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Revealing the Synergy between Oxide and Alloy Phases on the Performance of Bimetallic In-Pd Catalysts for CO₂ Hydrogenation to Methanol

Snider, J.L., Streibel, V., Hubert, M.A., Choksi, T.S., Valle, E., Upham, D.C., Schumann, J., Duyar, Melis S., Gallo, A., Abild-Pedersen, F. and Jaramillo, T.F. (2019) Revealing the Synergy between Oxide and Alloy Phases on the Performance of Bimetallic In-Pd Catalysts for CO₂ Hydrogenation to Methanol ACS Catalysis, 9 (4). pp. 3399-3412.

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Abstract

In2O3 has recently emerged as a promising catalyst for methanol synthesis from CO2. In this work, we present the promotional effect of Pd on this catalyst and investigate structure–performance relationships using in situ X-ray spectroscopy, ex situ characterization, and microkinetic modeling. Catalysts were synthesized with varying In:Pd ratios (1:0, 2:1, 1:1, 1:2, 0:1) and tested for methanol synthesis from CO₂/H₂ at 40 bar and 300 °C. In:Pd(2:1)/SiO₂ shows the highest activity (5.1 μmol MeOH/gInPds) and selectivity toward methanol (61%). While all bimetallic catalysts had enhanced catalytic performance, characterization reveals methanol synthesis was maximized when the catalyst contained both In–Pd intermetallic compounds and an indium oxide phase. Experimental results and density functional theory suggest the active phase arises from a synergy between the indium oxide phase and a bimetallic In–Pd particle with a surface enrichment of indium. We show that the promotion observed in the In–Pd system is extendable to non precious metal containing binary systems, in particular In–Ni, which displayed similar composition–activity trends to the In–Pd system. Both palladium and nickel were found to form bimetallic catalysts with enhanced methanol activity and selectivity relative to that of indium oxide.

Item Type: Article
Divisions : Faculty of Engineering and Physical Sciences > Chemical and Process Engineering
Authors :
NameEmailORCID
Snider, J.L.
Streibel, V.
Hubert, M.A.
Choksi, T.S.
Valle, E.
Upham, D.C.
Schumann, J.
Duyar, Melis S.m.duyar@surrey.ac.uk
Gallo, A.
Abild-Pedersen, F.
Jaramillo, T.F.
Date : 5 April 2019
DOI : 10.1021/acscatal.8b04848
Copyright Disclaimer : © 2019 American Chemical Society.
Uncontrolled Keywords : Bimetallic; CO₂ utilization; In situ characterization; In-Ni; In-Pd; In₂O₃; Intermetallic; Methanol synthesis
Depositing User : Clive Harris
Date Deposited : 12 Jun 2019 09:32
Last Modified : 12 Jun 2019 09:32
URI: http://epubs.surrey.ac.uk/id/eprint/851974

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