)and excellent long-term cycling stability(over 400 cycles at 1 C).We believe that the COF-based composite electrolyte can become one of the most promising high-performance SSEs for solid-state LMBs.

关键词： solid-state electrolytes covalent organic frameworks lithium dendrites solid-state lithium metal batteries

Covalent Triazine Framework Nanosheets:Synthesis and Energy Conversion and Storage

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Chinese Journal of Chemistry 2024年第3期42卷 301-316页

作者： Zhao Liu Congxu Wang Wenjing Yuan yuxi xu School of Materials Science & Engineering Hebei University of TechnologyTianjin300130 China School of Engineering Westlake UniversityHangzhouZhejiang310024 China

Covalent triazine framework nanosheets (CTF NSs),an emerging class of two-dimensional nanomaterials,have received great attention due to their abundant active sites,permanent porosity,molecular structural diversity,superior chemical/thermal stability,and short charge diffusion path,enabling technological breakthroughs in a myriad of applications. The forefront developments and applications of CTF NSs as photocatalysts and electrochemical electrodes have conferred superior performance and made great impact in the field of energy and advanced catalysis. This forward-looking review aims to summarize the research trends,synthesis,properties of CTF NSs and their CTF counterpart,and highlight their progress in applications with respect to energy storage and conversion devices. Finally,the current challenges and future perspectives for CTF NSs are also presented.

关键词： Covalent triazine framework Nanosheets Photocatalysis Energy storage Charge transfer

Rational synthesis of carbon shell coated polyaniline/ MoS2 monolayer composites for high-performance supercapacitors

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Nano Research 2016年第4期9卷 951-962页

作者： Chao Yang Zhongxin Chen Imran Shakir yuxi xu Hongbin Lu State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science Collaborative Innovation Center of Polymers and Polymer Composite Materials Fudan University Shanghai 200433 China Sustainable Energy Technologies (SET) center College of Engineering King Saud University PO-BOX 800 Riyadh 11421 Kingdom of Saudi Arabia

Conducting polymers generally show high specific capacitance but suffer from poor rate capability and rapid capacitance decary which greatly limits their practical applications in supercapacitor electrodes. To this end, many studies have focused on improving the overall capacitive performance by synthesizing nanostructured conducting polymers or by depositing a range of coatings to increase the active surface area exposed to the electrolyte and enhance the charge transport efficiency and structural stability. Despite this, simultaneously achieving high specific capacitance, good rate performance, and long cycle life remains a considerable challenge. Among the various two-dimensional （2D） layered materials, octahedral （1T） phase molybdenum disulfide （MoS2） nano- sheets have high electrical conductivity, large specific surface areas, and unique surface chemical characteristics, making them an interesting substrate for the controlled growth of nanostructured conducting polymers. This paper reports the rational synthesis of carbon shell-coated polyaniline （PANI） grown on 1T MoS2 monolayers （MoS2/PANI@C）. The composite electrode comprised of MoS2/ PANI@C with a -3 nm carbon shell exhibited a remarkable specific capacitance of up to 678 F-g-1 （1 mV.s-1）, superior capacity retention of 80% after 10,000 cycles and good rate performance （81% at 10 mV.s-1） due to the multiple synergic effects between the PANI nanostructure and 1T MoS2 substrates as well as protection by the uniform thin carbon shell. These properties are comparable to the best overall capacitive performance achieved for conducting polymers-based supercapacitor electrodes reported thus far.

关键词： supercapadtor polyaniline molybdenum disulfide carbon shell cycle stability

Interface tuning of Cu+/CuO by zirconia for dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO2 catalyst

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Journal of Energy Chemistry 2020年第10期29卷 248-256页

作者： Yujun Zhao Huanhuan Zhang yuxi xu Shengnian Wang Yan xu Shengping Wang Xinbin Ma Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Center of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Chemical Engineering Institute for Micromanufacturing.Louisiana Tech UniversityRustonLA 71272USA

An efficient ZrO2-doped Cu/SiO2 catalyst was fabricated through hydrolysis precipitation method(HP)and used to produce ethylene glycol(EG)through dimethyl oxalate(DMO)*** states for zirconia on copper catalyst and roles in DMO hydrogenation were investigated through various characterization tools,including N2 physical adsorption,XRD,H2-TPR,Methyl glycolate-TPD-MS,XPS,XAES as *** with common ammonia evaporation and co-precipitation methods used in catalyst preparation,this HP method is found to effectively suppress the agglomeration and further size growth of copper nanoparticles by enhancing the interactions between copper and zirconia *** importantly,uniform distribution of ZrO2 dopant is achieved due to the pseudo-homogeneous reactions in the mixing step of catalyst preparation.A proper amount of zirconium dopant helps achieve the desirable proportion of Cu+/(Cu++CuO)for surface copper species,especially promotes the production of Cu+species originated from Cu-ZrO2 species at the interface of copper and zirconia *** comparison with Cu+species formed from copper phyllosilicates reduction,the Cu+sites derived from Cu-ZrO2 species show higher adsorption ability of MG,an important intermediate species in ethylene glycol *** adsorbed MG molecules further react with atomic hydrogen shifted from adjacent metallic copper surface,leading to a higher catalytic *** the EG production via DMO hydrogenation,the turnover frequency(TOF)normalized by CuO species on CuZr/SiO2 catalyst is 1.8 times than that of traditional Cu/SiO2 *** to the enhanced synergy effect between Cu+and Cuo active sites,a lower activation energy of ester hydrogenation on this ZrO2-doped Cu/SiO2 catalyst is believed to be responsible for the significant improvement.

关键词： Copper Zirconia Hydrogenation Ethylene glycol

Coupled biodegradation of p-nitrophenol and p-aminophenol in bioelectrochemical system:Mechanism and microbial functional diversity

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Journal of Environmental Sciences 2021年第10期33卷 134-144页

作者： Jianjun Luo yuxi xu Jing Wang Libin Zhang Xinbai Jiang Jinyou Shen Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological EngineeringNanjing University of Science and TechnologyNanjing 210094China

Biodegradation mechanisms and microbial functional diversity during coupled pnitrophenol(PNP)and p-aminophenol(PAP)degradation were studied in a bioelectrochemical *** in the biocathode and PAP in the bioanode were almost completely removed within 28 hr and 68 hr *** degradation followed the steps including hydrating hydroxyalkylation,dehydrogenating carbonylation,and hydrolating ring cleavage,*** analysis based on the KEGG and egg NOG database annotations revealed the microbial composition and functional genes/enzymes related to phenol degradation in the *** predominant bacteria genera were Lautropia,Pandoraea,Thiobacillus,Ignavibacterium,Truepera and *** recognized biodegradation genes/enzymes related to pollutant degradation were as follows:pmo,hbd,&ppo for phenol degradation,nzba,amie,&badh for aromatic degradation,and CYP&p450 for xenobiotics degradation,*** co-occurrence of ARGs(antibiotic resistant genes),such as ade F,Mex J,Erm F,PDC-93 and Escherichiacolimdf A,etc.,were annotated in CARD database during the biodegradation *** Proteobacteria&Actinobacteria phylum was the primary host of both the biodegradation genes&ARGs in this *** microbial functional diversity ensured the effective biodegradation of the phenol pollutants in the bioelectrochemical system.

关键词： Phenols biodegradation Functional diversity Functional gene Metagenome

Recent progress in COF-based electrode materials for rechargeable metal-ion batteries

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Nano Research 2023年第5期16卷 6753-6770页

作者： Shunhang Wei Jiwei Wang Yuzhao Li Zebo Fang Lei Wang yuxi xu Zhejiang Engineering Research Center of MEMS Shaoxing UniversityShaoxing 312000China School of Engineering Westlake UniversityHangzhou 310024China School of Mechatronics Engineering and Automation Foshan UniversityFoshan 528225China Department of Chemistry Binghamton UniversityBinghamtonNew York 13902USA China Electronics Corporation Beijing 100086China

Covalent organic frameworks(COFs)have emerged as promising electrode materials for rechargeable metal-ion batteries and have gained much attention in recent years due to their high specific surface area,inherent porosity,tunable molecular structure,robust framework,abundant active ***,compared with inorganic materials and small organic molecules,COFs have the advantages of multi-electron transfer,short pathways,high cycling *** great progress on COF-based electrodes has been made,the corresponding electrochemical performance is still far from satisfactory for practical *** this review,we first summarize the fundamental background of COFs,including the species of COFs(different active covalent bonds)and typical synthesis methods of ***,the key challenges and the latest research progress of COF-based cathodes and anodes for metal-ion batteries are reviewed,including Li-ion batteries,Na-ion batteries,K-ion batteries,Zn-ion batteries,et ***,the effective strategies to enhance electrochemical performance of COF-based electrodes are ***,this review also covers the typical superiorities of COFs used in energy devices,as well as providing some perspectives and outlooks in this *** hope this review can provide fundamental guidance for the development of COFbased electrodes for metal-ion batteries in the further research.

关键词： covalent organic frameworks metal-ion batteries electrochemical performance synthetic methods structure–property relationship

Monomer-dependent synthesis of secondary amine-linked triazine-based two-dimensional polymers nanosheets

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Science China Chemistry 2020年第7期63卷 966-972页

作者： Ranran Zhao Chaoqun Niu Mohamed FAly Aboud Imran Shakir Chengbing Yu yuxi xu School of Materials Science and Engineering Shanghai UniversityShanghai 201800China School of Engineering Westlake UniversityHangzhou 310024China Sustainable Energy Technologies Center College of EngineeringKing Saud UniversityRiyadh 11421Kingdom of Saudi Arabia

Expanding the structural diversity of crystalline two-dimensional polymers(2DPs) is highly desired but remains a considerable challenge. Herein we report the first synthesis of novel crystalline secondary amine-linked triazine-based 2DPs(SAT-2DPs) by using benzidine or 4, 4′′-diamino-p-terphenyl and cyanuric chloride under solvothermal conditions. We find the structures of diamine-based monomers play a crucial role in deciding whether the synthesized material is crystalline 2DPs nanosheets or amorphous nanoparticles, which is unexpected and provides an important understanding of the 2D polymerization *** obtained SAT-2DPs not only show a lateral size of micrometers and an ultrathin thickness of a few nanometers, but also demonstrate high crystallinity with a unique ABC stacking configuration, excellent solvent dispersibility and superior thermal stability. In addition, the resultant SAT-2DPs are used to guide uniform lithium-ion deposition due to their abundant nitrogen atoms and ordered open channels. The assembled asymmetric coin cells(Li|Cu) with SAT-2DPs realize the average coulombic efficient up to 99.3% during discharge-charge cycles. This work provides valuable insights into the synthesis of new 2DPs for various applications.

关键词： nanosheets,two-dimensional polymers crystalline solution synthesis monomer-dependent