Curvature-Dependent Electrochemical Hydrogen Peroxide Synthesis Performance of Oxidized Carbon Nanotubes

作者：Fangxin She, Zhongyuan Guo, Fangzhou Liu, Zixun Yu, Jiaxiang Chen, Yameng Fan, Yaojie Lei, Yuan Chen, Hao Li, Wei Li · 发表于：ACS Catalysis · 年份：2024 · DOI：10.1021/acscatal.4c01637 · 被引用次数：49 · 研究领域：Electrocatalysts for Energy Conversion、Fuel Cells and Related Materials、Advanced battery technologies research

Surface oxidized carbon nanotubes (o-CNTs) can produce sustainable hydrogen peroxide (H 2 O 2 ) by the two-electron transferred oxygen reduction reaction (2e-ORR). The C atoms neighboring to surface epoxy (C–O–C) groups are recognized as active sites. Herein, we report the CNT curvature, or diameter, dependent ORR activity of o-CNT catalysts. Computation modeling suggests that the curvature can alter epoxy group geometry, exerting greater strain on the C–O bond in smaller diameter o-CNTs that leads to improved activity. This theoretical prediction is further experimentally validated by five o-CNTs of different diameters but comparable oxygenous groups. The o-CNT with the smallest diameter (8 nm) delivers the highest H 2 O 2 Faradaic efficiency (>85%, or molar selectivity >90%) and a mass activity of 161 A g –1 at 0.65 V. This curvature effect provides a strategy to design and synthesize efficient electrocatalysts for peroxide production and beyond.