Chem ( IF 19.1 ) Pub Date : 2021-08-30 , DOI: 10.1016/j.chempr.2021.08.007 June Sung Lim 1 , Jae Hyung Kim 1, 2 , Jinwoo Woo 1 , Du San Baek 1 , Kyuwook Ihm 3 , Tae Joo Shin 4 , Young Jin Sa 5 , Sang Hoon Joo 1, 6
The electrosynthesis of H2O2 via the 2e− oxygen reduction reaction (ORR) is an attractive method for the clean and continuous on-site production of H2O2, for which the development of active and selective electrocatalysts remains a significant challenge. Although carbon nanomaterials have demonstrated promising performance for H2O2 production, the lack of understanding of the active sites and key structural factors has impeded their development. In this work, we have prepared carbon-based model catalysts to investigate the active oxygen functional groups and structural factor. We have identified that the carboxyl group at the edge sites of graphitic carbons is the major active site for the 2e− ORR, and the carbonyl group is a secondary active site. The nanoporous carbon catalyst with abundant active edge sites and optimized structure exhibited the highest H2O2 electrosynthesis activity among the carbon-based catalysts reported to date and excellent long-term stability (168 h) with 99% H2O2 faradic efficiency.
中文翻译:
通过活性位点识别设计高活性纳米多孔碳 H2O2 生产电催化剂
通过 2e -氧还原反应 (ORR)电合成 H 2 O 2是清洁和连续现场生产 H 2 O 2 的一种有吸引力的方法,为此开发活性和选择性电催化剂仍然是一个重大挑战。尽管碳纳米材料已显示出对 H 2 O 2生产,缺乏对活动地点和关键结构因素的了解阻碍了它们的发展。在这项工作中,我们制备了碳基模型催化剂来研究活性氧官能团和结构因素。我们已经确定石墨碳边缘位点的羧基是 2e - ORR的主要活性位点,羰基是次要活性位点。具有丰富活性边缘位点和优化结构的纳米多孔碳催化剂在迄今为止报道的碳基催化剂中表现出最高的 H 2 O 2电合成活性和优异的长期稳定性(168 小时),H 2 O 2法拉第效率为 99% 。