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Ni–In synergy in CO2 hydrogenation to methanol

DOI: 10.1021/acscatal.1c03170 DOI Help

Authors: Jiadong Zhu (Eindhoven University of Technology) , Francesco Cannizzaro (Eindhoven University of Technology) , Liang Liu (Eindhoven University of Technology) , Hao Zhao (Eindhoven University of Technology) , Nikolay Kosinov (Eindhoven University of Technology) , Ivo. A. W. Filot (Eindhoven University of Technology) , Jabor Rabeah (Leibniz-Institut für Katalyse an der Universität Rostock e. V.) , Angelika Brückner (Leibniz-Institut für Katalyse an der Universität Rostock e. V.) , Emiel J. M. Hensen (Eindhoven University of Technology)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Catalysis , VOL 15 , PAGES 11371 - 11384

State: Published (Approved)
Published: August 2021
Diamond Proposal Number(s): 22225

Open Access Open Access

Abstract: Indium oxide (In2O3) is a promising catalyst for selective CH3OH synthesis from CO2 but displays insufficient activity at low reaction temperatures. By screening a range of promoters (Co, Ni, Cu, and Pd) in combination with In2O3 using flame spray pyrolysis (FSP) synthesis, Ni is identified as the most suitable first-row transition-metal promoter with similar performance as Pd–In2O3. NiO–In2O3 was optimized by varying the Ni/In ratio using FSP. The resulting catalysts including In2O3 and NiO end members have similar high specific surface areas and morphology. The main products of CO2 hydrogenation are CH3OH and CO with CH4 being only observed at high NiO loading (≥75 wt %). The highest CH3OH rate (∼0.25 gMeOH/(gcat h), 250 °C, and 30 bar) is obtained for a NiO loading of 6 wt %. Characterization of the as-prepared catalysts reveals a strong interaction between Ni cations and In2O3 at low NiO loading (≤6 wt %). H2-TPR points to a higher surface density of oxygen vacancy (Ov) due to Ni substitution. X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, and electron paramagnetic resonance analysis of the used catalysts suggest that Ni cations can be reduced to Ni as single atoms and very small clusters during CO2 hydrogenation. Supportive density functional theory calculations indicate that Ni promotion of CH3OH synthesis from CO2 is mainly due to low-barrier H2 dissociation on the reduced Ni surface species, facilitating hydrogenation of adsorbed CO2 on Ov.

Journal Keywords: CO2 hydrogenation; CH3OH; flame spray pyrolysis; Ni promotion; Ni−In synergy

Diamond Keywords: Carbon Capture and Storage (CCS)

Subject Areas: Chemistry, Environment


Instruments: B18-Core EXAFS

Added On: 30/08/2021 15:08

Discipline Tags:

Earth Sciences & Environment Climate Change Physical Chemistry Catalysis Chemistry

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS)