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Oxygen reduction electrocatalysis:From conventional to single-atomic platinum-based catalysts for proton exchange membrane fuel cells

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Frontiers in energy 2024年第2期18卷 206-222页

作者： Cheng YUAN Shiming ZHANG Jiujun ZHANG institute for sustainable energy/college of sciences Shanghai UniversityShanghai 200444China

Platinum(Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).However,their catalysis and stability performance still need to be further improved in terms of corrosion of both carbon support and Pt catalyst particles as well as Pt loading *** on the developed synthetic strategies of alloying/nanostructuring Pt particles and modifying/innovating supports in developing conventional Pt-based catalysts,Pt single-atom catalysts(Pt SACs)as the recently burgeoning hot materials with a potential to achieve the maximum utilization of Pt are comprehensively reviewed in this *** design thoughts and synthesis of various isolated,alloyed,and nanoparticlecontained Pt SACs are *** single-atomic Pt coordinating with non-metals and alloying with metals as well as the metal-support interactions of Pt single-atoms with carbon/non-carbon supports are emphasized in terms of the ORR activity and stability of the *** advance further research and development of Pt SACs for viable implementation in PEMFCs,various technical challenges and several potential research directions are outlined.

关键词： oxygen reduction electrocatalysis Pt singleatom catalysts conventional Pt-based catalysts design thoughts and synthesis metal-support interactions

Self assembled electron blocking and lithiophilic interface towards dendrite-free solid-state lithium battery

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Chinese Chemical Letters 2024年第4期35卷 220-225页

作者： Caixia Li Yi Qiu Yufeng Zhao Wuliang Feng institute for sustainable energy&college of sciences Shanghai UniversityShanghai 200444China Key Laboratory of Advanced energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

The poor interfacial contact is one of the biggest challenges that solid-state lithium batteries suffer *** the solid-state electrolyte surface energy by transforming the interface from lithiophobic to lithiophilic is effective to promote the interfacial contact, but electronic conductive interphases usually increase the risk of electron attack, thus leading to uncontrollable Li dendrite growth. Herein, we propose a self-assembled thermodynamic stable Li I interphase to simultaneously improve the interfacial contact between the garnet electrolyte Li_7La_(3)Zr_(2)O_(12)(LLZO) and Li anode, and prohibit the electron attack. The direct contact between LLZO and Li and the high temperature Li melting process was ascribed to Zr4+reduction, which facilitated Li dendrite formation and propagation. With the modification of the high lithiophilic I_(2) thin film, the area specific interfacial resistance of LLZO/Li was reduced from 1525 Ω/cm^(2) to 57 Ω/cm^(2). More importantly, LLZO was protected from being reduced due to the outstanding electronic insulativity of the Li I interphase, which leaded to a high critical current density of 1.2/7.0 m A/cm^(2) in the time/capacity-constant modes, respectively.

关键词： Li_7La_(3)Zr_(2)O_(12) LiI interphase Interfacial contact Li dendrite Thermodynamic stable

Decouple charge transfer reactions in the Li-ion battery

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Journal of energy Chemistry 2024年第5期92卷 759-798页

作者： Yuxuan Bai Qiu-An Huang Kai Wu Jiujun Zhang institute for sustainable energy/college of sciences Shanghai UniversityShanghai 200444China Ningde Contemporary Innovation Laboratory Contemporary Amperex Technology Co.LimitedNingde 352100FujianChina

In the development of Li-ion batteries(LIBs)with high energy/power density,long cycle-life,fast charging,and high safety,an insight into charge transfer reactions is *** electrochemical impedance spectroscopy(EIS)is regarded as a powerful diagnosis tool,it is not a direct but an indirect *** respect to this,some critical questions need to be answered:(i)why EIS can reflect the kinetics of charge transfer reactions;(ii)what the inherent logical relationship between impedance models under different physical scenes is;(iii)how charge transfer reactions compete with each other at multiple *** work aims at answering these questions via developing a theory framework so as to mitigate the blindness and uncertainty in unveiling charge transfer reactions in *** systematically answer the above questions,this article is organized into a three-in-one(review,tutorial,and research)type and the following contributions are made:(i)a brief review is given for impedance model development of the LIBs over the past half century;(ii)an open source code toolbox is developed based on the unified impedance model;(iii)the competive mechanisms of charge transfer reactions are unveiled based on the developed EIS-Toolbox@*** work not only clarifies theoretical fundamentals,but also provides an easy-to-use open source code for EIS-Toolbox@LIB to optimize fast charge/discharge,mitigate cycle aging,and improve energy/power density.

关键词： Electrochemical impedance spectroscopy Unified impedance model Charge transfer reactions Solid/electrolyte diffusion Porous electrode EIS-Toolbox@LIB

Model reduction of fractional impedance spectra for time–frequency analysis of batteries, fuel cells, and supercapacitors

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Carbon energy 2024年第1期6卷 108-141页

作者： Weiheng Li Qiu-An Huang Yuxuan Bai Jia Wang Linlin Wang Yuyu Liu Yufeng Zhao Xifei Li Jiujun Zhang institute for sustainable energy/college of sciences Shanghai UniversityShanghaiChina Shanxi Key Laboratory of Nanomaterials and Nanotechnology School of Mechanical and Electrical EngineeringXi'an University of Architecture and TechnologyXi'anShaanxiChina Xi'an Key Laboratory of New energy Materials and Devices School of Materials Science and EngineeringInstitute of Advanced Electrochemical EnergyXi'an University of TechnologyXi'anShaanxiChina

Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and *** increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently *** present work formularizes a thorough model reduction of fractional impedance spectra for electrochemical energy devices involving not only the model reduction from fractional-order models to integer-order models and from high-to low-order RC circuits but also insight into the evolution of the characteristic time constants during the whole reduction *** following work has been carried out:(i)the model-reduction theory is addressed for typical Warburg elements and RC circuits based on the continued fraction expansion theory and the response error minimization technique,respectively;(ii)the order effect on the model reduction of typical Warburg elements is quantitatively evaluated by time–frequency analysis;(iii)the results of time–frequency analysis are confirmed to be useful to determine the reduction order in terms of the kinetic information needed to be captured;and(iv)the results of time–frequency analysis are validated for the model reduction of fractional impedance spectra for lithium-ion batteries,supercapacitors,and solid oxide fuel *** turn,the numerical validation has demonstrated the powerful function of the joint time–frequency *** thorough model reduction of fractional impedance spectra addressed in the present work not only clarifies the relationship between time-domain transient analysis and frequency-domain stationary analysis but also enhances the reliability of the joint time–frequency analysis for electrochemical energy devices.

关键词： battery,fuel cell,supercapacitor fractional impedance spectroscopy model reduction time-frequency analysis

Low carbon alcohol fuel electrolysis of hydrogen generation catalyzed by a novel and effective Pt–CoTe/C bifunctional catalyst system

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Green energy & Environment 2024年第4期9卷 758-770页

作者： Yang Zhou Lice Yu Jinfa Chang Ligang Feng Jiujun Zhang School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou225002JiangsuChina NanoScience Technology Center University of Central FloridaOrlandoFL32826USA college of sciences&institute for sustainable energy Shanghai UniversityShanghai200444China

Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts for membrane electrode fabrication are required to drive the electrolysis ***,the efficient catalytic promotion effect of a novel catalyst promoter,CoTe,on Pt is demonstrated for low carbon alcohol fuels of methanol and ethanol electrolysis for hydrogen *** and density functional theory calculation results indicate that the optimized electronic structure of Pt–CoTe/C resulting from the synergetic effect between Pt and CoTe further regulates the adsorption energies of CO and H*that enhances the catalytic ability for methanol and ethanol ***,the good water activation ability of CoTe and the strong electronic effect of Pt and CoTe increased the tolerance ability to the poisoning species as demonstrated by the CO-stripping *** high catalytic kinetics and stability,as well as the promotion effect,were also carefully ***,71.9%and 75.5%of the initial peak current density was maintained after 1000 CV cycles in acid electrolyte for methanol and ethanol oxidation;and a low overpotential of 30 and 35 mV was required to drive the hydrogen evolution reaction in methanol and ethanol solution at the current density of 10 mA cm^(-2).In the two-electrode system for alcohol fuels electrolysis,using the optimal Pt–CoTe/C catalyst as bi-functional catalysts,the cell potential of 0.66 V(0.67 V)was required to achieve 10 mA cm^(-2) for methanol(ethanol)electrolysis,much smaller than that of water electrolysis(1.76 V).The current study offers a novel platform for hydrogen generation via low carbon alcohol fuel electrolysis,and the result is helpful to the catalysis mechanism understanding of Pt assisted by the novel promoter.

关键词： Methanol electrolysis Ethanol electrolysis Cobalt telluride Pt-based electrocatalyst Hydrogen evolution reaction

Recent advances,challenges,and perspectives on carbon capture

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Frontiers of Environmental Science & Engineering 2024年第6期18卷 75-104页

作者： Shihan Zhang Yao Shen Chenghang Zheng Qianqian Xu Yifang Sun Min Huang Lu Li Xiongwei Yang Hao Zhou Heliang Ma Zhendong Li Yuanhang Zhang Wenqing Liu Xiang Gao institute of energy and sustainable Development Zhejiang University of TechnologyHangzhou 310014China college of Environment Zhejiang University of TechnologyHangzhou 310014China Baima Lake Laboratory Hangzhou 310051China institute of Carbon Neutrality College of Energy EngineeringZhejiang UniversityHangzhou 310027China State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China Key Laboratory of Environmental Optics and Technology Anhui Institute of Optics and Fine MechanicsHFIPSChinese Academy of SciencesHefei 230031China

Carbon capture,utilization and storage(CCUS)technologies play an essential role in achieving Net Zero Emissions *** the lack of timely reviews on the recent advancements in promising CCUS technologies,it is crucial to provide a prompt review of the CCUS advances to understand the current research gaps pertained to its industrial *** that end,this review first summarized the developmental history of CCUS technologies and the current large-scale ***,based on a visually bibliometric analysis,the carbon capture remains a hotspot in the CCUS *** that the materials applied in the carbon capture process determines its *** a result,the state-of-the-art carbon capture materials and emerging capture technologies were comprehensively summarized and *** between state-of-art carbon capture process and its ideal counterpart are analyzed,and insights into the research needs such as material design,process optimization,environmental impact,and technical and economic assessments are provided.

关键词： Carbon capture,utilization and storage Visualization analysis Research hotspots and trends CO_(2)capture technology

Subnanometric bimetallic Pt–Pd clusters in zeolites for efficient hydrogen production and selective tandem hydrogenation of nitroarenes

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Science China Chemistry 2024年第9期67卷 2911-2917页

作者： Jiafu Li Tao Cai Yanran Feng Xia Liu Ning Wang Qiming Sun institute of sustainable energy and Resources College of Chemistry and Chemical Engineering Key Laboratory of Shandong Provincial Universities for Functional Molecules and Materials Qingdao University Innovation Center for Chemical sciences College of Chemistry Chemical Engineering and Materials Science Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University

The solvolysis of ammonia borane（AB） and the hydrogenation of nitroarenes represent significant reactions for hydrogen generation and value-added chemical synthesis. The strategic engineering of the catalysts is imperative for surmounting obstacles associated with their stability and catalytic efficiency. In this work, subnanometric bimetallic Pt–Pd clusters were encapsulated within silicalite-1（S-1） zeolites through a ligand-protected in-situ hydrothermal synthesis method. The synergetic effect of bimetallic composition and zeolite confinement markedly enhances the catalytic performance of representative Pt0.5Pd0.5@S-1-H catalyst, affording exceptional turnover frequency（TOF） values of 1,043 and 573 molH2molmetal-1min-1for AB hydrolysis and methanolysis at ambient conditions, respectively, surpassing most of the state-of-the-art Pt-based *** and isotopic experiments reveal that the bimetallic catalytic system remarkably boosts the O–H cleavage of water,thereby facilitating the H2production from AB hydrolysis. Remarkably, a conspicuous synergistic effect is demonstrated in the shape-selective tandem hydrogenation of nitroarenes, with the bimetallic catalyst facilitating both AB hydrolysis and nitroarene hydrogenation, giving a high TOF value of 1,260 h-1under atmospheric pressure. This study not only demonstrates the effectiveness of bimetallic nanocatalysts encapsulated in zeolites for hydrogen production from chemical hydrogen storage materials, but also paves the way for the design of catalysts with multifunctional active sites capable of synergistically promoting tandem catalytic processes.

关键词： subnanometer bimetallic cluster zeolite synergistic effect ammonia borane solvolysis selective tandem hydrogenation

Suppression of multistep phase transitions of O3-type cathode for sodium-ion batteries

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Chinese Chemical Letters 2024年第5期35卷 453-458页

作者： Shengyu Zhao Qinhao Shi Wuliang Feng Yang Liu Xinxin Yang Xingli Zou Xionggang Lu Yufeng Zhao institute for sustainable energy&college of sciences Shanghai UniversityShanghai 200444China State Key Laboratory of Advanced Special Steel&Shanghai Key Laboratory of Advanced Ferrometallurgy&School of Materials Science and Engineering Shanghai UniversityShanghai 200444China

O3-type layered oxide cathodes have been widely investigated due to their high reversible capacities and sufficient Na+***,such materials usually suffer from complex multistep phase transitions along with drastic volume changes,leading to the unsatisfied cycle ***,we report a Mg/Ti co-doped O3-type NaNi_(0.5)Mn_(0.5)O_(2),which can effectively suppress the complex multistep phase transition and realize a solid-solution reaction within a wide voltage *** is confirmed that,the Mg/Ti co-doping is beneficial to enhance the structural stability and integrity by absorbing micro-strain and ***,the as obtained sample delivers an outstanding cyclic performance(82.3%after 200 cycles at 1 C)in the voltage range of 2.0-4.0 V,and a high discharge capacity of 86.6 mAh/g after 100 cycles within the wide voltage range(2.0-4.5 V),which outperform the existing *** co-doping strategy offers new insights into high performance O3-type cathode for sodium ion batteries.

关键词： Sodium ion batteries Mg/Ti co-doping Phase transition Cyclic performance High voltage performance

Travel behavior resilience:Theory,method,and empirical studies

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Journal of Geographical sciences 2024年第8期34卷 1657-1674页

作者： HUANG Jie WANG Jiaoe Key Laboratory of Regional sustainable Development Modelling Institute of Geographic Sciences and Natural Resources ResearchCASBeijing 100101China college of Resources and Environment University of Chinese Academy of SciencesBeijing 100049China

Resilience studies have long been a focal point in the fields of geography,social science,urban studies,and ***,resilience studies from multiple disciplines have scrutinized resilience at an individual *** one important behavior in the daily life of human beings,travel behavior is characterized by spatial dependence,spatiotemporal dynamics,and group ***,how to understand the interaction between travel behavior(or demand)and transportation supply and their dynamics is a fundamental question in transportation studies when transportation systems encounter unexpected *** paper refines the definition of travel behavior resilience based on fundamental theories from multiple disciplines,including ecology,transportation engineering,and ***,this paper proposes a conceptual theoretical framework of travel behavior resilience based on the dynamic equilibrium characteristics of transportation supply and *** general,travel behavior has three stages of variation,namely,dramatic reduction,rapid growth,and fluctuation recovery,which have helped capture the travel behavior resilience ***,we construct a corresponding evaluation methodology that is suitable for multiscale and multidimensional *** emphasize that the evaluation of travel behavior resilience should be process-oriented with temporal continuity or capture the inflection points of travel *** multisource big data such as mobile phone signaling data and smart card data,this paper reviews empirical studies on travel behavior resilience,exploring its spatial heterogeneity and group *** location-based analysis,we confirm that people show greater travel behavior resilience in places where people engage in various socioeconomic *** group-based analysis shows that age and socioeconomic attributes of mobility groups significantly affect travel behavior *** behavior resilience can be o

关键词： resilience residential travel social group urban transportation big data