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

Snider, Jonathan L.; Streibel, Verena; Hubert, McKenzie A.; Choksi, Tej S.; Valle, Eduardo; Upham, D. Chester; Schumann, Julia; Duyar, Melis S.; Gallo, Alessandro; Abild-Pedersen, Frank; Jaramillo, Thomas F.

doi:10.1021/acscatal.8b04848

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

Journal Article · Fri Mar 08 00:00:00 EST 2019 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.8b04848· OSTI ID:1529234

Snider, Jonathan L. ^[1]; Streibel, Verena ^[2]; Hubert, McKenzie A. ^[1];

^[2]; Valle, Eduardo ^[1]; Upham, D. Chester ^[1]; Schumann, Julia ^[3];

^[2];

^[3];

^[2]

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

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/g_InPds) 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. As a result, both palladium and nickel were found to form bimetallic catalysts with enhanced methanol activity and selectivity relative to that of indium oxide.

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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; DGE-114747

OSTI ID:: 1529234

Journal Information:: ACS Catalysis, Vol. 9, Issue 4; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 133 works

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Palladium doping of In ₂ O ₃ towards a general and selective catalytic hydrogenation of amides to amines and alcohols Sorribes, Iván; Lemos, Samantha C. S.; Martín, Santiago Catalysis Science & Technology, Vol. 9, Issue 24 https://doi.org/10.1039/c9cy02128k	journal	January 2019
Intermetallic PdIn catalyst for CO ₂ hydrogenation to methanol: mechanistic studies with a combined DFT and microkinetic modeling method Wu, Panpan; Yang, Bo Catalysis Science & Technology, Vol. 9, Issue 21 https://doi.org/10.1039/c9cy01242g	journal	January 2019
Capsule‐Structured Copper–Zinc Catalyst for Highly Efficient Hydrogenation of Carbon Dioxide to Methanol Guo, Yongle; Guo, Xinwen; Song, Chunshan ChemSusChem, Vol. 12, Issue 22 https://doi.org/10.1002/cssc.201902485	journal	October 2019
Atomic-scale engineering of indium oxide promotion by palladium for methanol production via CO2 hydrogenation Frei, Matthias S.; Mondelli, Cecilia; García-Muelas, Rodrigo ETH Zurich https://doi.org/10.3929/ethz-b-000356743	text	January 2019

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

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