Zhang Zitao, Chen Weibin, Chu Hsing Kai, Xiong Feng, Zhang Kexin, Yan Huacai, Meng Fanqi, Gao Song, Ma Bing, Hai Xiao, Zou Ruqiang
School of Materials Science and Engineering, Peking University, Beijing, 100871, China.
Angew Chem Int Ed Engl. 2024 Sep 23;63(39):e202410123. doi: 10.1002/anie.202410123. Epub 2024 Aug 12.
Carbon-based materials have been utilized as effective catalysts for hydrogen peroxide electrosynthesis via two-electron oxygen reduction reaction (2e ORR), however the insufficient selectivity and productivity still hindered the further industrial applications. In this work, we report the Fe-O motif activated graphitic carbon material which enabled highly selective HO electrosynthesis operating at high current density with excellent anti-poisoning property. In the bulk production test, the concentration of HO cumulated to 8.6 % in 24 h and the corresponding production rate of 33.5 mol g h outperformed all previously reported materials. Theoretical model backed by in situ characterization verified α-C surrounding the Fe-O motif as the actual reaction site in terms of thermodynamics and kinetics aspects. The strategy of activating carbon reaction site by metal center via oxo-bridge provides inspiring insights for the rational design of carbon materials for heterogeneous catalysis.
碳基材料已被用作通过两电子氧还原反应（2e ORR）进行过氧化氢电合成的有效催化剂，然而选择性和生产率不足仍然阻碍了其进一步的工业应用。在这项工作中，我们报道了一种Fe-O基序活化的石墨碳材料，该材料能够在高电流密度下进行高选择性的HO电合成，并且具有优异的抗中毒性能。在批量生产测试中，HO的浓度在24小时内累积至8.6%，相应的生产率为33.5 mol g h，优于所有先前报道的材料。由原位表征支持的理论模型从热力学和动力学方面验证了Fe-O基序周围的α-C是实际反应位点。通过氧桥由金属中心活化碳反应位点的策略为合理设计用于多相催化的碳材料提供了启发性的见解。
