Impact of Pore Structure on Two‐Electron Oxygen Reduction Reaction in Nitrogen‐Doped Carbon Materials: Rotating Ring‐Disk Electrode vs. Flow Cell

• Published in: ChemSusChem Vol. 15; no. 5; pp. e202102587 - n/a
• Main Authors: Xu, Hui, Lv, Xue‐Hui, Wang, Hao‐Yu, Ye, Jin‐Yu, Yuan, Jiayin, Wang, Yu‐Cheng, Zhou, Zhi‐You, Sun, Shi‐Gang
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 08.03.2022
• Subjects: Carbon; Carbon - chemistry; electrocatalysis; Electrodes; Electrons; electrosynthesis; Hydrogen peroxide; Nitrogen - chemistry; Oxidation-Reduction; Oxygen - chemistry; oxygen reduction reaction; Oxygen reduction reactions; porous materials; Rotating disks; Rotation; Selectivity; porous materials; electrosynthesis; oxygen reduction reaction; electrocatalysis; hydrogen peroxide
• ISSN: 1864-5631; 1864-564X; 1864-564X
• DOI: 10.1002/cssc.202102587

The impact of pore structure on the two‐electron oxygen reduction reaction (ORR) in nitrogen‐doped carbon materials is currently under debate, and previous studies are mainly limited to the rotating ring‐disk electrode (RRDE) rather than the practical flow cell (FC) system. In this study, assisted by a group of reliable pore models, the impact of two pore structure parameters, that is, Brunauer–Emmett–Teller surface area (SBET) and micropore surface fraction (fmicro), on ORR activity and selectivity are investigated in both RRDE and FC. The ORR mass activity correlates positively to the SBET in the RRDE and FC because a higher SBET can host more active sites. The H2O2 selectivity is independent of fmicro in the RRDE but correlates negatively to fmicro in the FC. The inconsistency results from different states of the electrode in the RRDE and the FC. These insights will guide the design of carbon materials for H2O2 synthesis. A pore excuse for selectivity: The two‐electron oxygen reduction reaction (ORR) selectivity is independent of the micropore surface fraction (fmicro) in a rotating ring‐disk electrode (RRDE) but correlates negatively to fmicro in a flow cell (FC). The inconsistency results from the different reaction microenvironments in the RRDE to and the FC.