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Strong Interaction Between redox mediators and Defect-Rich Carbons Enabling Simultaneously Boosted Voltage Windows and Capacitance for Aqueous Supercapacitors

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Energy & Environmental Materials 2024年第4期7卷 269-276页

作者： Lu Guan Yifan Zhu Yi Wan Mengdi Zhang Qiang Li Xiaoling Teng Yunlong Zhang Hao Yang Yan Zhang Han Hu Mingbo Wu State Key Laboratory of Heavy Oil Processing College of Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580China College of Physics University-Industry Joint Center for Ocean Observation and Broadband CommunicationQingdao UniversityQingdao 266071China

Energy density,the Achilles’heel of aqueous supercapacitors,is simultaneously determined by the voltage window and specific capacitance of the carbon materials,but the strategy of synchronously boosting them has rarely been ***,we demonstrate that the rational utilization of the interaction between redox mediators(RMs)and carbon electrode materials,especially those with rich intrinsic defects,contributes to extended potential windows and more stored charges *** 4-hydroxy-2,2,6,6-tetramethylpiperidinyloxyl(4OH-TEMPO)and intrinsic defect-rich carbons as the RMs and electrode materials,respectively,the potential window and capacitance are increased by 67%and sixfold in a neutral ***,this strategy could also be applied to alkaline and acid *** first-principle calculation and experimental results demonstrate that the strong interaction between 4OH-TEMPO and defectrich carbons plays a key role as preferential adsorbed RMs may largely prohibit the contact of free water molecules with the electrode materials to terminate the water splitting at elevated *** the RMs offering weaker interaction with the electrode materials,the water splitting still proceeds with a thus sole increase of the stored *** results discovered in this work could provide an alternative solution to address the low energy density of aqueous supercapacitors.

关键词： defect-rich carbons redox mediators strong interaction supercapacitors voltage windows

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A molecular sieve-containing protective separator to suppress the shuttle effect of redox mediators in lithium-oxygen batteries

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Nano Research 2023年第7期16卷 9453-9460页

作者： Xinbin Wu Huiping Wu Shundong Guan Ying Liang 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 UniversityBeijing 100084China High-Tech Institute of Xi’an Xi’an 710025China

Lithium-oxygen(Li-O_(2))batteries have a great potential in energy storage and conversion due to their ultra-high theoretical specific energy,but their applications are hindered by sluggish redox reaction kinetics in the charge/discharge *** mediators(RMs),as soluble catalysts,are widely used to facilitate the electrochemical processes in the Li-O_(2)batteries.A drawback of RMs is the shuttle effect due to their solubility and mobility,which leads to the corrosion of a Li metal anode and the degradation of the electrochemical performance of the ***,we synthesize a polymer-based composite protective separator containing molecular *** nanopores with a diameter of 4Åin the zeolite powder(4A zeolite)are able to physically block the migration of 2,2,6,6-tetramethylpiperidinyloxy(TEMPO)molecules with a larger size;therefore,the shuttle effect of TEMPO is *** the assistance of the zeolite molecular sieves,the cycle life of the Li-O_(2)batteries is significantly extended from~20 to 170 cycles at a current density of 250 mA·g^(-1)and a limited capacity of 500 mAh·g^(-1).Our work provides a highly effective approach to suppress the shuttle effects of RMs and boost the electrochemical performance of Li-O_(2)batteries.

关键词： lithium-oxygen batteries redox mediators shuttle effects protective separators zeolite molecular sieves

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Supercapacitors as redox mediators for decoupled water splitting

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Chinese Chemical Letters 2023年第2期34卷 481-484页

作者： Mingrui Guo Jing Zhan Zekun Wang Xiaorui Wang Zhang Dai Ting Wang College of Chemistry and Chemical Engineering Institute for Sustainable Energy and ResourcesQingdao UniversityQingdao 266071China National Engineering Research Center for Colloidal Materials School of Chemistry and Chemical EngineeringShandong UniversityJi'nan 250100China Shandong Shengtong Optical Materials Technology Co. Ltd.Dongying 257500China

With the help of the redox mediator, decoupled water-splitting allows O_(2)and H_(2)to be produced at different times, at different rates, and even in different cells, which promotes both the operation safety and the utilization of renewable power sources. However, the current densities and stabilities of these redox mediators are commonly low, which require further improvements for practical applications. Here, we propose to use supercapacitors as solid state redox mediators for decoupled water splitting. For demonstration, Na_(0.5)MnO_(2)(pseudocapacitor) and active carbon(double layer capacitor), are both used as the redox mediator. These supercapacitors show superior current density(1 A/cm^(2)) and ultralong cycle-life(8000 cycles) compared with commonly investigated battery-based mediators(NiOOH/Ni(OH)_(2)). Our research proves supercapacitors can be used as redox relay with high current density and stability, which may bring new insights in the design of decoupled water splitting systems.

关键词： Decoupled water splitting redox mediators Supercapacitors High current density Ultralong cycle-life

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Decoupled water electrolysis:Flexible strategy for pure hydrogen production with small voltage inputs

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Journal of Energy Chemistry 2024年第7期94卷 340-356页

作者： Kexin Zhou Jiahui Huang Daili Xiang Aijiao Deng Jialei Du Hong Liu Institute for Advanced Interdisciplinary Research(iAIR) Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of ShandongUniversity of JinanJinan 250022ShandongChina State Key Laboratory of Crystal Materials Shandong UniversityJinan 250100ShandongChina Zhengzhou Vocational College of Industrial Safety Zhengzhou 451192HenanChina

Hydrogen gas is widely regarded as an ideal green energy carrier and a potential alternative to fossil fuels for coping with the aggravating energy crisis and environmental ***,the vast majority of the world's hydrogen is produced by reforming fossil fuels;however,this hydrogen-making technology is not sustainable or environmentally friendly because ofits high energy consumption and large carbon ***-driven water splitting(2H_(2)0-2H_(2)+0_(2))becomes an extensively studied scheme for sustain-able hydrogen *** water electrolysis requires an input voltage higher than 1.23 V and forms a gas mixture of H_(2)/O_(2),which results in high electricity consumption,potential safety hazards,and harmful reactive oxygen *** virtue of the auxiliary redox mediators(RMs)as the robust H^(+)/e^(-)reservoir,decoupled electrolysis splits water at a much lower potential and evolves O_(2)(H_(2)O+RMS_(ox)-O_(2)+H-RMS_(red))and H_(2)(H-RMS_(red)-H_(2)+RMS_(ox))at separate times,rates,and spaces,thus pro-ducing the puretarget hydrogen gas *** electrolysis has accelerated the development ofwater electrolysis technology for H_(2) ***,itis still lack of a comprehensive and in-depth review in this field based on different types of *** review highlights the basic principles and critical progress of this emerging water electrolysis mode over the past *** representative examples are then dis-played in detail according to the differences in the *** rational choice and design of RMs have also been ***,novel applications of decoupled water splitting are briefly discussed,including the manufacture of valuable chemicals,Cl_(2) production,pollutant degradation,and other half-reactions in artificial ***,thekey characteristics and disadvantages of each type of mediator are sum-marized in *** addition,we present an outlook for future directions in decoupled

关键词： Hydrogen production Conventional water splitting Decoupled water splitting redox mediators Biomimetics

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An integrated approach to improve the performance of lean–electrolyte lithium–sulfur batteries

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Journal of Energy Chemistry 2022年第4期31卷 585-592页

作者： Hualin Ye Jianguo Sun Yun Zhao Jim Yang Lee Department of Chemical and Biomolecular Engineering National University of Singapore119260Singapore Department of Mechanical Engineering National University of Singapore117575Singapore

While the sulfur conversion reaction kinetics in Li–S batteries is nowadays improved by the use of appropriate electrocatalysts,it remains a challenge for the batteries to perform well under the lean electrolyte condition where polysulfide shuttle,electrode passivation and the loss of electrolyte due to side reactions,are *** challenges are addressed in this study by the tandem use of a polysulfide conversion catalyst and a redox–targeting mediator in a gel sulfur ***,the gel cathode reduces the polysulfide mobility and hence the polysulfide shuttle and the passivation of the lithium anode by the crossover *** redox mediator restrains the deposition of inactive sulfur species in the cathode thereby enabling the Fe–N and Co–N co–doped carbon catalyst to prolong its catalytic ***,the integrated catalytic system is able to increase the discharge capacity of high–loading (6.8 mg cm^(-2)) lean–electrolyte (4.0μL mg^(-1)) Li–S batteries from~630 to~1316 m Ah g^(-1),concurrently with an improvement of the cycle life (600 cycles with 46%capacity retention at 1.0 m A cm^(-2)).redox mediator assisted catalysis in a gel cathode is therefore an effective strategy to extend the application of the sulfur conversion catalyst in lean electrolyte Li–S batteries.

关键词： redox mediators Gel electrolytes Polysulfide catalysis Lean electrolyte Lithium–sulfur batteries

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Utilizing hybrid faradaic mechanism via catalytic and surface interactions for high-performance flexible energy storage system

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Journal of Energy Chemistry 2023年第8期83卷 541-548,I0013页

作者： Dong-Gyu Lee Hyeonggeun Choi Yeonsu Park Min-Cheol Kim Jong Bae Park Suok Lee Younghyun Cho Wook Ahn A-Rang Jang Jung Inn Sohn John Hong Young-Woo Lee Department of Energy Engineering Soonchunhyang UniversityAsan 31538Republic of Korea Division of Physics and Semiconductor Science Dongguk University-SeoulSeoul 04620Republic of Korea Jeonju Centre Korea Basic Science InstituteJeonju 54907Republic of Korea Division of Electrical Electronic and Control EngineeringKongju National UniversityCheonan 31080Republic of Korea School of Materials Science and Engineering Kookmin UniversitySeoul 02707Republic of Korea

Improving the capacitance and energy density is a significant challenge while developing practical and flexible energy storage system(ESS).redox mediators(RMs),as redox-active electrolyte additives,can provide additional energy storing capability via electrochemical faradaic contribution on electrodes for high-performance flexible ***,determining effective material combinations between electrodes and RMs is essential for maximizing surface faradaic redox reactions for energy-storage *** this study,an electrode-RM system comprising heterostructured hybrid(carbon fiber(CF)/MnO_(2)) faradaic electrodes and iodine RMs(I-RMs) in a redox-active electrolyte is *** CF/MnO_(2)with the 1-RMs(CF/MnO_(2)-I) induces dominant catalytic faradaic interaction with the I-RMs,significantly enhancing the surface faradaic kinetics and increasing the overall energy-storage *** CF/MnO_(2)-I ESSs show a 12.6-fold(or higher) increased volumetric energy density of 793.81 mWh L^(-1)at a current of 10 μA relative to ESSs using CF/MnO_(2)without I-RMs(CF/MnO_(2)).Moreover,the CF/MnO_(2)-I retains 93.1% of its initial capacitance after 10,000 cycles,validating the excellent ***,the flexibility of the ESSs is tested at different bending angles(180° to 0°),demonstrating its feasibility for flexible and high-wear ***,CF/MnO_(2)electrodes present a practical material combination for high-performance flexible energy-storage devices owing to the catalytic faradaic interaction with I-RMs.

关键词： Energy storage system redox mediators Faradaic electrodes Catalytic interactions Mechanical stability

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redox Mediator Chemistry Regulated Aqueous Batteries:Insights into Mechanisms and Prospects

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CCS Chemistry 2022年第9期4卷 2874-2887页

作者： Tengsheng Zhang Qianru Chen Xinran Li Jiahao Liu Wanhai Zhou Boya Wang Zaiwang Zhao Wei Li Dongliang Chao Dongyuan Zhao Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsSchool of Chemistry and MaterialsFudan UniversityShanghai 200433

redox mediators(RMs),serving as intermediate electron carriers or reservoirs,play vital roles in developing new charge transfer energy storage systems with high voltage or capacity in aqueous ***,the underlying mechanism and selection criteria of RMs remain unclear in aqueous batteries,which hinders the further exploitation of new RMs and aqueous battery chemistries.

关键词： redox mediators aqueous batteries mechanism selection criteria high-efficiency highenergy

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