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

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.

Authors:
 [1]; ORCiD logo [1];  [2];  [3];  [4];  [4];  [1];  [5]; ORCiD logo [6]; ORCiD logo [2]; ORCiD logo [7]; ORCiD logo [1]
  1. Univ. of California, San Diego, CA (United States)
  2. Univ. of Calgary, AB (Canada)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
  4. Columbia Univ., New York, NY (United States)
  5. Central South Univ., Changsha (China)
  6. Univ. of California, Irvine, CA (United States)
  7. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry; Columbia Univ., New York, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); ACS Petroleum Research Fund; Canada First Research Excellence Fund Program
OSTI Identifier:
1633870
Report Number(s):
BNL-216061-2020-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
SC0012704; FG02-13ER16381; 59989-DNI5
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; Electrocatalysis; Nanoscale materials

Citation Formats

Chang, Qiaowan, Zhang, Pu, Mostaghimi, Amir Hassan Bagherzadeh, Zhao, Xueru, Denny, Steven R., Lee, Ji Hoon, Gao, Hongpeng, Zhang, Ying, Xin, Huolin L., Siahrostami, Samira, Chen, Jingguang G., and Chen, Zheng. Promoting H2O2 production via 2-electron oxygen reduction by coordinating partially oxidized Pd with defect carbon. United States: N. p., 2020. Web. https://doi.org/10.1038/s41467-020-15843-3.
Chang, Qiaowan, Zhang, Pu, Mostaghimi, Amir Hassan Bagherzadeh, Zhao, Xueru, Denny, Steven R., Lee, Ji Hoon, Gao, Hongpeng, Zhang, Ying, Xin, Huolin L., Siahrostami, Samira, Chen, Jingguang G., & Chen, Zheng. Promoting H2O2 production via 2-electron oxygen reduction by coordinating partially oxidized Pd with defect carbon. United States. https://doi.org/10.1038/s41467-020-15843-3
Chang, Qiaowan, Zhang, Pu, Mostaghimi, Amir Hassan Bagherzadeh, Zhao, Xueru, Denny, Steven R., Lee, Ji Hoon, Gao, Hongpeng, Zhang, Ying, Xin, Huolin L., Siahrostami, Samira, Chen, Jingguang G., and Chen, Zheng. Fri . "Promoting H2O2 production via 2-electron oxygen reduction by coordinating partially oxidized Pd with defect carbon". United States. https://doi.org/10.1038/s41467-020-15843-3. https://www.osti.gov/servlets/purl/1633870.
@article{osti_1633870,
title = {Promoting H2O2 production via 2-electron oxygen reduction by coordinating partially oxidized Pd with defect carbon},
author = {Chang, Qiaowan and Zhang, Pu and Mostaghimi, Amir Hassan Bagherzadeh and Zhao, Xueru and Denny, Steven R. and Lee, Ji Hoon and Gao, Hongpeng and Zhang, Ying and Xin, Huolin L. and Siahrostami, Samira and Chen, Jingguang G. and Chen, Zheng},
abstractNote = {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.},
doi = {10.1038/s41467-020-15843-3},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {2020},
month = {5}
}

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