化学
电催化剂
催化作用
碳纤维
可逆氢电极
氨生产
无机化学
金属
过氧化氢
选择性
电解质
化学工程
电化学
纳米技术
电极
复合数
材料科学
有机化学
物理化学
工程类
复合材料
参比电极
作者
Chang Zhang,Wangqiang Shen,Kun Guo,Mo Xiong,Jian Zhang,Xing Lu
摘要
Metal-free carbon-based materials are considered one of the most promising two-electron oxygen reduction reaction (2e– ORR) electrocatalysts for the green synthesis of hydrogen peroxide (H2O2). However, most reported carbon electrocatalysts perform much more effectively in alkalis than in acids. Herein, by creatively using fullerene (C60) as the precursor subject to ammonia treatment, we designed and synthesized a pentagonal defect-rich nitrogen-doped carbon nanomaterial (PD/N–C). It achieves outstanding ORR activity, 2e– selectivity, and stability in acidic electrolytes, surpassing the benchmark PtHg4 alloy catalyst. Impressively, the flow cell based on the PD/N–C catalyst achieves nearly 100% Faraday efficiency with a remarkable H2O2 yield, representing the best improvement among all the metal-free catalysts. Experimental and theoretical results reveal that such superb 2e– ORR performance of PD/N–C originates from the synergism between pentagonal defects and nitrogen dopants. This work presents an effective strategy for the design and construction of highly efficient acid-resistant carbon electrocatalysts for H2O2 production and beyond.
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