Lithium promotion of Pt/m-ZrO2 catalysts for low temperature water-gas shift

Rajabi, Zahra; Martinelli, Michela; Watson, Caleb D.; Cronauer, Donald C.; Jeremy Kropf, A.; Jacobs, Gary

doi:10.1016/j.ijhydene.2022.03.022

Title: Lithium promotion of Pt/m-ZrO₂ catalysts for low temperature water-gas shift

Journal Article · 25 March 2023 · International Journal of Hydrogen Energy

DOI: https://doi.org/10.1016/j.ijhydene.2022.03.022 · OSTI ID:1962411

Rajabi, Zahra ^[1]; Martinelli, Michela ^[2]; Watson, Caleb D. ^[1]; Cronauer, Donald C. ^[3];

^[3]; Jacobs, Gary ^[1]

Univ. of Texas at San Antonio, TX (United States)
Univ. of Kentucky, Lexington, KY (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Low temperature water-gas shift (LTS) is an important reaction occurring in a fuel processor for producing and purifying hydrogen. Platinum supported on m-ZrO₂ belongs to a family of catalysts consisting of metal nanoparticles and an active partially reducible oxide, with the catalysis proposed to occur at the boundary between metal particles and the support. In this investigation, increasing the loading of lithium dopant increased the LTS rate up to 0.54 wt % lithium, where conversion was 2.4 times that of the unpromoted catalyst at 260°C. Further increases in lithium loading up to 1.5 wt % decreased the rate, although it remained higher than that of the unpromoted catalyst. Infrared spectroscopy and CO₂ temperature programmed desorption experiments showed three effects with increasing lithium loading: (1) lithium promoter weakened the C–H bond of formate, the proposed rate limiting step of the interfacial surface formate mechanism; (2) high levels of lithium suppressed the platinum site capacity required for hydrogen transfer; and (3) high levels of lithium increased catalyst basicity. Aspects (2) and (3) tended to inhibit desorption of product CO₂, an acidic molecule the removal of which is metal-catalyzed. XANES and XPS experiments revealed that electron transfer to enrich Pt nanoparticles is unlikely the root cause of C–H bond weakening in formate. However, other electronic effects (e.g., electrostatic effects or molecular rearrangement due to enhanced basicity) were not ruled out.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; USDOE Office of Fossil Energy (FE); University of Texas at San Antonio, TX (United States)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1962411

Journal Information:: International Journal of Hydrogen Energy, Vol. 47, Issue 72; ISSN 0360-3199

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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