Intrinsic selectivity and structure sensitivity of Rhodium catalysts for C2+ oxygenate production [On the intrinsic selectivity and structure sensitivity of Rhodium catalysts for C2+ oxygenate production]

Yang, Nuoya; Medford, Andrew J.; Liu, Xinyan; Studt, Felix; Bligaard, Thomas; Bent, Stacey F.; Nørskov, Jens K.

doi:10.1021/jacs.5b12087

Title: Intrinsic selectivity and structure sensitivity of Rhodium catalysts for C₂₊ oxygenate production [On the intrinsic selectivity and structure sensitivity of Rhodium catalysts for C₂₊ oxygenate production]

Journal Article · Sun Jan 31 00:00:00 EST 2016 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b12087· OSTI ID:1351912

Yang, Nuoya ^[1]; Medford, Andrew J. ^[2]; Liu, Xinyan ^[2]; Studt, Felix ^[2]; Bligaard, Thomas ^[2]; Bent, Stacey F. ^[1]; Nørskov, Jens K. ^[2]

Stanford Univ., Stanford, CA (United States)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Synthesis gas (CO + H₂) conversion is a promising route to converting coal, natural gas, or biomass into synthetic liquid fuels. Rhodium has long been studied as it is the only elemental catalyst that has demonstrated selectivity to ethanol and other C₂₊ oxygenates. However, the fundamentals of syngas conversion over rhodium are still debated. In this work a microkinetic model is developed for conversion of CO and H₂ into methane, ethanol, and acetaldehyde on the Rh (211) and (111) surfaces, chosen to describe steps and close-packed facets on catalyst particles. The model is based on DFT calculations using the BEEF-vdW functional. The mean-field kinetic model includes lateral adsorbate–adsorbate interactions, and the BEEF-vdW error estimation ensemble is used to propagate error from the DFT calculations to the predicted rates. The model shows the Rh(211) surface to be ~6 orders of magnitude more active than the Rh(111) surface, but highly selective toward methane, while the Rh(111) surface is intrinsically selective toward acetaldehyde. A variety of Rh/SiO₂ catalysts are synthesized, tested for catalytic oxygenate production, and characterized using TEM. The experimental results indicate that the Rh(111) surface is intrinsically selective toward acetaldehyde, and a strong inverse correlation between catalytic activity and oxygenate selectivity is observed. Furthermore, iron impurities are shown to play a key role in modulating the selectivity of Rh/SiO₂ catalysts toward ethanol. The experimental observations are consistent with the structure-sensitivity predicted from theory. As a result, this work provides an improved atomic-scale understanding and new insight into the mechanism, active site, and intrinsic selectivity of syngas conversion over rhodium catalysts and may also guide rational design of alloy catalysts made from more abundant elements.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1351912

Journal Information:: Journal of the American Chemical Society, Vol. 138, Issue 11; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 167 works

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Title: Intrinsic selectivity and structure sensitivity of Rhodium catalysts for C₂₊ oxygenate production [On the intrinsic selectivity and structure sensitivity of Rhodium catalysts for C₂₊ oxygenate production]