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Atomic/nano-scale in-situ probing the shuttling effect of redox mediator in Na-O_(2) batteries

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Journal of Energy Chemistry 2021年第5期30卷 438-443页

作者： Kai Yang Yiwei Li Langlang Jia Yan Wang Zijian Wang YuChen jia Shichun Yang Magda Titirici Xinhua Liu Luyi Yang Feng Pan School of Advanced Materials Peking University Shenzhen Graduate SchoolShenzhen 518055GuangdongChina School of Transportation Science and Engineering Beihang UniversityBeijing 100191China Department of Chemical Engineering Imperial College LondonLondon SW72AZUK

Sodium-oxygen batteries(Na-O_(2))have attracted extensive attention as promising energy storage systems due to their high energy density and low *** mediators are often employed to improve Na-O_(2) battery performance,however,their effect on the formation mechanism of the oxygen reduction product(NaO_(2))is still ***,we have investigated the formation mechanism of NaO_(2) during the discharge process in the presence of a redox mediator with the help of atomic/nano-scale in-situ characterization tools used in concert(*** force microscope,electrochemical quartz crystal microbalance(EQCM)and laser nano-particle analyzer).As a result,real-time observations on different time scales show that by shuttling electrons to the electrolyte,the redox mediator enables formation of NaO_(2) in the solution-phase instead of within a finite region near the electrode *** findings provide new fundamental insights on the understanding of Na-O_(2) batteries and new consequently perspectives on designing high performance metal-O_(2) batteries and other related functions.

关键词： Na-O_(2)battery In-situ AFM EQCM redox mediator Shuttling effect

Remarkable improvement of cyclic stability in Li-O2 batteries using ruthenocene as a redox mediator

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Chinese Chemical Letters 2020年第7期31卷 1997-2002页

作者： Cuicui Zhu Yiping Wang Ling Shuai Yizhao Tang Ming Qiu Jian Xie Jia Liu Wen Wen Hengquan Chen Suifei Nan Mei Dou Qinggang He College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China Institute of Nanoscience and Nanotechnology College of Physical Science and TechnologyCentral China Normal UniversityWuhan 430079China School of Materials Science and Engineering Zhejiang UniversityHangzhou 310027China Nation&Local United Engineering Laboratory for Power Batteries Faculty of ChemistryNortheast Normal UniversityChangchun 130024China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Ningbo Research Institute Zhejiang UniversityNingbo 315100China

Nonaqueous Li-O2 batteries attract attention for their theoretical specific energy ***,due to the difficulty of decomposition of Li2 O2,Li-O2 batteries have high charge overpotential and poor cycling *** all kinds of catalysts have been studied on the *** to heterogeneous solid catalysts,soluble catalysts achieve faster and more effective transport of electrons by reversible redox ***,we first report ruthenocene(Ruc) as a mobile redox mediator in a Li-O2 battery.0.01 mol/L Ruc in the electrolyte effectively reduces the charging voltage by 610 ***,Ruc greatly increases the cycling life by four-fold(up to 83 cycles) with a simple ketjen black(KB) *** results of SEM,XPS and XRD confirm that less discharge product residue accumulated after *** verify the reaction mechanisms of the mediato r,free energy profiles of the possible reaction pathways based on DFT are provided.

关键词： Li-O2 battery redox mediator Ruthenocene Li2O2 Cycling life

Viologens-based redox mediators with tunable HOMO–LUMO energy gap for highly effective hydrogen peroxide electrosynthesis

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Nano Research 2023年第12期16卷 12936-12941页

作者： Yang Gao Xiaohui Xu Yue Niu Xinran Hu Zeyu Li Longkun Yang Linjie Zhi Bin Wang CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China The Beijing Key Laboratory for Nano-Photonics and Nano-Structure(NPNS) Department of PhysicsCapital Normal UniversityBeijing 100048China College of New Energy China University of Petroleum(East China)Qingdao 266580China

In comparison with the developing nano-carbon catalysts,some small organic molecules are also emerging as catalysts with typical features,however,their working mechanism is still ***,we synthesized a series of viologen-based heterogeneous catalysts with the same molecular skeleton but different substituent groups through anion exchange *** viologen-based molecules were used as a model catalyst to investigate the underlying structure–function relationship for small molecules-based H_(2)O_(2) *** from the commonly reported carbon-based electrocatalysts,viologens can produce H_(2)O_(2) in a synergistic manner,which means that viologens can not only directly catalyze oxygen reduction but also serve as a redox *** found that the ring current and H_(2)O_(2) selectivity of viologens deliver an increasing trend with the increase of the alkyl chain length of alkyl-substituted viologens and further increase when using benzyl as the substituent *** a result,a benzyl-substituted viologen(BV)delivers the best electrocatalytic performance among the samples,including the highest H_(2)O_(2) selectivity of 96.9%at 0.6 V and the largest ring current density of about 13.6 mA·***,density functional theory(DFT)calculations disclose that the carbon atoms bonded with positively charged N are the active sites and the small highest occupied molecular orbital(HOMO)–lowest unoccupied molecular orbital(LUMO)energy gap of BV is beneficial to the synergistic mechanism for H_(2)O_(2) *** work sheds new insight into the efficient H_(2)O_(2) production in a synergistic manner for small molecules-based electrocatalysts.

关键词： viologens electrocatalysis hydrogen peroxide redox mediator oxygen reduction

Strategies to suppress the shuttle effect of redox mediators in lithium-oxygen batteries

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Journal of Energy Chemistry 2021年第9期30卷 135-149页

作者： Xinbin Wu Wei Yu Kaihua Wen Huanchun Wang Xuanjun Wang Ce-Wen Nan Liangliang Li State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua University100084 BeijingChina High-Tech Institute of Xi’an Xi’anChina

Rechargeable lithium-oxygen(Li-O_(2))batteries are the next generation energy storage devices due to their ultrahigh theoretical *** mediators(RMs)are widely used as a homogenous electrocatalyst in non-aqueous Li-O_(2)batteries to enhance their discharge capacity and reduce charge ***,the shuttle effect of RMs in the electrolyte solution usually leads to corrosion of the Li metal anode and uneven Li deposition on the anode surface,resulting in unwanted consumption of electrocatalysts and deterioration of the *** is therefore necessary to take some measures to prevent the shuttle effect of RMs and fully utilize the soluble ***,we summarize the strategies to suppress the RM shuttle effect reported in recent years,including electrolyte additives,protective separators and electrode *** mechanisms of these strategies are analyzed and their corresponding requirements are *** electrochemical properties of Li-O_(2)batteries with different strategies are summarized and *** challenges and perspectives on preventing the shuttle effect of RMs are described for future *** review provides guidance for achieving shuttle-free redox mediation and for designing Li-O_(2)cells with a long cycle life,high energy efficiency and highly reversible electrochemical reactions.

关键词： Lithium-oxygen battery redox mediator Shuttle effect Electrolyte additive Protective separator

Improving the True Cycling of redox mediators-assisted Li-O_(2) Batteries

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Energy & Environmental Materials 2021年第2期4卷 201-207页

作者： Deqing Cao Fengjiao Yu Yuhui Chen Xiangwen Gao State Key Laboratory of Materials-oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjingJiangsu 211816China Materials Science and Engineering Program and Texas Materials Institute University of Texas at AustinAustinTX 78712USA State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China

The application of redox mediators has been considered as a promising strategy to boost the performance of aprotic Li-O_(2)***,the issues brought with redox mediators,especially on the Li anode side have been ***,we propose a facile approach of preparing a gel polymer membrane that not only allow uniform Li plating/stripping withlarge current densities over extended cycling but also inhibit the diffusion of redox mediators and avoid redox shuttling,self-discharge,and internal *** importantly,the gel polymer membrane prevents the penetration of O_(2)and superoxide intermediates from the Li ***,it ensures the successful application of both lithium anode and redox mediators in Li-O_(2)batteries to achieve the desired high capacity and rate ***,it helps understand the benefit and problems of added redox mediators and reactive oxygen species so that theperformance of such Li-O_(2)batteries can be truly evaluated.

关键词： gel polymer electrolyte Li-O_(2)batteries redox mediator redox shuttle effect

Insoluble carbonaceous materials as electron shuttles enhance the anaerobic/anoxic bioremediation of redox pollutants:Recent advances

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Chinese Chemical Letters 2022年第1期33卷 71-79页

作者： Ning Li Jin Jiang Yanbin Xu Hanping Pan Xiaonan Luo Yingbin Hu Jie Cao Key Laboratory for City Cluster Environmental Safety and Green Development of the Ministry of Education Institute of Environmental and Ecological EngineeringGuangdong University of TechnologyGuangzhou 510006China Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou) Guangzhou 511458China School of Environmental Science and Engineering Guangdong University of TechnologyGuangzhou 510006China

Carbonaceous materials can accelerate extracellular electron transfer for the biotransformation of many recalcitrant,redox-sensitive contaminants and have received considerable attention in fields related to anaerobic *** important electron shuttles(ESs),carbonaceous materials effectively participate in redox biotransformation processes,especially microbially-driven Fe reduction or oxidation coupled with pollutions transformation and anaerobic fermentation for energy and by-product *** related bioprocesses are reviewed here to show that carbonaceous ESs can facilitate electron transfer between microbes and extracellular *** classification and characteristics of carbon-containing ESs are summarized,with an emphasis on activated carbon,graphene,carbon nanotubes and carbonbased immobilized *** influencing factors,including carbon material properties(redox potential,electron transfer capability and solubility)and environmental factors(temperature,p H,substrate concentration and microbial species),on pollution catalytic efficiency are ***,we briefly describe the prospects of carbonaceous ESs in the field of microbial-driven environmental remediation.

关键词： Carbonaceous materials Electron shuttle redox mediator Extracellular electron transfer Anaerobic bioremediation

Metal-air batteries: progress and perspective

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Science Bulletin 2022年第23期67卷 2449-2486,M0004页

作者： Yuhui Chen Jijing Xu Ping He Yu Qiao Shaohua Guo Huijun Yang Haoshen Zhou State Key Laboratory of Materials-oriented Chemical Engineering Nanjing Tech UniversityNanjing 211816China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China Center of Energy Storage Materials&Technology College of Engineering and Applied SciencesNational Laboratory of Solid State MicrostructuresNanjing UniversityNanjing 210093China State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Energy Technology Research Institute National Institute of Advanced Industrial Science and TechnologyUmezonoTsukuba 305-8568Japan

The metal-air batteries with the largest theoretical energy densities have been paid much more ***,metal-air batteries including Li-air/O_(2),Li-CO_(2),Na-air/O_(2).and Zn-air/O_(2) batteries,are complex systems that have their respective scientific problems,such as metal dendrite forming/deforming,the kinetics of redox mediators for oxygen reduction/evolution reactions,high overpotentials,desolution of CO_(2),H_(2)O,*** the air and related side reactions on both anode and *** should be the main direction to address these shortages to improve ***,we summarized recently research progress in these metal-air/O_(2) *** perspectives are also provided for these research fields.

关键词： Li-air battery Solid-state Li-air Sealed/closed Li-O2 battery redox mediator Na-air/Zn-air battery

Nonmacrocyclic Iron(II)Soluble redox mediators Leading to High-Rate Li-O_(2)Battery

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CCS Chemistry 2021年第5期3卷 1350-1358页

作者： Baoxing Wang Xiao Wang Xueyi Cheng Jing Zhang Minglei Yan Guochang Li Lijun Yang Qiang Wu Xizhang Wang Zheng Hu Key Laboratory of Mesoscopic Chemistry of MOE Jiangsu Provincial Laboratory for Nano technologySchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023

The lithium-oxygen(Li-O_(2))battery is highly promising but suffers from poor cycling life,especially at high rates;hence,the need for high-efficient accelerating agents is *** macrocyclic Fe-based redox mediators,such as iron(II)phthalocyanine(FePc)and heme,have been developed and anticipated to be ideal due to their bifunctional charge and superoxide shuttling ***,they still operate far below expectations,which could result from the low concentrations in electrolyte due to the strongπ-πinteraction at carbon ***,the authors report a new type of nonmacrocyclic Fe-based redox mediators,iron(II)acetylacetonate[Fe(acac)2]and iron(II)glycinate[Fe(gly)2],which have weakπ-πinteraction with the carbon cathode,thus,remain at high concentrations in the *** Fe(gly)2@Li-O_(2)battery reaches a long life of 321 cycles at 0.5 A g^(−1),which is much superior to the counterpart with the typical macrocyclic FePc,and particularly exhibits a long life of 167 cycles at 2.0 A g^(−1)and 136 cycles at ultrahigh 5.0 A g^(−1).This study demonstrates an efficient strategy to achieve a high-rate performance of Li-O_(2)batteries by developing nonmacrocyclic Fe-based redox mediators with high-efficient electron and superoxide shuttling.

关键词： lithium-oxygen battery redox mediator nonmacrocyclic iron(II)mediator superoxide shuttling high-rate performance

A design of Nafion-coated bilayered quasi-solid electrolyte for lithium-O_(2) batteries with high performance

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Chinese Journal of Chemical Engineering 2021年第6期34卷 208-216页

作者： Yingfei Hou Lin Jiang Yaoyao Zhang Zhiwen Qin Chi Jiang Ming Wang State Key Laboratory of Heavy Oil Processing China University of Petroleum(East China)Qingdao 266580China

Lithium-air(also known as lithium-oxygen)batteries have attracted considerable global attention in recent years due to their extremely high energy density(11,140 W·h·kg^(-1)).The electrolyte is a key element in lithium-air batteries and the traditional organic electrolyte has great safety risk due to *** the contrary,the polymer electrolyte has the advantages of high safety,high stability and easy processing comparing with the organic liquid *** this paper,a new idea was proposed to coat the Nafion membrane on a layer of polymer for blocking the oxidation reduction electric(RM)and Li based on the selective permeability on lithium ion of the Nafion ***-made thicknesscontrollable Nafion membrane,polyvinylidene fluoride-hexafluoropropylene copolymer(PVDF-HFP)and 2,2,6,6-tetramethylpiperidinooxy(TEMPO)were used to prepare a quasi solid polymer electrolyte(NSPE).Electrochemical workstation and LAND battery testing system were used to perform a galvanostatic charge/discharge test on Li-O_(2).The ionic conductivity of NSPE was 4.3×10^(-4)S·cm^(-1)at room temperature and the discharge platform was 2.6 V and the charging voltage was 3.7 V after 50 cycles with the cut-off capacity of 500 mA·h·g^(-1).

关键词： Lithium-air battery Polymer electrolyte redox mediator P(VDF-HFP) Nafion