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Interfacial/bulk synergetic effects accelerating charge transferring for advanced lithium-ion capacitors

Chinese chemical Letters 2024年第6期35卷 168-175页

作者： Chang Liu Zirui Song Xinglan Deng Shihong Xu Renji Zheng Wentao Deng Hongshuai Hou Guoqiang Zou Xiaobo Ji School of Chemistry and chemical Engineering Hunan Institute of EngineeringXiangtan 411104China College of Chemistry and chemical Engineering Central South UniversityChangsha 410083China key laboratory of Hunan Province for Clean and Efficient Utilization of Strategic Calcium-Containing Mineral Resources School of Minerals Processing and BioengineeringCentral South UniversityChangsha 410083China

The exploration of advanced materials through rational structure/phase design is the key to develop highperformance lithium-ion capacitors(LICs).However,high complexity of material preparation and difficulty in quantity production largely hinder the further ***,Cu_(5)FeS_(4-x)/C(CFS@C)heterojunction with rich sulfur vacancies has successfully achieved from natural bornite,presenting low costeffective and bulk-production *** functional theory(DFT)calculations indicate that rich vacancies in bulk phase can decrease band gap of bornite and thus improve its intrinsic electron conductivity,as well as the heterojunction spontaneously evokes a built-in electric field between its interfacial region,largely reducing the migration barrier from 1.27 e V to 0.75 e *** from these merits,the CFS@C electrodes deliver outperformed lithium storage performance,e.g.,high reversible capacity(822.4m Ah/g at 0.1 A/g),excellent cycling stability(up to 820 cycles at 2 A/g and 540 cycles at 5 A/g with respective capacity retention of over or nearly 100%).With CFS@C as anode and porous carbon nanosheets(PCS)as cathode,the assembled CFS@C//PCS LIC full cells exhibit high energy/power density characteristics of 139.2 Wh/kg at 2500 W/*** work is expected to offer significant insights into structure modifications/devising toward natural minerals for advanced energy-storage systems.

关键词： Bulk/interfacial modification Heterostructure Sulfur vacancies Lithium ion capacitors Capacitors

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High-performance oxygen reduction catalysts in both alkaline and acidic fuel cells based on pre-treating carbon material and iron precursor

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Science Bulletin 2017年第23期62卷 1602-1608页

作者： Ping Song Heather M.Barkholtz Ying Wang Weilin Xu Dijia Liu Lin Zhuang State key laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of Sciences chemical Sciences and Engineering Division Argonne National Laboratory College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University

We demonstrate a new and simple method for pre-treating the carbon material and iron precursor to prepare oxygen reduction reaction(ORR) catalysts, which can produce super-high performance and stability in alkaline solution, with high performance in acid solution. This strategy using cheap materials is simply controllable. Moreover, it has achieved smaller uniform nanoparticles to exhibit high stability, and the synergetic effect of Fe and N offered much higher performance in ORR than commercial Pt/C, with high maximum power density in alkaline and acid fuel cell test. So it can make this kind of catalysts be the most promising alternatives of Pt-based catalysts with best performance/price.

关键词： Pre-treatment Uniform nanoparticle Super-high performance High stability Fuel cell

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Mn single-atoms decorated CNT electrodes for high-performance supercapacitors

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Nano Research 2024年第5期17卷 4039-4046页

作者： Qian Rong Chao Yuwen Yingkai Liu Yuanrong Liu Chunyang Wang Yang Wang Ding Zhang Zhen Wen Yunnan key laboratory of Opto-Electronic Information Technology Institute of Physics and Electronic InformationYunnan Normal UniversityKunming 650500China Faculty of Metallurgical and Energy Engineering Kunming University of Science and TechnologyKunming 650093China Department of Physics and Astronomy University of CaliforniaIrvineCA 92697USA School of Materials Science and Engineering National Institute for Advanced MaterialsSmart Sensing Interdisciplinary Science CenterNankai UniversityTianjin 300350China Jiangsu key laboratory for carbon-Based Functional Materials and Devices Institute of Functional Nano and Soft Materials(FUNSOM)Soochow UniversitySuzhou 215123China

Developing highly robust and efficient electrode materials is of critical importance to promoting the energy density of current supercapacitors for ***,we report an efficient catalyst with monodispersed Mn single-atoms embedded in carbon nanotubes(Mn-CNTs)for enhancing the electrode performance of supercapacitors.A high specific capacitance(1523.6 F·g^(-1) at 1.0 A·g^(-1))can be achieved,which is about twice as high as the specific capacitance of the electrode material without the introduction of Mn ***,the asymmetric electrochemical capacitor created with Mn-CNT and activated carbon exhibits a high energy density of 180.8 Wh·kg^(-1) at a power density of 1.4 kW·kg^(-1),much higher than most reported *** study shows that the integration of Mn atoms into the CNT can enhance the charge transport capacity and the number of polar active sites of Mn-CNT and then facilitate chemical interactions between Mn-CNT and OH-.This work provides a novel strategy to enable high-energy storage in supercapacitors by introducing single-atoms into carbon nanotubes to improve electrodes’energy density and cycle life.

关键词： carbon nanotube(CNT) supercapacitor single-atoms power density energy density

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Meta‐analysis of commercial Pt/C measurements for oxygenreduction reactions via data mining

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Chinese Journal of Catalysis 2022年第1期43卷 116-122页

作者： Mingbo Ruan Jing Liu Ping Song Weilin Xu State key laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical Power Changchun Institute of Applied Chemistry Chinese Academy of Science Changchun 130022 Jilin China University of Science and Technology of China Hefei 230026 Anhui China

近几十年来,聚合物电解质膜燃料电池(PEMFC)因其在零排放汽车、固定式和便携式发电设备中的应用而得到迅速发展.燃料电池的阴极氧还原反应(ORR)和阳极氢氧化反应(HOR)常用的催化剂为Pt基催化剂,因此整个燃料电池系统的成本高昂.而ORR的... 详细信息

近几十年来,聚合物电解质膜燃料电池(PEMFC)因其在零排放汽车、固定式和便携式发电设备中的应用而得到迅速发展.燃料电池的阴极氧还原反应(ORR)和阳极氢氧化反应(HOR)常用的催化剂为Pt基催化剂,因此整个燃料电池系统的成本高昂.而ORR的反应速率比HOR慢得多,阴极上的Pt消耗量远高于阳极上.为了降低燃料电池Pt的用量,近年来,许多类型的非铂或低铂ORR电催化剂被报道作为传统Pt基催化剂的可能替代品,以降低成本促进燃料电池的大规模应用.为了评估新催化剂的ORR性能,一般来说,都是以最先进的商业Pt/C的ORR性能作为参考标准进行比较.最简单常用的方法是采用旋转盘电极测试技术,比较线性扫描曲线上极限扩散电流一半处的电位(半波电位E1/2):半波电位越高,说明其ORR性能越好.众所周知, Pt/C催化剂的本征活性主要与其微观结构和组成有关,而不是与测试方案有关,理想情况下,不同实验室对相同类型的商用Pt/C的测量结果应该是相同的.然而,不同实验室采用的测试方案不同,所得的商业Pt/C的“表观”ORR性能差异巨大.显然,在不考虑不同实验室之间测试方案的微小差异的情况下,作为参比的Pt/C电催化剂的这种明显的性能差异使得来自不同实验室的不同催化剂之间的ORR性能的比较变得无序和不可靠.为解决此问题,需要一种标准的简单测试方案作为商业Pt/C甚至其他类型电催化剂的测试参考,以便在不同的实验室中获得易于重复的“表观”结果.本文通过对全球不同实验室的514篇参考文献进行数据挖掘并进行综合分析发现,同类型Pt/C参比的“表观”活性差异可能主要归因于测试方案的差异,如铂负载(μg/cm2)、玻碳电极的尺寸和线性扫描速率等.基于这些主要影响因素,本文重点分析了商业Pt/C的表观活性(E1/2)与测试方案中各因素之间的相关性.经初步分析发现,大部分测试采用非欧姆补偿和负向扫描(从高电位向低电位扫描),在此前提下,本文深入分析了酸性和碱性电解质溶液中Pt载量、电极尺寸、扫描速率以及不同生产厂家对Pt/C的E1/2的影响.结果发现,在直径为4 mm、Pt负载量为20μg/cm2的玻碳工作电极上,以10 mV/s的扫描速率,在酸性和碱性电解质中都可以获得可靠的商业Pt/C最可重复的ORR催化性能(E1/2=0.84±0.03 V),且在高氯酸中的E1/2值比在硫酸中更高,并得到实验证实.本文结果可作为商业Pt/C的ORR半波电位的“黄金参考”,用于评估其他ORR催化剂在酸性和碱性电解液中的性能.这项工作为作为ORR性能参考标准的商业Pt/C的可靠测试提供了参考.

关键词：氧还原反应商业铂碳深度分析验证实验

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Engineering the HER catalytic behavior of heteroatom-doped molybdenum disulfide via versatile partial cation exchange

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Journal of Energy Chemistry 2020年第2期29卷 15-19页

作者： Zhaoyan Luo Junjie Ge Changpeng Liu Wei Xing State key laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina University of Science and Technology of China Hefei 230026AnhuiChina

Water electrolysis is regarded as an environmental friendly and effective technique for large-scale hydrogen(H2)production[1,2].To date,Pt-based electrocatalysts are still the most efficient HER catalysts[3].However,the prohibitive cost and scarcity of precious metal catalysts have restricted its large-scale ***,finding an earth-abundant and effective alternative electrocatalysts is crucial to the development of‘hydrogen economy'.

关键词： Electrocatalyst MoS2 Dual-metal doping Electron level matching Hydrogen evolution reaction

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Recent progress in single-molecule fluorescence technology in nanocatalysis

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Nano Research 2022年第12期15卷 10316-10327页

作者： Jing Cao Dezheng Zhang Weilin Xu State key laboratory of Electroanalytical Chemistry and jilin Province key laboratory of low carbon chemical power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China University of Science and Technology of China Hefei230026China

Nanoparticles(NPs)play a vital role in the energy catalysis process,so understanding the heterogeneous catalytic properties of nanocatalysts is of great significance for rationally guiding the design of ***,the traditional method obtains the average information based on the whole and cannot study the catalytic activity of a single *** is critical to investigate the catalytic activity of individual nanoparticles using in situ *** review summarizes some of ***'s recent accomplishments in studying the catalytic behavior of nanoparticles at the single-particle level using single-molecule fluorescence microscopy(SMFM).These achievements include revealing the effect of size,shape,and surface atoms of Pd nanoparticles on catalytic kinetics and dynamics as well as obtaining the activation energy of single Au nanoparticles for catalytic reactions by single-molecule *** is the first time to study the kinetics and dynamics of single-atom Pt ***,the method was extended to study the Pt deactivation process for hydrogen oxidation reactions as well as the catalytic kinetics of two-electron oxygen reduction reactions of individual Fe3O4 nanoparticles in ***,single-molecule super-resolution techniques were used to observe the evolution of the activity of single Sb doped TiO2 nanorod *** studies are of guiding significance for in-depth understanding and realization of rational design of optimal catalysts.

关键词： single-molecule fluorescence microscopy nanocatalysis kinetics and dynamics activation energy electrocatalysis super-resolution imaging

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Recent advances in active sites identification and regulation of M-N/C electro-catalysts towards ORR

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Science China Chemistry 2019年第6期62卷 669-683页

作者： Jie Liu Zhao Jin Xian Wang Junjie Ge Changpeng Liu Wei Xing State key laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences University of Science and Technology of China laboratory of Advanced power Sources Changchun Institute of Applied Chemistry Chinese Academy of Sciences jilin Province key laboratory of low carbon chemical power Sources

Transition metal and nitrogen co-doped carbon(M–N/C) catalysts are recognized as the most prospective alternatives for platinum-based electro-catalysts towards oxygen reduction reaction(ORR) in polymer electrolyte fuel cells. Recently, significant progress has been achieved in the identification and regulation of active sites of this kind of catalysts. In this mini review,we summarize the techniques and strategies to identify active sites in M–N/C catalysts, the main debates on active sites types, the measurement method for active site density, the reactivity descriptors for M–N/C catalysts, and directions to the design of ORR M–N/C catalysts.

关键词： ORR electro-catalysts M–N/C active sites

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Recent progress on single-molecule nanocatalysis based on single-molecule fluorescence microscopy

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Science Bulletin 2017年第4期62卷 290-301页

作者： Yuwei Zhang Tao Chen Ping Song Weilin Xu State key laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China jilin provincial key laboratory of low carbon chemical power Changchun Institute of Applied ChemistryChinese Academy of SdencesChangchun 130022China Graduate University of Chinese Academy of Sciences Beijing 100049China

Understanding the heterogeneous catalytic properties of nanoparticles is of great significance for the development of high efficient nanocatalysts, but the intrinsic heterogeneities of nanocatalysts were always covered in traditional ensemble studies. This issue can be overcome if one can follow the catalysis of individual nanoparticles in real time. This paper mainly summarizes recent developments in single- molecule nanocatalysis at single particle level in Changchun Institute of Applied Chemistry, Chinese Academy of Sciences. These developments include the revealing of catalytic kinetics of different types （plane ＆ edge） of surface atoms on individual Pd nanocubes, the observing of in situ deactivation of indi- vidual carbon-supported Pt nanoparticles during the electrocatalytic hydrogen-oxidation reaction, and the measurement of catalytic activation energies on single nanocatalysts for both product formation process and dissociation process, etc. These studies further indicate the advantages or unique abilities of single-molecule methods in the studies of nanocatalvsis or even chemical reactions.

关键词： Single-molecule nanocatalysis Single-molecule fluorescence microscopy Activation energy Electrocatalysis Super-resolution imaging

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Recent development of methanol electrooxidation catalysts for directmethanol fuel cell

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Journal of Energy Chemistry 2018年第6期27卷 1618-1628页

作者： Liyuan Gong Zhiyuan Yang Kui Li Wei Xing Changpeng Liu Junjie Ge State key laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun 130022 jilinChina University of Chinese Academy of Sciences Beijing 100039 China laboratory of Advanced power Sources Changchun Institute of Applied Chemistry Chinese Academy of Sdences Changchun 130022 Jilin China jilin Province key laboratory of low carbon chemical power Sources Changchun 130022 Jilin China

Direct methanol fuel cells （DMFCs） are very promising power source for stationary and portable miniatureelectric appliances due to its high efficiency and low emissions of pollutants. As the key material, cata-lysts for both cathode and anode face several problems which hinder the commercialization of *** this review, we mainly focus on anode catalysts of DMFCs. The process and mechanism of methanolelectrooxidation on Pt and Pt-based catalysts in acidic medium have been introduced. The influences ofsize effect and morphology on electrocatalytic activity are discussed though whether there is a size effectin MOP, catalyst is under debate. Besides, the non Pt catalysts are also listed to emphasize though Pt isstill deemed as the indispensable element in anode catalyst of DMFCs in acidic medium. Different cata-lyst systems are compared to illustrate the level of research at present. ome debates need to be verifiedwith experimental evidences.

关键词： DMFCs Methanol electrooxidation Anode catalysts

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Tuning strategies and structure effects of electrocatalysts for carbon dioxide reduction reaction

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Chinese Journal of Catalysis 2022年第7期43卷 1618-1633页

作者： Cong Liu Xuanhao Mei Ce Han Xue Gong Ping Song Weilin Xu State key laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina.

carbon dioxide emissions have increased due to the consumption of fossil fuels,making the neutralization and utilization of CO_(2) a pressing *** a clean and efficient energy conversion process,electrocatalytic reduction can reduce carbon dioxide into a series of alcohols and acidic organic molecules,which can effectively realize the utilization and transformation of carbon *** review focuses on the tuning strategies and structure effects of catalysts for the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).The tuning strategies for the active sites of catalysts have been reviewed from intrinsic and external *** structure effects for the CO_(2)RR catalysts have also been discussed,such as tandem catalysis,synergistic effects and confinement *** expect that this review about tuning strategies and structure effects can provide guidance for designing highly efficient CO_(2)RR electrocatalysts.

关键词： CO_(2)RR Tuning strategies Active sites regulation Structure effect Tandem catalysis Synergistic effect

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