A Pentagonal Defect-Rich Metal-Free Carbon Electrocatalyst for Boosting Acidic O2 Reduction to H2O2 Production,Journal of the American Chemical Society

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A Pentagonal Defect-Rich Metal-Free Carbon Electrocatalyst for Boosting Acidic O2 Reduction to H2O2 Production
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-05-09 , DOI: 10.1021/jacs.3c00689
Chang Zhang _{1,

2} , Wangqiang Shen ₁ , Kun Guo ₁ , Mo Xiong ₃ , Jian Zhang ₂ , Xing Lu ₁

Affiliation

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.

中文翻译：

一种富含五边形缺陷的无金属碳电催化剂促进酸性 O2 还原生成 H2O2

_{无金属碳基材料被认为是用于绿色合成过氧化氢 (H 2} O ₂ )的最有前途的双电子氧还原反应 (2e ^– ORR) 电催化剂之一。然而，大多数报道的碳电催化剂在碱中比在酸中表现得更有效。在此，我们创造性地使用富勒烯（C ₆₀）作为氨处理的前驱体，设计并合成了一种富含五角缺陷的氮掺杂碳纳米材料（PD/N–C）。它在酸性电解质中实现了出色的 ORR 活性、2e-^选择性和稳定性，超过了基准 PtHg ₄合金催化剂。令人印象深刻的是，基于 PD/N–C 催化剂的流通池实现了接近 100% 的法拉第效率和显着的 H ₂ O ₂产率，代表了所有无金属催化剂中最好的改进。实验和理论结果表明，PD/N-C 如此出色的 2e ^- ORR 性能源于五方缺陷和氮掺杂之间的协同作用。_{这项工作为设计和构建用于 H 2} O ₂生产及其他用途的高效耐酸碳电催化剂提供了一种有效的策略。

更新日期：2023-05-09

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