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Carbon nanocages bridged with graphene enable fast kinetics for dual-carbon lithium-ion capacitors

Green Energy & Environment 2024年第3期9卷 573-583页

作者： Shani Li Yanan Xu Wenhao Liu Xudong Zhang Yibo Ma Qifan Peng Xiong Zhang Xianzhong Sun Kai Wang Yanwei Ma Institute of Electrical Engineering Chinese Academy of SciencesBeijing100190China University of Chinese Academy of Sciences Beijing100049China Innovation Academy for Green Manufacture Beijing100190China Beijing Institute of Technology Beijing100081China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou450001China

Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.

关键词： Hierarchical carbon framework Nanocage ZIF Graphene Lithium-ion capacitors

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Hierarchically Structured Nb_(2)O_5 Microflowers with Enhanced Capacity and Fast-Charging Capability for Flexible Planar Sodium Ion Micro-Supercapacitors

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Nano-Micro Letters 2024年第4期16卷 97-109页

作者： Jiaxin Ma Jieqiong Qin Shuanghao Zheng Yinghua Fu Liping Chi Yaguang Li Cong Dong Bin Li Feifei Xing Haodong Shi Zhong‑Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences457 Zhongshan RoadDalian 116023People’s Republic of China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001People’s Republic of China College of Science Henan Agricultural UniversityNo.63 Agricultural RoadZhengzhou 450002People’s Republic of China Dalian National Laboratory for Clean Energy Chinese Academy of Sciences457 Zhongshan RoadDalian 116023People’s Republic of China University of Chinese Academy of Sciences 19A Yuquan RoadShijingshan DistrictBeijing 100049People’s Republic of China Hebei Key Lab of Optic‑Electronic Information and Materials The College of Physics Science and TechnologyInstitute of Life Science and Green DevelopmentHebei UniversityBaoding 071002People’s Republic of China

Planar Na ion micro-supercapacitors(NIMSCs) that offer both high energy density and power density are deemed to a promising class of miniaturized power sources for wearable and portable microelectron-ics. Nevertheless, the development of NIMSCs are hugely impeded by the low capacity and sluggish Na ion kinetics in the negative ***, we demonstrate a novel carbon-coated Nb_(2)O_5 microflower with a hierarchical structure composed of vertically intercrossed and porous nanosheets, boosting Na ion storage performance. The unique structural merits, including uniform carbon coating, ultrathin nanosheets and abun-dant pores, endow the Nb_(2)O_5 microflower with highly reversible Na ion storage capacity of 245 mAh g^(-1) at 0.25 C and excellent rate *** from high capacity and fast charging of Nb_(2)O_5 microflower, the planar NIMSCs consisted of Nb_(2)O_5 negative electrode and activated car-bon positive electrode deliver high areal energy density of 60.7 μWh cm^(-2),considerable voltage window of 3.5 V and extraordinary cyclability. Therefore, this work exploits a structural design strategy towards electrode materials for application in NIMSCs, holding great promise for flexible microelectronics.

关键词： Nb_(2)O_5 nanosheets Microflowers Sodium ion micro-supercapacitors Flexibility Energy storage

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Engineering Rubisco to enhance CO_(2) utilization

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Synthetic and Systems Biotechnology 2024年第1期9卷 55-68页

作者： Lei Zhao Zhen Cai Yin Li Yanping Zhang cas Key Laboratory of Microbial Physiological and Metabolic Engineering State Key Laboratory of Microbial ResourcesInstitute of MicrobiologyChinese Academy of SciencesBeijing100101China University of Chinese Academy of Sciences Beijing100049China Seeds Research Syngenta Biotechnology ChinaZhong Guan Cun Life Science ParkBeijingChina

Ribulose-1,5-bisphosphate carboxylase/oxygenase(Rubisco)is a pivotal enzyme that mediates the fixation of CO_(2).As the most abundant protein on earth,Rubisco has a significant impact on global carbon,water,and nitrogen ***,the significantly low carboxylation activity and competing oxygenase activity of Rubisco greatly impede high carbon fixation *** review first summarizes the current efforts in directly or indirectly modifying plant Rubisco,which has been challenging due to its high conservation and limitations in chloroplast transformation ***,recent advancements in understanding Rubisco biogenesis with the assistance of chaperones have enabled successful heterologous expression of all Rubisco forms,including plant Rubisco,in *** breakthrough facilitates the acquisition and evaluation of modified proteins,streamlining the measurement of their ***,the establishment of a screening system in *** opens up possibilities for obtaining high-performance mutant enzymes through directed ***,this review emphasizes the utilization of Rubisco in microorganisms,not only expanding their carbon-fixing capabilities but also holding significant potential for enhancing biotransformation processes.

关键词： Rubisco Plant CO_(2)fixation Microbial Carbon fixation pathway Synthetic biology Enzyme engineering

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Divalent anion intercalation and etching-hydrolysis strategies to construct ultra-stable electrodes for seawater splitting

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Science China Chemistry 2024年第2期67卷 687-695页

作者： Jiajia Lu Yang Liu Han-Pu Liang Key Laboratory of Biofuels Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao266101China Henan Provincial Key Laboratory of Nanocomposites and Applications Institute of Nano-Structured Functional MaterialsHuanghe Science and Technology CollegeZhengzhou450006China School of Materials Science and Engineering Henan Normal UniversityXinxiang453007China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China Shandong Energy Institute Qingdao266101China

Developing stable electrodes for seawater splitting remains a great challenge due to the detachment of catalysts at a large operating current and severe anode corrosion caused by ***,divalent anion intercalation and etching-hydrolysis strategies are deployed to synthesize the ultra-stable anode,dendritic Fe(OH)_(3) grown on Ni(SO_4)_(0.3)(OH)_(1.4)–Ni(OH)_(2).Experimental results reveal that the anode exhibits good activity and excellent stability in alkaline simulated *** 500 h,the current density operated at 1.72 V remains 99.5%,about 210 m A cm^(-2).The outstanding stability originates from the etchinghydrolysis strategy,which strengthens the interaction between the catalyst and the carrier and retards thus the detachment of catalysts at a large current ***,theoretical simulations confirm that the intercalated divalent anions,such as SO_4^(2-) and CO_(3)^(2-),can weaken the adsorption strength of chlorine on the surface of catalysts and hinder the coupling and hybridization between chlorine and nickel,which slows down the anode corrosion and improves catalytic ***,the twoelectrode system shows the remarkable 95.1% energy efficiency at 2,000 A m-2and outstanding stability in 6 mol L^(-1) KOH +seawater at 80 ℃.

关键词： seawater splitting stability divalent anion intercalation etching-hydrolysis

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Recent advances and key perspectives of in-situ studies for oxygen evolution reaction in water electrolysis

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Green Energy & Environment 2024年第10期9卷 1497-1517页

作者： Yi Wang Zichen Xu Xianhong Wu Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Shijingshan District Dalian National Laboratory for Clean Energy Chinese Academy of Sciences

Electricity-driven water splitting to produce hydrogen is one of the most efficient ways to alleviate energy crisis and environmental pollution problems, in which the anodic oxygen evolution reaction(OER) is the key half-reaction of performance-limiting in water splitting. Given the complicated reaction process and surface reconstruction of the involved catalysts under actual working conditions, unraveling the real active sites, probing multiple reaction intermediates and clarifying catalytic pathways through in-situ characterization techniques and theoretical calculations are essential. In this review, we summarize the recent advancements in understanding the catalytic process, unlocking the water oxidation active phase and elucidating catalytic mechanism of water oxidation by various in-situ characterization techniques. Firstly, we introduce conventionally proposed traditional catalytic mechanisms and novel evolutionary mechanisms of OER, and highlight the significance of optimal catalytic pathways and intrinsic stability. Next, we provide a comprehensive overview of the fundamental working principles,different detection modes, applicable scenarios, and limitations associated with the in-situ characterization techniques. Further, we exemplified the in-situ studies and discussed phase transition detection, visualization of speciation evolution, electronic structure tracking, observation of reaction active intermediates, and monitoring of catalytic products, as well as establishing catalytic structure–activity relationships and catalytic mechanism. Finally, the key challenges and future perspectives for demystifying the water oxidation process are briefly proposed.

关键词： In-situ studies Water splitting Oxygen evolution reaction Catalytic mechanism

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Regulating surface electron structure of PtNi nanoalloy via boron doping for high‐current‐density Li‐O2 batteries with low overpotential and long‐life cyclability

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SmartMat 2024年第1期5卷 110-120页

作者： Yajun Ding Yuanchao Huang Yuejiao Li Tao Zhang Zhong‐Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianChina State Key Laboratory of Silicon Materials and School of Materials Science and Engineering Zhejiang UniversityHangzhouChina Institute of Advanced Semiconductors Hangzhou Innovation CenterZhejiang UniversityHangzhouChina University of Chinese Academy of Sciences BeijingChina State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghaiChina Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalianChina

The realization of high‐efficiency,reversible,stable,and safe Li‐O2 batteries is severely hindered by the large overpotential and side reactions,especially at high rate ***,rational design of cathode catalysts with high activity and stability is crucial to overcome the terrible issues at high current ***,we report a surface engineering strategy to adjust the surface electron structure of boron(B)‐doped PtNi nanoalloy on carbon nanotubes(PtNiB@CNTs)as an efficient bifunctional cathodic catalyst for high‐rate and long‐life Li‐O2 ***,the Li‐O2 batteries assembled with as‐prepared PtNiB@CNT catalyst exhibit ultrahigh discharge capacity of 20510 mA·h/g and extremely low overpotential of 0.48 V at a high current density of 1000 mA/g,both of which outperform the most reported Pt‐based catalysts ***,our Li‐O2 batteries offer excellent rate capability and ultra‐long cycling life of up to 210 cycles at 1000 mA/g under a fixed capacity of 1000 mA·h/g,which is two times longer than those of Pt@CNTs and PtNi@***,it is revealed that surface engineering of PtNi nanoalloy via B doping can efficiently tailor the electron structure of nanoalloy and optimize the adsorption of oxygen species,consequently delivering excellent Li‐O2 battery ***,this strategy of regulating the nanoalloy by doping nonmetallic elements will pave an avenue for the design of high‐performance catalysts for metal‐oxygen batteries.

关键词： B doping bifunctional catalyst Li‐O2 battery low charge overpotential PtNi nanoalloy

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A confined growth strategy to construct 3DOM SiO_(2) nanoreactor insitu embedded Co_(3)O_(4) nanoparticles catalyst for the catalytic combustion of VOCs:Superior H_(2)O and SO_(2) resistance

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Nano Research 2024年第1期17卷 207-220页

作者： Weigao Han Shilin Wu Fang Dong Weiliang Han Yinghao Chu Linghui Su Zhicheng Tang State Key Laboratory for Oxo Synthesis and Selective Oxidation National Engineering Research Center for Fine Petrochemical IntermediatesLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China Dalian National Laboratory for Clean Energy Dalian 116023China College of Architecture and Environment Sichuan UniversityChengdu 610000China

SO_(2)poisoning is a common problem in the catalytic combustion of volatile organic compounds(VOCs).In this work,we took three-dimensionally ordered macroporous and mesoporous(3DOM)SiO_(2)as the nanoreactor to protect active sites from SO_(2)erosion in the catalytic combustion of ***,the confined growth of metal active nanoparticles in the multi-stage pore is also full of *** we successfully confined Co_(3)O_(4)nanoparticles(NPs)in macroporous and mesoporous ***,the precursors’growth in the pore was controlled and nanoreactors with different pore sizes were prepared by adjusting the loading amount and preparation *** is discovered that the Co_(3)O_(4)NPs confined in 3DOM SiO_(2)nanoreactor showed superior sulfur and water *** functional theory(DFT)calculations verified that the Co-Si catalyst had high SO_(2)adsorption energy(-0.48 eV),which illustrated that SO_(2)was hard to attach to the surface of the Co-Si *** SiO_(2)nanoreactor had low SO_(2)adsorption energy(-5.15 eV),which indicated that SO_(2)was easily absorbed on SiO_(2)*** illustrated that the SiO_(2)nanoreactor could protect effectively active sites from SO_(2)erosion.

关键词： zeolitic imidazolate frameworks(ZIFs) Co_(3)O_(4) benzene catalytic combustion nanoreactor sulfur and water resistance

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Balanced Polysulfide Containment and Lithium Ion Transport in Lithium-Sulfur Batteries via Nitrogen-doped Carbon Hollow Multi-shelled Structures on Modified Separators

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Chemical Research in Chinese Universities 2024年第4期40卷 690-698页

作者： RAO Fu XIAO Qian WEI Yanze WANG Jiangyan YU Ranbo WANG Dan State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190P.R.China Key Laboratory of Biopharmaceutical Preparation and Delivery Chinese Academy of SciencesBeijing100190P.R.China University of Chinese Academy of Sciences Beijing100049P.R.China Department of Physical Chemistry School of Metallurgical and Ecological EngineeringUniversity of Science&Technology BeijingBeijing100083P.R.China

Representing the next-generation technology in lithium-ion batteries,lithium-sulfur(Li-S)batteries offer increased specific energy without relying on scarce metals like nickel and cobalt,but suffer from a low practical specific energy due to poor conductivity and a short lifespan due to the shuttle effect of *** the confinement of polysulfides and the transport of lithium ions requires highly elaborate modifiers for *** multi-shelled structures(HoMSs)show promise as hierarchical mesostructures for separators,offering multiple shell layers and internal cavities that effectively inhibit polysulfide *** design of these structures is crucial to address these challenges *** this study,nitrogen-doped carbon HoMS(NC HoMS)was created using polymer templates through a precisely controlled polymerization *** featuring NC HoMS-modified separators exhibit improved capacity and cycling stability in comparison to those utilizing commercial ***,triple-shelled NC HoMS strikes a balance in polysulfide containment and lithium ion *** a sulfur loading of 6.34 mg/cm^(2),the Li-S battery can consistently complete 100 charge-discharge cycles,starting with a discharge capacity of 966.4 mA·h/g with a 75.8%capacity retention *** HoMS holds potential as the separator modifier in addressing the polysulfide shuttle problem and facilitating the Li-ion transportation for advanced Li-S batteries.

关键词： Hollow multi-shelled structure Carbon material Li-S battery Separator modification Shuttle effect

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High-Voltage and Fast-Charging Lithium Cobalt Oxide Cathodes: From Key Challenges and Strategies to Future Perspectives

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Engineering 2024年第6期37卷 105-127页

作者： Gongrui Wang Zhihong Bi Anping Zhang Pratteek Das Hu Lin Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China

Lithium-ion batteries(LIBs)with the“double-high”characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable ***,the lithium ion(Li+)-storage performance of the most commercialized lithium cobalt oxide(LiCoO_(2),LCO)cathodes is still far from satisfactory in terms of high-voltage and fast-charging capabilities for reaching the double-high ***,we systematically summarize and discuss high-voltage and fast-charging LCO cathodes,covering in depth the key fundamental challenges,latest advancements in modification strategies,and future perspectives in this *** and elaborated discussions are first presented on key fundamental challenges related to structural degradation,interfacial instability,the inhomogeneity reactions,and sluggish interfacial *** provide an instructive summary of deep insights into promising modification strategies and underlying mechanisms,categorized into element doping(Li-site,cobalt-/oxygen-site,and multi-site doping)for improved Li+diffusivity and bulkstructure stability;surface coating(dielectrics,ionic/electronic conductors,and their combination)for surface stability and conductivity;nanosizing;combinations of these strategies;and other strategies(i.e.,optimization of the electrolyte,binder,tortuosity of electrodes,charging protocols,and prelithiation methods).Finally,forward-looking perspectives and promising directions are sketched out and insightfully elucidated,providing constructive suggestions and instructions for designing and realizing high-voltage and fast-charging LCO cathodes for next-generation double-high LIBs.

关键词： Lithium cobalt oxide High energy/power density Fast-charging High-voltage Lithium-ion battery

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Interfacial assembly of 2D polydopamine/graphene heterostructures with well-defined mesopore and tunable thickness for high-energy planar micro-supercapacitors

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Chinese Chemical Letters 2024年第7期35卷 439-444页

作者： Jieqiong Qin Zhi Yang Jiaxin Ma Liangzhu Zhang Feifei Xing Hongtao Zhang Shuxia Tian Shuanghao Zheng Zhong-Shuai Wu College of Science Henan Agricultural UniversityZhengzhou 450002China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China Mechanical and Electrical Engineering Institute Zhengzhou University of Light IndustryZhengzhou 450002China

Two-dimensional(2D)mesoporous pseudocapacitive polymer/graphene heterostructures combine the advanced merits of 2D materials and mesoporous materials,possessing unique nanosheet structure,large specific surface area(SSA),abundant oxygen/nitrogen-containing groups,desirable electrical conductivity and admirable electrochemical redox activity,and hold great potential for constructing high-performance planar micro-supercapacitors(MSCs).Herein,we demonstrate the interfacial assembly of 2D mesoporous polydopamine/graphene(mPDG)heterostructures with well-defined mesopore structure(12 nm)and adjustable thickness(7.5–14.1 nm)for planar high-energy pseudocapacitive *** to medium thickness,exposed mesopore of 12 nm and large SSA of 108 m^(2)/g,the m PDG with 10.8 nm thickness reveals prominent mass capacitance of 419 F/g and impressive cycling stability with~96%capacitance retention after 5000 ***,the symmetric mPDG-based MSCs with“water-in-salt”gel electrolyte present wide voltage window of 1.6 V,superior volumetric energy density of 11.5 mWh/cm^(3),outstanding flexibility and self-integration ***,this work offers a new platform of controllably synthesizing 2D mesoporous heterostructures for high-performance MSCs.

关键词： 2D materials Mesopores Heterostructures Polydopamine High energy density Micro-supercapacitors

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