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

Hui Li, Peng Wen, Dominique S. Itanze, Zachary D. Hood, Shiba Adhikari, Chang Lu, Xiao Ma, Chaochao Dun, Lin Jiang, David L. Carroll, Yejun Qiu () and Scott M. Geyer ()
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Hui Li: Wake Forest University
Peng Wen: Shenzhen Engineering Lab of Flexible Transparent Conductive Films, School of Materials Science and Engineering, Harbin Institute of Technology
Dominique S. Itanze: Wake Forest University
Zachary D. Hood: Center for Nanophase Materials Sciences (CNMS), Oak Ridge National Laboratory (ORNL)
Shiba Adhikari: Material Science and Technology Division (MSTD), Oak Ridge National Laboratory (ORNL)
Chang Lu: Wake Forest University
Xiao Ma: Wake Forest University
Chaochao Dun: Center for Nanotechnology and Molecular Materials, Department of Physics, Wake Forest University
Lin Jiang: Institute of Functional Nano and Soft Materials (FUNSOM), Soochow University
David L. Carroll: Center for Nanotechnology and Molecular Materials, Department of Physics, Wake Forest University
Yejun Qiu: Shenzhen Engineering Lab of Flexible Transparent Conductive Films, School of Materials Science and Engineering, Harbin Institute of Technology
Scott M. Geyer: Wake Forest University

Nature Communications, 2020, vol. 11, issue 1, 1-12

Abstract: Abstract 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).

Date: 2020
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DOI: 10.1038/s41467-020-17584-9

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