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Ultrahigh oxygen-doped carbon quantum dots for highly efficient H2O2 production via two-electron electrochemical oxygen reduction
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2022-08-15 , DOI: 10.1039/d2ee01797k
Ying Guo, Rong Zhang, Shaoce Zhang, Hu Hong, Yuwei Zhao, Zhaodong Huang, Cuiping Han, Hongfei Li, Chunyi Zhi

Direct electrochemical two-electron oxygen reduction (2eORR) into H2O2 provides a promising alternative for on-site green H2O2 production to the predominant anthraquinone oxidation technology. Oxidized carbon materials have demonstrated their impressive 2eORR activity due to oxygenated functional groups beneficial to the H2O2 formation pathways. However, the 2eORR capability of O-doped carbon catalysts is hindered by the density of O-induced active sites due to the rather low O content (<15%). Herein, we reported a carbon quantum dot (CQD) catalyst with an ultrahigh O content (30.4 at%) fabricated by using glucose (C6H12O6) as the carbon source due to its high atomic ratio of oxygen-to-carbon. The O-rich CQD catalyst exhibits an excellent catalytic capability of H2O2 production with nearly 100% selectivity, exceeding all reported O-doped carbon catalysts. Besides, the CQD catalyst exhibits great potential in practical H2O2 production with a high yield of 10.06 mg cm−2 h−1 and Faraday efficiency of 97.7%, as well as good stability over 10 hours. Experimental and theoretical investigations confirm that the great majority of the C–O bonds are from the etheric groups in the CQD catalyst, and the carbon atoms of the C–O bonds are the most active sites for the 2eORR.

中文翻译:

超高氧掺杂碳量子点通过双电子电化学氧还原高效生产 H2O2

直接电化学双电子氧还原 (2eORR) 为 H 2 O 2为主要的蒽醌氧化技术提供了现场绿色 H 2 O 2生产的有希望的替代方案。由于有利于 H 2 O 2形成途径的氧化官能团,氧化碳材料已证明其令人印象深刻的 2eORR 活性。然而,由于 O 含量相当低(<15%),O 掺杂碳催化剂的 2eORR 能力受到 O 诱导的活性位点密度的阻碍。在此,我们报道了一种使用葡萄糖 (C 6 H 12 O ) 制备的具有超高 O 含量 (30.4 at%) 的碳量子点 (CQD) 催化剂。6)作为碳源,因为它的氧碳原子比高。富氧CQD催化剂表现出优异的H 2 O 2生成催化能力,选择性接近100%,超过了所有报道的O掺杂碳催化剂。此外,CQD催化剂在实际生产H 2 O 2方面表现出巨大的潜力,其产率高达10.06 mg cm -2 h -1,法拉第效率为97.7%,并且在10小时内具有良好的稳定性。实验和理论研究证实,绝大多数C-O键来自CQD催化剂中的醚基,C-O键的碳原子是2eORR最活跃的位点。
更新日期:2022-08-15
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