Promoting H2O2 production via 2-electron oxygen reduction by coordinating partially oxidized Pd with defect carbon

Qiaowan Chang, Pu Zhang, Amir Hassan Bagherzadeh Mostaghimi, Xueru Zhao, Steven R. Denny, Ji Hoon Lee, Hongpeng Gao, Ying Zhang, Huolin L. Xin (), Samira Siahrostami (), Jingguang G. Chen () and Zheng Chen ()
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Qiaowan Chang: University of California San Diego
Pu Zhang: University of California San Diego
Amir Hassan Bagherzadeh Mostaghimi: University of Calgary
Xueru Zhao: Brookhaven National Laboratory
Steven R. Denny: Columbia University
Ji Hoon Lee: Columbia University
Hongpeng Gao: University of California San Diego
Ying Zhang: Central South University
Huolin L. Xin: University of California
Samira Siahrostami: University of Calgary
Jingguang G. Chen: Brookhaven National Laboratory
Zheng Chen: University of California San Diego

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Electrochemical synthesis of H2O2 through a selective two-electron (2e−) oxygen reduction reaction (ORR) is an attractive alternative to the industrial anthraquinone oxidation method, as it allows decentralized H2O2 production. Herein, we report that the synergistic interaction between partially oxidized palladium (Pdδ+) and oxygen-functionalized carbon can promote 2e− ORR in acidic electrolytes. An electrocatalyst synthesized by solution deposition of amorphous Pdδ+ clusters (Pd3δ+ and Pd4δ+) onto mildly oxidized carbon nanotubes (Pdδ+-OCNT) shows nearly 100% selectivity toward H2O2 and a positive shift of ORR onset potential by ~320 mV compared with the OCNT substrate. A high mass activity (1.946 A mg−1 at 0.45 V) of Pdδ+-OCNT is achieved. Extended X-ray absorption fine structure characterization and density functional theory calculations suggest that the interaction between Pd clusters and the nearby oxygen-containing functional groups is key for the high selectivity and activity for 2e− ORR.

Date: 2020
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DOI: 10.1038/s41467-020-15843-3

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