Sun Lina, Sun Liping, Huo Lihua, Zhao Hui
Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education, School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, China.
Key Laboratory of Molten Salts and Functional Materials of Heilongjiang Province, School of Science, Heihe University, Heihe 164300, China.
Nanomaterials (Basel). 2023 Mar 27;13(7):1188. doi: 10.3390/nano13071188.
HO generation via an electrochemical two-electron oxygen reduction (2e ORR) is a potential candidate to replace the industrial anthraquinone process. In this study, porous carbon catalysts co-doped by nitrogen and oxygen are successfully synthesized by the pyrolysis and oxidation of a ZIF-67 precursor. The catalyst exhibits a selectivity of ~83.1% for 2e ORR, with the electron-transferring number approaching 2.33, and generation rate of 2909.79 mmol g h at 0.36 V (vs. RHE) in KOH solution (0.1 M). The results prove that graphitic N and -COOH functional groups act as the catalytic centers for this reaction, and the two functional groups work together to greatly enhance the performance of 2e ORR. In addition, the introduction of the -COOH functional group increases the hydrophilicity and the zeta potential of the carbon materials, which also promotes the 2e ORR. The study provides a new understanding of the production of HO by electrocatalytic oxygen reduction with MOF-derived carbon catalysts.
通过电化学双电子氧还原（2e ORR）生成过氧化氢是替代工业蒽醌法的一个潜在候选方法。在本研究中，通过对ZIF-67前驱体进行热解和氧化，成功合成了氮氧共掺杂的多孔碳催化剂。该催化剂对2e ORR的选择性约为83.1%，电子转移数接近2.33，在0.1 M KOH溶液中，于0.36 V（相对于可逆氢电极）时的生成速率为2909.79 mmol g⁻¹ h⁻¹。结果表明，石墨态氮和羧基官能团作为该反应的催化中心，这两个官能团协同作用极大地提高了2e ORR的性能。此外，羧基官能团的引入增加了碳材料的亲水性和zeta电位，这也促进了2e ORR。该研究为利用金属有机框架衍生的碳催化剂通过电催化氧还原生产过氧化氢提供了新的认识。
