Tailoring the Selectivity of 1,3-Butadiene versus 1-Butene Adsorption on Pt(111) by Ultrathin Ionic Liquid Films

Winter L, Trzeciak S, Fernandez C, Massicot S, Talwar T, Maier F, Zahn D, Steinrück HP (2023)


Publication Type: Journal article

Publication year: 2023

Journal

Pages Range: 10866-10877

DOI: 10.1021/acscatal.3c02126

Abstract

The solid catalyst with ionic liquid layer (SCILL) concept is a promising approach to enhance the selectivity of hydrogenation reactions, like the selective hydrogenation of 1,3-butadiene to 1-butene using transition-metal catalysts. In this context, the adsorption dynamics of 1,3-butadiene and 1-butene were studied on Pt(111) modified with ultrathin layers of the ionic liquid (IL) 1,3-dimethylimidazolium bis(trifluoromethanesulfonyl)imide ([C1C1Im][Tf2N]). The sticking coefficients of the two hydrocarbons are measured using the direct method of King and Wells. Both olefins show pronounced precursor-mediated dynamics on clean Pt(111) and on the IL-modified surface. Increasing the IL coverage leads to an increased blocking of adsorption sites for the incoming olefins. Coadsorbed hydrogen does not significantly affect the precursor and site-blocking effects for 1,3-butadiene. Interestingly, a smaller IL amount is needed to prevent 1-butene adsorption compared to 1,3-butadiene adsorption, which is proposed to be directly related to the IL’s influence on selective hydrogenation in SCILL catalysis. Indeed, molecular dynamics simulations show IL film densification/relaxation as the key mechanism to allowing/excluding olefin adsorption on the metal. Being a function of IL coverage, the energy of film penetration is used to control the effective olefin adsorption energy and thus creates an operation regime for suppressing 1-butene while permitting 1,3-butadiene adsorption.

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How to cite

APA:

Winter, L., Trzeciak, S., Fernandez, C., Massicot, S., Talwar, T., Maier, F.,... Steinrück, H.-P. (2023). Tailoring the Selectivity of 1,3-Butadiene versus 1-Butene Adsorption on Pt(111) by Ultrathin Ionic Liquid Films. ACS Catalysis, 10866-10877. https://doi.org/10.1021/acscatal.3c02126

MLA:

Winter, Leonhard, et al. "Tailoring the Selectivity of 1,3-Butadiene versus 1-Butene Adsorption on Pt(111) by Ultrathin Ionic Liquid Films." ACS Catalysis (2023): 10866-10877.

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