Experimental Proof of the Bifunctional Mechanism for the Hydrogen Oxidation in Alkaline Media

Li, Jingkun; Ghoshal, Shraboni; Bates, Michael K.; Miller, Todd E.; Davies, Veronica; Stavitski, Eli; Attenkofer, Klaus; Mukerjee, Sanjeev; Ma, Zi-Feng; Jia, Qingying

doi:10.1002/anie.201708484

Experimental Proof of the Bifunctional Mechanism for the Hydrogen Oxidation in Alkaline Media

Journal Article · Mon Oct 16 00:00:00 EDT 2017 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201708484· OSTI ID:1433947

^[1]; Ghoshal, Shraboni ^[1]; Bates, Michael K. ^[1]; Miller, Todd E. ^[1]; Davies, Veronica ^[1]; Stavitski, Eli ^[2]; Attenkofer, Klaus ^[2]; Mukerjee, Sanjeev ^[1]; Ma, Zi-Feng ^[3]; ^[1]

Northeastern Univ., Boston, MA (United States). Dept. of Chemistry and Chemical Biology
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Shanghai Jiao Tong Univ. (China). Shanghai Electrochemical Energy Devices Research Center and Dept. of Chemical Engineering

Realization of the hydrogen economy relies on effective hydrogen production, storage, and utilization. The slow kinetics of hydrogen evolution and oxidation reaction (HER/HOR) in alkaline media limits many practical applications involving hydrogen generation and utilization, and how to overcome this fundamental limitation remains debatable. Here we present a kinetic study of the HOR on representative catalytic systems in alkaline media. Electrochemical measurements show that the HOR rate of Pt-Ru/C and Ru/C systems is decoupled to their hydrogen binding energy (HBE), challenging the current prevailing HBE mechanism. The alternative bifunctional mechanism is verified by combined electrochemical and in situ spectroscopic data, which provide convincing evidence for the presence of hydroxy groups on surface Ru sites in the HOR potential region and its key role in promoting the rate-determining Volmer step. The conclusion presents important references for design and selection of HOR catalysts.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Sponsoring Organization:: National Natural Science Foundation of China (NSFC); USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-76SF00515; SC0012704

OSTI ID:: 1433947

Report Number(s):: BNL--203460-2018-JAAM

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 49 Vol. 56; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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