Scalable neutral H2O2 electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways

Li, Hui; Wen, Peng; Itanze, Dominique S.; Hood, Zachary D.; Adhikari, Shiba; Lu, Chang; Ma, Xiao; Dun, Chaochao; Jiang, Lin; Carroll, David L.; Qiu, Yejun; Geyer, Scott M.

doi:10.1038/s41467-020-17584-9

Title: Scalable neutral H₂O₂ electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways

Journal Article · Thu Aug 06 00:00:00 EDT 2020 · Nature Communications

DOI:https://doi.org/10.1038/s41467-020-17584-9· OSTI ID:1815618

Li, Hui ^[1]; Wen, Peng ^[2]; Itanze, Dominique S. ^[1]; Hood, Zachary D. ^[3];

^[4];

^[1];

^[5]; Jiang, Lin ^[6]; Carroll, David L. ^[5]; Qiu, Yejun ^[2];

^[1]

Wake Forest Univ., Winston-Salem, NC (United States). Dept. of Chemistry
Harbin Inst. of Technology, Shenzhen (China). School of Materials Science and Engineering, Shenzhen Engineering Lab of Flexible Transparent Conductive Film
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Wake Forest Univ., Winston-Salem, NC (United States). Center for Nanotechnology and Molecular Materials and Dept. of Physics
Soochow Univ., Suzhou, Jiangsu (China). Inst. of Functional Nano and Soft Materials (FUNSOM)

Despite progress in small scale electrocatalytic production of hydrogen peroxide (H₂O₂) using a rotating ring-disk electrode, further work is needed to develop a non-toxic, selective, and stable O₂-to-H₂O₂ electrocatalyst for realizing continuous on-site production of neutral hydrogen peroxide. We report ultrasmall and monodisperse colloidal PtP₂ nanocrystals that achieve H₂O₂ production at near zero-overpotential with near unity H₂O₂ selectivity at 0.27 V vs. RHE. Density functional theory calculations indicate that P promotes hydrogenation of OOH* to H₂O₂ by weakening the Pt-OOH* bond and suppressing the dissociative OOH* to O* pathway. Atomic layer deposition of Al₂O₃ prevents NC aggregation and enables application in a polymer electrolyte membrane fuel cell (PEMFC) with a maximum r(H₂O₂) of 2.26 mmol h^-1 cm^-2 and a current efficiency of 78.8% even at a high current density of 150 mA cm^-2. Catalyst stability enables an accumulated neutral H₂O₂ concentration in 600 mL of 3.0 wt% (pH = 6.6).

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation of Guangdong Province; Shenzhen Bureau of Science, Technology and Innovation Commission

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1815618

Journal Information:: Nature Communications, Vol. 11, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Scalable neutral H₂O₂ electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways