Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlatio...Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently required.The 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 process.The 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 cells.In turn,the numerical validation has demonstrated the powerful function of the joint time–frequency analysis.The 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.展开更多
Developing sustainable and clean electrochemical energy conversion technologies is a crucial step in addressing the challenges of energy shortage and environmental pollution. Exploring and developing new electrocataly...Developing sustainable and clean electrochemical energy conversion technologies is a crucial step in addressing the challenges of energy shortage and environmental pollution. Exploring and developing new electrocatalysts with excellent performance and low cost will facilitate the commercial use of these energy conversion technologies. Recently, dual-atom catalysts(DACs) have attracted considerable research interest since they exhibit higher metal atom loading and more flexible active sites compared to single-atom catalysts(SACs). In this paper, the latest preparation methods and characterization techniques of DACs are systematically reviewed. The advantages of homonuclear and heteronuclear DACs and the catalytic mechanism and identification technologies between the two DACs are highlighted. The current applications of DACs in the field of electrocatalysis are summarized. The development opportunities and challenges of DACs in the future are prospected. The ultimate goal is to provide new ideas for the preparation of new catalysts with excellent properties by customizing diatomic catalysts for electrochemical applications.展开更多
基金support from the National Science Foundation of China(22078190)the National Key R&D Plan of China(2020YFB1505802).
文摘Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently required.The 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 process.The 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 cells.In turn,the numerical validation has demonstrated the powerful function of the joint time–frequency analysis.The 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.
文摘Developing sustainable and clean electrochemical energy conversion technologies is a crucial step in addressing the challenges of energy shortage and environmental pollution. Exploring and developing new electrocatalysts with excellent performance and low cost will facilitate the commercial use of these energy conversion technologies. Recently, dual-atom catalysts(DACs) have attracted considerable research interest since they exhibit higher metal atom loading and more flexible active sites compared to single-atom catalysts(SACs). In this paper, the latest preparation methods and characterization techniques of DACs are systematically reviewed. The advantages of homonuclear and heteronuclear DACs and the catalytic mechanism and identification technologies between the two DACs are highlighted. The current applications of DACs in the field of electrocatalysis are summarized. The development opportunities and challenges of DACs in the future are prospected. The ultimate goal is to provide new ideas for the preparation of new catalysts with excellent properties by customizing diatomic catalysts for electrochemical applications.