Rationally designed indium oxide catalysts for CO ₂ hydrogenation to methanol with high activity and selectivity

Abstract

Renewable energy-driven methanol synthesis from CO2 and green hydrogen is a viable and key process in both the “methanol economy” and “liquid sunshine” visions. Recently, In2O3-based catalysts have shown great promise in overcoming the disadvantages of traditional Cu-based catalysts. Here, we report a successful case of theory-guided rational design of a much higher performance In2O3 nanocatalyst. Density functional theory calculations of CO2 hydrogenation pathways over stable facets of cubic and hexagonal In2O3 predict the hexagonal In2O3(104) surface to have far superior catalytic performance. This promotes the synthesis and evaluation of In2O3 in pure phases with different morphologies. Confirming our theoretical prediction, a novel hexagonal In2O3 nanomaterial with high proportion of the exposed {104} surface exhibits the highest activity and methanol selectivity with high catalytic stability. The synergy between theory and experiment proves highly effective in the rational design and experimental realization of oxide catalysts for industry-relevant reactions.

Novel Heterogeneous Catalysts for CO2 Hydrogenation to Liquid Fuels

“… 75 , 76 Researchers have clearly demonstrated the structure sensitivity of the In 2 O 3 catalyst in terms of both the phase and the exposed facet by combined computational and experimental studies. 77 , 78 Dang et al reported a successful work of computer-aided rational design of more efficient In 2 O 3 catalysts for CO 2 hydrogenation to CH 3 OH. 78 On the basis of density functional theory (DFT) calculations, they designed and synthesized a highly efficient hexagonal In 2 O 3 catalyst with a high proportion of the exposed {104} surface.…”

“… 77 , 78 Dang et al reported a successful work of computer-aided rational design of more efficient In 2 O 3 catalysts for CO 2 hydrogenation to CH 3 OH. 78 On the basis of density functional theory (DFT) calculations, they designed and synthesized a highly efficient hexagonal In 2 O 3 catalyst with a high proportion of the exposed {104} surface. CH 3 OH selectivity is as high as 92.4% with a CO 2 conversion of more than 17% under 300 °C, 5.0 MPa, 9000 mL g cat –1 h –1 , H 2 /CO 2 = 6.…”

Bismuth atom tailoring of indium oxide surface frustrated Lewis pairs boosts heterogeneous CO2 photocatalytic hydrogenation

“…This situation is tipping the delicate balance of CO 2 in our atmosphere, leading to global warming. To this end, the photocatalytic hydrogenation of CO 2 into value-added chemicals and fuels has attracted global attention, touted a promising means of achieving a carbonneutral economy [1][2][3] . Although materials such as Pd/Nb 2 O 5 4 , Ru/ Al 2 O 3 5 , LDH nanosheets 6 , and Co-PS@SiO 2 7 have been successfully employed as photocatalysts for CO 2 hydrogenation, a photocatalyst does not currently exist that can meet all the stringent requirements for practical application, including a broad solar response, high conversion efficiency, robust stability and low cost.…”

Thermocatalytic hydrogenation of CO2 into aromatics by tailor‐made catalysts: Recent advancements and perspectives

“…Cr 2 O 3 , In 2 O 3 ‐ZrO 2 , and Zn‐ZrO 2 have also been verified to be active for methanol synthesis at higher temperatures (300‐400°C) from CO 2 hydrogenation. The oxygen vacancies in the reducible metal oxides are responsible for the activation of CO 2 molecule 24‐26 …”