Three‐dimensional (3D)‐printed MXene high‐voltage aqueous micro‐supercapacitors with ultrahigh areal energy density and low‐temperature tolerance
Yuanyuan Zhu,
Qingxiao Zhang,
Jiaxin Ma,
Pratteek Das,
Liangzhu Zhang,
Hanqing Liu,
Sen Wang,
Hui Li,
Zhong‐Shuai Wu
Affiliations
Yuanyuan Zhu
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian China
Qingxiao Zhang
Shanghai Key Laboratory of Rare Earth Functional Materials and Education Ministry Key Laboratory of Resource Chemistry Shanghai Normal University Shanghai China
Jiaxin Ma
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian China
Pratteek Das
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian China
Liangzhu Zhang
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian China
Hanqing Liu
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian China
Sen Wang
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian China
Hui Li
Shanghai Key Laboratory of Rare Earth Functional Materials and Education Ministry Key Laboratory of Resource Chemistry Shanghai Normal University Shanghai China
Zhong‐Shuai Wu
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian China
Abstract The rapid advancement in the miniaturization, integration, and intelligence of electronic devices has escalated the demand for customizable micro‐supercapacitors (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 high‐concentration (18 mol 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 high‐voltage WiB gel electrolyte and 3D‐printed microelectrodes, quasi‐solid‐state M‐SMSCs operating stably at 1.8 V are constructed, and achieve an ultrahigh areal energy density of 1772 μWh cm−2 and excellent low‐temperature tolerance, with a long‐term operation at −40°C. 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.