Fullerene-derived boron-doped defective nanocarbon for highly selective H2O2 electrosynthesis
Wanqiang Shen+, Chang Zhang+, Muneerah Alomar, Zhiling Du*, Zepeng yang, Junjie Wang, Guangqing Xu, Jian Zhang*, Jun Lv*, and Xing Lu*
Nano Research
https://doi.org/10.1007/s12274-023-5999-x
Abstract
Electrochemical synthesis of hydrogen peroxide (H2O2) via the two-electron (2e) pathway of oxygen reduction reaction (ORR) provides a promising alternative to the current industrial anthraquinone process. However, it still lacks efficient electrocatalysts to achieve high ORR activity and 2e- selectivity simultaneously. Herein, a boron-doped defective nanocarbon (B-DC) electrocatalyst is synthesized by using fullerene frameworks as the precursor and boric oxide as the boron source. The obtained B-DC materials have a hierarchical porous structure, befitting boron dopants, and abundant topological pentagon defects, exhibiting a high ORR onset potential of 0.78 V and a dominated 2e- selectivity (over 95 %). Remarkably, when B-DC electrocatalyst was employed in a real device, it achieves a high H2O2 yield rate (247 mg L-1 h-1), quantitative Faraday efficiency (~100%), and ultrafast organic pollutant degradation rate. The theoretical calculation reveals that the synergistic effect of topological pentagon defects and the incorporation of boron dopants promotes the activation of the O2 molecule and facilitates the desorption of oxygen intermediate. This finding will be very helpful for the comprehension of the synergistic effect of topological defects and heteroatom dopants for boosting the electrocatalytic performance of nanocarbon toward H2O2 production.