The rapid advancement in the miniaturization,integration,and intelligence of electronic devices has escalated the demand for customizable microsupercapacitors(MSCs)with high energy density.However,efficient microfabri...The rapid advancement in the miniaturization,integration,and intelligence of electronic devices has escalated the demand for customizable microsupercapacitors(MSCs)with high energy density.However,efficient microfabrication of safe and high‐energy MXene MSCs for integrating microelectronics remains a significant challenge due to the low voltage window in aqueous electrolytes(typically≤0.6 V)and limited areal mass loading of MXene microelectrodes.Here,we tackle these challenges by developing a highconcentration(18mol kg^(−1))“water‐in‐LiBr”(WiB)gel electrolyte for MXene symmetric MSCs(M‐SMSCs),demonstrating a record high voltage window of 1.8 V.Subsequently,additive‐free aqueous MXene ink with excellent rheological behavior is developed for three‐dimensional(3D)printing customizable all‐MXene microelectrodes on various substrates.Leveraging the synergy of a highvoltage WiB gel electrolyte and 3D‐printed microelectrodes,quasi‐solid‐state MSMSCs operating stably at 1.8 V are constructed,and achieve an ultrahigh areal energy density of 1772μWhcm^(−2) and excellent low‐temperature tolerance,with a long‐term operation at−40℃.Finally,by extending the 3D printing protocol,M‐SMSCs are integrated with humidity sensors on a single planar substrate,demonstrating their reliability in miniaturized integrated microsystems.展开更多
基金National Natural Science Foundation of China,Grant/Award Numbers:22005297,22125903,51872283,22209175,22209176National Key Research and Development Program of China,Grant/Award Number:2022YFA1504100+8 种基金Support Program for Excellent Young Talents in Universities of Anhui Province,Grant/Award Number:2022AH030134Anhui Province Higher Education Innovation Team:Key Technologies and Equipment Innovation Team for Clean Energy,Grant/Award Number:2023AH010055Strategic Priority Research Program of the Chinese Academy of Sciences,Grant/Award Number:XDB36030200Dalian Innovation Support Plan for High Level Talents,Grant/Award Number:2019RT09Dalian National Laboratory for Clean Energy(DNL),CAS,DNL Cooperation Fund,CAS,Grant/Award Numbers:DNL202016,DNL202019,DNL202003DICP,Grant/Award Number:DICP I2020032Doctor Research Startup Foundation of Suzhou University,Grant/Award Number:2023BSK015China Postdoctoral Science Foundation,Grant/Award Numbers:2020M680995,2021M693127International Postdoctoral Exchange Fellowship Program,Grant/Award Number:YJ20210311。
文摘The rapid advancement in the miniaturization,integration,and intelligence of electronic devices has escalated the demand for customizable microsupercapacitors(MSCs)with high energy density.However,efficient microfabrication of safe and high‐energy MXene MSCs for integrating microelectronics remains a significant challenge due to the low voltage window in aqueous electrolytes(typically≤0.6 V)and limited areal mass loading of MXene microelectrodes.Here,we tackle these challenges by developing a highconcentration(18mol kg^(−1))“water‐in‐LiBr”(WiB)gel electrolyte for MXene symmetric MSCs(M‐SMSCs),demonstrating a record high voltage window of 1.8 V.Subsequently,additive‐free aqueous MXene ink with excellent rheological behavior is developed for three‐dimensional(3D)printing customizable all‐MXene microelectrodes on various substrates.Leveraging the synergy of a highvoltage WiB gel electrolyte and 3D‐printed microelectrodes,quasi‐solid‐state MSMSCs operating stably at 1.8 V are constructed,and achieve an ultrahigh areal energy density of 1772μWhcm^(−2) and excellent low‐temperature tolerance,with a long‐term operation at−40℃.Finally,by extending the 3D printing protocol,M‐SMSCs are integrated with humidity sensors on a single planar substrate,demonstrating their reliability in miniaturized integrated microsystems.