Alcohols electrooxidation coupled with H2 production at high current densities promoted by a cooperative catalyst

Zhenhua Li; Yifan Yan; Si-Min Xu; Hua Zhou; Ming Xu; Lina Ma; Mingfei Shao; Xianggui Kong; Bin Wang; Lirong Zheng; Haohong Duan

doi:10.1038/s41467-021-27806-3

Alcohols electrooxidation coupled with H₂ production at high current densities promoted by a cooperative catalyst

Nat Commun. 2022 Jan 10;13(1):147. doi: 10.1038/s41467-021-27806-3.

Authors

Zhenhua Li^#¹, Yifan Yan^#¹, Si-Min Xu^#¹, Hua Zhou^#², Ming Xu¹, Lina Ma¹, Mingfei Shao¹, Xianggui Kong¹, Bin Wang³, Lirong Zheng⁴, Haohong Duan⁵

Affiliations

¹ State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing, 100029, China.
² Department of Chemistry, Tsinghua University, Beijing, 100084, China.
³ Beijing Research Institute of Chemical Industry, Sinopec Group, Beijing, 100013, China.
⁴ Institute of High Energy Physics, the Chinese Academy of Sciences, Beijing, 100049, China.
⁵ Department of Chemistry, Tsinghua University, Beijing, 100084, China. hhduan@mail.tsinghua.edu.cn.

^# Contributed equally.

Abstract

Electrochemical alcohols oxidation offers a promising approach to produce valuable chemicals and facilitate coupled H₂ production. However, the corresponding current density is very low at moderate cell potential that substantially limits the overall productivity. Here we report the electrooxidation of benzyl alcohol coupled with H₂ production at high current density (540 mA cm^-2 at 1.5 V vs. RHE) over a cooperative catalyst of Au nanoparticles supported on cobalt oxyhydroxide nanosheets (Au/CoOOH). The absolute current can further reach 4.8 A at 2.0 V in a more realistic two-electrode membrane-free flow electrolyzer. Experimental combined with theoretical results indicate that the benzyl alcohol can be enriched at Au/CoOOH interface and oxidized by the electrophilic oxygen species (OH*) generated on CoOOH, leading to higher activity than pure Au. Based on the finding that the catalyst can be reversibly oxidized/reduced at anodic potential/open circuit, we design an intermittent potential (IP) strategy for long-term alcohol electrooxidation that achieves high current density (>250 mA cm^-2) over 24 h with promoted productivity and decreased energy consumption.

Abstract

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