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Emerging two-dimensional Mo-based materials for rechargeable metal-ion batteries:Advances and perspectives

Journal of Energy Chemistry 2024年第2期89卷 487-518,I0012页

作者： Qingqing Ruan Yuehua Qian Mengda Xue Lingyun Chen qichun zhang Department of Applied Chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China Department of Materials Science and Engineering City University of Hong Kong999077Hong KongChina

With the rapid development of rechargeable metal-ion batteries(MIBs)with safety,stability and high energy density,significant efforts have been devoted to exploring high-performance electrode materials.In recent years,two-dimensional(2D)molybdenum-based(Mo-based)materials have drawn considerable attention due to their exceptional characteristics,including low cost,unique crystal structure,high theoretical capacity and controllable chemical compositions.However,like other transition metal compounds,Mo-based materials are facing thorny challenges to overcome,such as slow electron/ion transfer kinetics and substantial volume changes during the charge and discharge processes.In this review,we summarize the recent progress in developing emerging 2D Mo-based electrode materials for MIBs,encompassing oxides,sulfides,selenides,carbides.After introducing the crystal structure and common synthesis methods,this review sheds light on the charge storage mechanism of several 2D Mo-based materials by various advanced characterization techniques.The latest achievements in utilizing 2D Mo-based materials as electrode materials for various MIBs(including lithium-ion batteries(LIBs),sodium-ion batteries(SIBs)and zinc-ion batteries(ZIBs))are discussed in detail.Afterwards,the modulation strategies for enhancing the electrochemical performance of 2D Mo-based materials are highlighted,focusing on heteroatom doping,vacancies creation,composite coupling engineering and nanostructure design.Finally,we present the existing challenges and future research directions for 2D Mo-based materials to realize high-performance energy storage systems.

关键词： Molybdenum-based materials Two-dimensional materials Lithium-ion batteries Sodium-ion batteries Zinc-ion batteries

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Highly stableβ‑ketoenamine‑based covalent organic frameworks(COFs):synthesis and optoelectrical applications

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Frontiers of Optoelectronics 2022年第3期15卷 97-138页

作者： Yaqin Li Maosong Liu Jinjun Wu Junbo Li Xianglin Yu qichun zhang Key Laboratory for Green Chemical Process of Ministry of Education School of Chemical Engineering and PharmacyWuhan Institute of TechnologyWuhan 430074China School of Chemistry and Environmental Engineering Wuhan Institute of TechnologyWuhan 430074China Department of Materials Science and Engineering City University of HongkongHong Kong SAR 999077China Center of Super-Diamond and Advanced Films(COSDAF) City University of HongkongHong Kong SAR 999077China

Covalent organic frameworks(COFs)are one class of porous materials with permanent porosity and regular channels,and have a covalent bond structure.Due to their interesting characteristics,COFs have exhibited diverse potential applications in many felds.However,some applications require the frameworks to possess high structural stability,excellent crystallinity,and suitable pore size.COFs based onβ-ketoenamine and imines are prepared through the irreversible enol-to-keto tautomerization.These materials have high crystallinity and exhibit high stability in boiling water,with strong resistance to acids and bases,resulting in various possible applications.In this review,we frst summarize the preparation methods for COFs based onβ-ketoenamine,in the form of powders,flms and foams.Then,the efects of diferent synthetic methods on the crystallinity and pore structure of COFs based onβ-ketoenamine are analyzed and compared.The relationship between structures and diferent applications including fuorescence sensors,energy storage,photocatalysis,electrocatalysis,batteries and proton conduction are carefully summarized.Finally,the potential applications,large-scale industrial preparation and challenges in the future are presented.

关键词： Covalent organic frameworks β-ketoenamine Sensors Energy storage Batteries Photocatalysis

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Organic quantum materials:A review

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SmartMat 2023年第4期4卷 10-36页

作者： Xin Wang qichun zhang Department of Materials Science and Engineering City University of Hong KongHong KongChina

Interests in organic quantum materials(OQMs)have been explosively growing in the field of condensed physics of matter due to their rich chemistry and unique quantum properties.They are strongly correlated systems and show novel electromagnetic performance such as high-temperature superconducting,quantum sensing,spin electronics,quantum dots,topological insulating,quantum Hall effects,spin liquids,qubits,and so forth,which exhibit promising prospects in information communication and thus facilitate the construction of a modern intelligent society.This article reviews recent developments in the research on the electromagnetic characteristics of OQMs.We mainly give an overview on the progress of superconductors and quantum spin liquids based on organic materials and describe their possible mechanisms.Numerous experimental findings exhibit new exciton interactions and provide insights into exotic electronic properties.Finally,their association and strategies for realizing multiple quantum states in one system are discussed.

关键词： organic quantum materials spin liquids superconductors

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Construction of a cement-rebar nanoarchitecture for a solution-processed and flexible film of a Bi_(2)Te_(3)/CNT hybrid toward low thermal conductivity and high thermoelectric performance

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Carbon Energy 2022年第1期4卷 115-128页

作者： Zhijun Chen Haicai Lv qichun zhang Hanfu Wang Guangming Chen College of Materials Science and Engineering Shenzhen UniversityShenzhenChina College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhenChina Department of Materials Science and Engineering City University of Hong KongHong KongChina Center of Super-Diamond and Advanced Films(COSDAF) City University of Hong KongHong KongChina National Center for Nanoscience and Technology BeijingChina

Solution processability and flexibility still remain major challenges for many thermoelectric(TE)materials,including bismuth telluride(Bi_(2)Te_(3)),a typical and commercially available TE material.Here,we report a new solutionprocessed method to prepare a flexible film of a Bi_(2)Te_(3)/single-walled carbon nanotube(SWCNT)hybrid,where the dissolved Bi_(2)Te_(3) ion precursors are mixed with dispersed SWCNTs in solution and recrystallized on the SWCNT surfaces to form a“cement-rebar”-like architecture.The hybrid film shows an n-type characteristic,with a stable Seebeck coefficient of^(−1)00.00±1.69μVK^(−1) in air.Furthermore,an extremely low in-plane thermal conductivity of∼0.33Wm^(−1) K^(−1) is achieved at 300 K,and the figure of merit(ZT)reaches 0.47±0.02.In addition,the TE performance is independent of mechanical bending.The unique“cement-rebar”-like architecture is believed to be responsible for the excellent TE performances and the high flexibility.The results provide a new avenue for the fabrication of solution-processable and flexible TE hybrid films and will speed up the applications of flexible electronics and energy conversion.

关键词： Bi_(2)Te_(3) carbon nanotube hybrid solution-processed thermoelectrics

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Coupling of sulfur and boron in carbonaceous material to strengthen persulfate activation for antibiotic degradation:Active sites,mechanism,and toxicity assessment

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Chinese Chemical Letters 2023年第5期34卷 292-301页

作者： Feng Ye Wei Sun Kangfeng Pang Wenchao Yang Mengjie Pu qichun zhang Research Center for Eco-environmental Engineering Dongguan University of TechnologyDongguan 523830China Guangling College and School of Horticulture and Plant Protection Yangzhou UniversityYangzhou 225009China College of Life and Environmental Science Wenzhou UniversityWenzhou 325035China Center of Super-Diamond and Advanced Films(COSDAF) City University of HongkongHong KongChina

Carbon-mediated persulfate advanced oxidation processes(PS-AOPs)are appealing in contaminant remediation.For the first time,S,B-co-doped carbon-based persulfate activators were synthesized through direct carbonization of sodium lignosulfonate and boric acid.By degrading sulfamethoxazole(SMX),CSB-750 obtained 98.7%removal and 81.4%mineralization within 30 min.In comparison with solo S or B doping,S and B co-doped carbon showed the coupling effect for enhanced catalysis.The rate constant(kobs)of 0.1679 min^(-1)was 22.38-and 279.83-fold higher than those of CS-750(0.0075 min^(-1))and CB-750(0.0006 min^(-1)),respectively.The degradation was efficient at strong acidic and weak basic conditions(pH 3-9).Substantial inhibition effect was presented at strong basic condition(pH 10.95)and in presence of CO_(3)^(2-).The CO_(3)^(2-)-caused inhibition was the combined result of the cooperation of pH and quenching O_(2)^(·-).Thiophene sulfur,BC_(3),BC_(2)O,and structural defects were identified as the active sites for PS activation.Radical and nonradical pathways were both involved in the CSB-750/PS/SMX system,where^(1)O_(2)dominated the degradation,SO_(4)^(·-),·OH and direct electron transfer played the subordinate role,and O_(2)^(·-)served as a precursor for the formation of partial^(1)O_(2).The toxicity of degradation system,the effect of real water matrix,and the reusability of carbocatalysts were comprehensively analyzed.Nine possible degradation pathways were proposed.This work focuses on the catalytic performance improvement through the coupling effect of S,B co-doping,and develops an advanced heteroatom doping system to fabricate carbonaceous persulfate activators.

关键词： S B-co-doped carbons Advanced oxidation process Nonradical pathway Coupling effect

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Seeing Is Believing:A Wavy N-Heteroarene with 20 Six-Membered Rings Linearly Annulated in a Row

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CCS Chemistry 2022年第11期4卷 3491-3496页

作者： Zhongbo zhang Zilong Wang Naoki Aratani Xiaozhang Zhu qichun zhang School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798 Division of Materials Science Nara Institute of Science and TechnologyIkomaNara 630-0192 Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 Department of Materials Science and Engineering Center of Super-Diamond and Advanced Films(COSDAF)City University of Hong KongHong Kong SAR 999077

Structurally well-defined arenes with higher numbers of linearly-fused six-member rings(n≥10)are important and highly desirable not only because of their experimental challenges but also due to their fundamental interests and the curiosity of their structure-property relationships.In this research,we successfully synthesized a novel large N-heteroarene(N20)with 20 linearly-fused six-membered rings,which is the longest N-heteroarene(4.7 nm)confirmed by single-crystal X-ray diffraction(SCXRD)analysis so far.The as-prepared arene displays a wave-like framework rather than a rigid plane.Moreover,N20 shows high molar absorptivity of 364,000 M^(−1) cm^(−1) with its fluorescence extended to the near-infrared region.

关键词： N-heteroarenes single-crystal structure linear annulation optical properties

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Covalent organic framework containing dual redox centers as an efficient anode in Li-ion batteries

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SmartMat 2022年第4期3卷 685-694页

作者： Yifan Tong Zhaopeng Sun Jiawen Wang Weiwei Huang qichun zhang School of Environmental and Chemical Engineering Yanshan UniversityQinhuangdaoChina Department of Materials Science and Engineering City University of Hong KongKowloonHong KongChina Center of Super-Diamond and Advanced Films(COSDAF) City University of Hong KongKowloonHong KongChina

Covalent organic frameworks(COFs)with periodic channels and tunable chemical structures have been widely considered as promising electrode materials in rechargeable batteries.However,the design and construction of high-performance COFs-based electrodes still face some challenges in the introduction of multiple efficient redox centers as well as the reduction of dead mass.To address these issues,a unique COF containing double active centers(C═N and N═N)is developed as an anode in rechargeable lithium-ion batteries(LIBs).The as-prepared COF displays excellent electrochemical performance due to its remarkable structural stability and the existence of many active groups.Meanwhile,its electrochemical performance is significantly better than that of the small molecule compound or the linear polymer with the same construction units.Even at a high current density of 5 A/g,the LIBs with COF electrodes remain at a high discharge capacity of 227 mAh/g after 2000 cycles.Moreover,the distinction in electrochemical performances of these three materials is further revealed by calculation.This study illustrates the importance of molecular structure design for improving the performance of organic electrodes.

关键词： anodes covalent organic frameworks dual active sites molecular structure design

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A robust graphene oxide memristor enabled by organic pyridinium intercalation for artificial biosynapse application

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Nano Research 2023年第8期16卷 11278-11287页

作者： Yang Li Songtao Ling Ruiyu He Cheng zhang Yue Dong Chunlan Ma Yucheng Jiang Ju Gao Jinghui He qichun zhang Jiangsu Key Laboratory of Micro and Nano Heat Fluid Flow Technology and Energy Application School of Physical Science and TechnologySuzhou University of Science and TechnologySuzhou 215009China College of Chemistry Chemical Engineeringand Materials ScienceSoochow UniversitySuzhou 215123China Department of Materials Science and Engineering City University of Hong KongKowloonHong Kong 999077China Department of Chemistry&Center of Super-Diamond and Advanced Films(COSDAF) City University of Hong KongKowloonHong Kong 999077China

Graphene oxide(GO)-based memristors offer the promise of low cost,eco-friendliness,and mechanical flexibility,making them attractive candidates for outstanding flexible electronic devices.However,their resistive transitions often display abrupt change rather than bidirectional progressive tuning,which largely limits their applications for biological synapse emulation and neuromorphic computing.Here,a memristor with a novel layered structure of GO/pyridinium/GO is presented with tunable bidirectional feature.The inserted organic pyridinium intercalation succeeds in serving as a satisfactory buffer layer to intrinsically control the formation of conductive filaments during device operation,leading to progressive conductance regulation.Thus,the essential synaptic behaviors including analog memory characteristics,excitatory postsynaptic current,paired pulse facilitation,prepulse inhibition,spike-timing-dependent plasticity,and spike-rate-dependent plasticity are replicated.The emulation of brain-like“learning-forgetting-relearning”process is also implemented.Additionally,the instant responses of the memristor can be stimulated by low operational voltages and short pulse widths.This study paves one way for GO-based memristors to actuate appealing features such as bidirectional tuning and fast speed switching that are desirable for the development of bio-inspired neuromorphic systems.

关键词： graphene oxide nanoscale memristor 2D materials flexible electronics artificial synapses

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Novel isostructural iron‐series‐MOF calcined derivatives as positive and negative electrodes: A new strategy to obtain matched electrodes in a supercapacitor device

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SmartMat 2023年第3期4卷 56-69页

作者： Yawen Dong Jiadi Liu Hui zhang Qingqing Li Feifei Mao Aimin Lu Hua Wu Kuaibing Wang Cheng zhang qichun zhang Jiangsu Key Laboratory of Pesticide Sciences Department of ChemistryCollege of SciencesNanjing Agricultural UniversityNanjingChina College of Resources and Environmental Sciences Nanjing Agricultural UniversityNanjingChina Jiangsu Key Laboratory of Micro and Nano Heat Fluid Flow Technology and Energy Application School of Physical Science and TechnologySuzhou University of Science and TechnologySuzhouChina Department of Materials Science and Engineering City University of Hong KongHong Kong SARChina

The performance of asymmetric supercapacitors(ASCs)is strongly restricted by the capacity gap between the positive and negative electrodes.To address this issue,two new electrode materials deriving from Co‐and Fe‐based metal–organic frameworks(MOFs,Co‐TAMBA‐d,and Fe‐TAMBA‐d)through a single‐step sintering method have been developed by considering the superiorities of the derivatives of MOFs including large surface areas,sufficient metal‐atom‐doping content,and extreme surface wettability to the bath solution.The as‐prepared Co‐TAMBA‐d as a positive electrode delivers typical pseudocapacitive behavior with the improvement of capacity,which is better than those of pristine MOF materials,while Fe‐TAMBA‐d as negative electrodes displays better electrochemical behavior than those of activated carbon.ASCs based on these two electrodes exhibits excellent energy density and power density of 47Wh/kg and 1658 W/kg,respectively,where this device can maintain prominent cycling stability with capacity retention after 5000 cycles being about 75%.Furthermore,the capacity can feed a series of red light‐emitting diodes,which gives solid evidence of the potential utilization.These results can afford the feasibility of isostructural MOF derivatives as promising electrodes in novel ASCs.

关键词： asymmetric supercapacitor Co‐and Fe‐based MOFs isostructural MOFs MOF derivatives

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Flexible,durable,and anti-fouling nanocellulose-based membrane functionalized by block copolymer with ultra-high flux and efficiency for oil-in-water emulsions separation

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Nano Research 2023年第4期16卷 5665-5675页

作者： Jianfei Wu Yuxuan Su Ziwei Cui Yang Yu Jiafu Qu Jundie Hu Yahui Cai Jianzhang Li Dan Tian qichun zhang Co-Innovation Center of Efficient Processing and Utilization of Forest Resources College of Materials Science and EngineeringNanjing Forestry UniversityNanjing 210037China School of Materials Science and Engineering Suzhou University of Science and TechnologySuzhou 215009China Department of Materials Science and Engineering&Center of Super-Diamond and Advanced Films(COSDAF) City University of Hong KongHong Kong 999077China

The clearwater obtained from stabilized oily wastewater has become a worldwide challenge.Nowdays,the area of oil/water emulsion separation materials have accomplished great progress,but still faces the enormous problems of low flux,poor stability,and pollution resistance.Nanocelluloses(cellulose nanocrystals(CNC))with the advantages of hydrophilicity,ecofriendliness,and regeneration are ideal materials for the construction of separation membranes.In this paper,a flexible,antifouling,and durable nanocellulose-based membrane functionalized by block copolymer(poly(N-isopropylacrylamide)-b-poly(N,Ndimethylaminoethyl methacrylate))is prepared via chemical modification and self-assembly,showing high separation efficiency(above 99.6%)for stabilized oil-in-water emulsions,excellent anti-fouling and cycling stability,high-temperature resistance,and acid and alkali resistance.More importantly,the composite membrane has ultra-high flux in separating oil-in-water emulsions(29,003 L·m^(−2)·h^(−1)·bar^(−1))and oil/water mixture(51,444 L·m^(−2)·h^(−1)·bar^(−1)),which ensures high separation efficiency.With its durability,easy scale-up,and green regeneration,we envision this biomass-derived membrane will be an alternative to the existing commercial filter membrane in environmental remediation.

关键词： nanocellulose-based membrane oil/water emulsions separation ultra-high flux good durability anti-fouling property

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