Interfacial Water Manipulation with Ionic Liquids for the Oxygen Reduction Reaction

Li, Yawei; Malkani, Arnav; Gawas, Ramchandra; Intikhab, Saad; Xu, Bingjun; Tang, Maureen; Snyder, Joshua

doi:10.1021/acscatal.2c04914

Interfacial Water Manipulation with Ionic Liquids for the Oxygen Reduction Reaction

Journal Article · Fri Dec 16 00:00:00 EST 2022 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.2c04914· OSTI ID:2228285

^[1]; ^[2]; ^[3]; Intikhab, Saad ^[3]; ^[4]; ^[3]; ^[3]

Shanxi University, Taiyuan (China); Drexel University, Philadelphia, PA (United States); Drexel University
University of Delaware, Newark, DE (United States)
Drexel University, Philadelphia, PA (United States)
Peking University, Beijing (China); University of Delaware, Newark, DE (United States)

The role that interfacial water plays in both promoting and inhibiting the electrochemical oxygen reduction reaction (ORR) remains somewhat unclear and controversial. Here, we use electroanalytical chemistry, spectroscopy, and microkinetic modeling to probe the impact of hydrophobic ionic liquid (IL) thin films on interfacial water structure and its role in promoting or inhibiting the ORR. Through the use of in situ ATR-SEIRAS, we find that the IL thin films limit the content of water at the interface and prevent the formation of hydrogen bond stabilized water organization. The impact of this exclusion of water on the promotion of the ORR is through the reduced coverage of OH_ad spectator species. The decreased solvation of “active” OH_ad species weakens its interaction with the catalyst surface, lowering the barrier to the last step in the ORR mechanism. This “destabilized” OH_ad impact on ORR kinetics is confirmed through a microkinetic model. Furthermore, the results presented here highlight the mechanistic pathway through which hydrophobic ILs enhance ORR kinetics and point to pathways to both further improve this performance enhancement and the potential for integration of hydrophobic ILs into other technologically relevant elementary electrochemical reactions.

View Accepted Manuscript (DOE)

Research Organization:: Drexel University, Philadelphia, PA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0008434

OSTI ID:: 2228285

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 1 Vol. 13; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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