Design of Aligned Porous Carbon Films with Single‐Atom Co–N–C Sites for High‐Current‐Density Hydrogen Generation

作者：Rui Liu, Zhichao Gong, Jianbin Liu, Juncai Dong, Jiangwen Liao, Huan Liu, Haikang Huang, Jingjing Liu, Minmin Yan, Kang Huang, Haisheng Gong, Jian Xin Zhu, Chunyu Cui, Gonglan Ye, Huilong Fei · 发表于：Advanced Materials · 年份：2021 · DOI：10.1002/adma.202103533 · 被引用次数：154 · 研究领域：Electrocatalysts for Energy Conversion、Catalytic Processes in Materials Science、Advanced battery technologies research

Abstract Metal‐ and nitrogen‐doped carbon (M–N–C) materials as a unique class of single‐atom catalysts (SACs) have increasingly attracted attention as the replacement of platinum for the hydrogen evolution reaction (HER); however, their employment as HER electrodes at high current densities of industrial level remains a grand challenge. Herein, an aligned porous carbon film embedded with single‐atom Co–N–C sites of exceptional activity and stability at high current densities is designed. Within the film, the atomic CoNx moieties exhibit high intrinsic activity, while the multiscale porosity of the carbon frameworks with vertically aligned microchannels afford facilitated mass transfer under the conditions of high production rate and ultrathick electrodes. Moreover, the superwetting properties of the film promote electrolyte wetting and ensure the timely removal of the evolving H2 gas bubbles. The as‐designed film can work as an efficient HER electrode to deliver 500 and 1000 mA cm−2 in acid at overpotentials of 272 and 343 mV, respectively, and can operate uninterruptedly and stably at 1000 mA cm−2 for at least 32 h under static conditions. These findings pave the road toward the rational design of SACs with improved activity and stability at high current densities in gas‐evolving electrocatalytic processes.