Machine-learning-assisted material discovery of oxygen-rich highly porous carbon active materials for aqueous supercapacitors

• Published in: Nature communications Vol. 14; no. 1; p. 4607
• Main Authors: Wang, Tao, Pan, Runtong, Martins, Murillo L., Cui, Jinlei, Huang, Zhennan, Thapaliya, Bishnu P., Do-Thanh, Chi-Linh, Zhou, Musen, Fan, Juntian, Yang, Zhenzhen, Chi, Miaofang, Kobayashi, Takeshi, Wu, Jianzhong, Mamontov, Eugene, Dai, Sheng
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 01-08-2023; Nature Publishing Group; Nature Portfolio
• Subjects: 639/301/299/1013; 639/638/549/933; Capacitance; Carbon; Carbonaceous materials; Electrochemical analysis; Electrochemistry; Electrodes; Humanities and Social Sciences; Learning algorithms; Machine learning; multidisciplinary; Neutron scattering; Operating temperature; Oxygen; Oxygen content; Polymers; Pore size; Porous materials; Prepolymers; Science; Science (multidisciplinary); Spectroscopy; Sulfuric acid; Supercapacitors; Transport properties
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-023-40282-1

Porous carbons are the active materials of choice for supercapacitor applications because of their power capability, long-term cycle stability, and wide operating temperatures. However, the development of carbon active materials with improved physicochemical and electrochemical properties is generally carried out via time-consuming and cost-ineffective experimental processes. In this regard, machine-learning technology provides a data-driven approach to examine previously reported research works to find the critical features for developing ideal carbon materials for supercapacitors. Here, we report the design of a machine-learning-derived activation strategy that uses sodium amide and cross-linked polymer precursors to synthesize highly porous carbons (i.e., with specific surface areas > 4000 m
2
/g). Tuning the pore size and oxygen content of the carbonaceous materials, we report a highly porous carbon-base electrode with 0.7 mg/cm
2
of electrode mass loading that exhibits a high specific capacitance of 610 F/g in 1 M H
2
SO
4
. This result approaches the specific capacitance of a porous carbon electrode predicted by the machine learning approach. We also investigate the charge storage mechanism and electrolyte transport properties via step potential electrochemical spectroscopy and quasielastic neutron scattering measurements.
Machine-learning technology provides a data-driven approach to find the critical features for ideal carbon-based supercapacitors. Here, the authors report machine-Learning assisted discovery of oxygen rich highly porous carbons that exhibits a high specific capacitance.