TY - JOUR
T1 - Electrochemical oxygen reduction to hydrogen peroxide at practical rates in strong acidic media
AU - Zhang, Xiao
AU - Zhao, Xunhua
AU - Zhu, Peng
AU - Adler, Zachary
AU - Wu, Zhen-Yu
AU - Liu, Yuanyue
AU - Wang, Haotian
N1 - Funding Information:
This work was supported by the Robert A. Welch Foundation (grant no. C-2051-20200401) and the David and Lucile Packard Foundation (grant no. 2020-71371). Y.L. acknowledges the support by NSF (Grant No. 1900039), ACS PRF (60934-DNI6), and the Welch Foundation (Grant No. F-1959-20210327). The calculations used computational resources at XSEDE, TACC, Argonne National Lab, and Brookhaven National Lab. X.Z. acknowledges the support by the Fondazione Oronzio e Niccolò De Nora in Applied Electrochemistry.
Funding Information:
This work was supported by the Robert A. Welch Foundation (grant no. C-2051-20200401) and the David and Lucile Packard Foundation (grant no. 2020-71371). Y.L. acknowledges the support by NSF (Grant No. 1900039), ACS PRF (60934-DNI6), and the Welch Foundation (Grant No. F-1959-20210327). The calculations used computational resources at XSEDE, TACC, Argonne National Lab, and Brookhaven National Lab. X.Z. acknowledges the support by the Fondazione Oronzio e Niccolò De Nora in Applied Electrochemistry.
Publisher Copyright:
© 2022, The Author(s).
PY - 2022/12
Y1 - 2022/12
N2 - Electrochemical oxygen reduction to hydrogen peroxide (H2O2) in acidic media, especially in proton exchange membrane (PEM) electrode assembly reactors, suffers from low selectivity and the lack of low-cost catalysts. Here we present a cation-regulated interfacial engineering approach to promote the H2O2 selectivity (over 80%) under industrial-relevant generation rates (over 400 mA cm−2) in strong acidic media using just carbon black catalyst and a small number of alkali metal cations, representing a 25-fold improvement compared to that without cation additives. Our density functional theory simulation suggests a “shielding effect” of alkali metal cations which squeeze away the catalyst/electrolyte interfacial protons and thus prevent further reduction of generated H2O2 to water. A double-PEM solid electrolyte reactor was further developed to realize a continuous, selective (∼90%) and stable (over 500 hours) generation of H2O2 via implementing this cation effect for practical applications.
AB - Electrochemical oxygen reduction to hydrogen peroxide (H2O2) in acidic media, especially in proton exchange membrane (PEM) electrode assembly reactors, suffers from low selectivity and the lack of low-cost catalysts. Here we present a cation-regulated interfacial engineering approach to promote the H2O2 selectivity (over 80%) under industrial-relevant generation rates (over 400 mA cm−2) in strong acidic media using just carbon black catalyst and a small number of alkali metal cations, representing a 25-fold improvement compared to that without cation additives. Our density functional theory simulation suggests a “shielding effect” of alkali metal cations which squeeze away the catalyst/electrolyte interfacial protons and thus prevent further reduction of generated H2O2 to water. A double-PEM solid electrolyte reactor was further developed to realize a continuous, selective (∼90%) and stable (over 500 hours) generation of H2O2 via implementing this cation effect for practical applications.
UR - https://www.scopus.com/pages/publications/85130739301
U2 - 10.1038/s41467-022-30337-0
DO - 10.1038/s41467-022-30337-0
M3 - Journal article
SN - 2041-1723
VL - 13
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 2880
ER -