Insights into the Surface Electronic Structure and Catalytic Activity of InOx/Au(111) Inverse Catalysts for CO2 Hydrogenation to Methanol

Prabhakar Reddy, Kasala; Tian, Yi; Ramírez, Pedro J.; Islam, Arephin; Lim, Hojoon; Rui, Ning; Xie, Yilin; Hunt, Adrian; Waluyo, Iradwikanari; Rodriguez, José A.

doi:10.1021/acscatal.4c05837

Title: Insights into the Surface Electronic Structure and Catalytic Activity of InO_x/Au(111) Inverse Catalysts for CO₂ Hydrogenation to Methanol

Journal Article · 05 November 2024 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.4c05837 · OSTI ID:2477565

^[1]; Tian, Yi ^[2]; Ramírez, Pedro J. ^[3];

^[1];

^[1]; Xie, Yilin ^[4];

^[1];

^[5]

Brookhaven National Laboratory (BNL), Upton, NY (United States)
Stony Brook University, NY (United States)
Universidad Central de Venezuela, Caracas (Venezuela); Zoneca-CENEX, R&D Laboratories, Alta Vista, Monterrey (México)
Brown University, Providence, RI (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States); Stony Brook University, NY (United States)

In this article, the direct conversion of carbon dioxide (CO₂) into methanol (CH₃OH) via low-temperature hydrogenation is crucial for recycling anthropogenic CO₂ emissions and producing fuels or high value chemicals. Nevertheless, it continues to be a great challenge due to the trade-off between selectivity and catalytic activity. For CO₂ hydrogenation, In₂O₃ catalysts are known for their high CH₃OH selectivity. Subsequent studies explored depositing metals on In₂O₃ to enhance CO₂ conversion. Despite extensive research on metal (M) supported In₂O₃ catalysts, the role of In-M alloys and M/In₂O₃ interfaces in CO₂ activation and CH₃OH selectivity remains unclear. In this work, we have examined the behavior of In/Au(111) alloys and InO_x/Au(111) inverse systems during CO₂ hydrogenation using synchrotron-based ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) and catalytic tests in a batch reactor. Indium forms alloys with Au(111) after deposition. The In-Au(111) alloys display high reactivity towards CO₂ and can dissociate the molecule at room temperature to generate InO_x nanostructures. At very low coverages of In (≤ 0.05 ML), the InO_x nanostructures are not stable under CO₂ hydrogenation conditions and the active In-Au(111) alloys produces mainly CO and little methanol. An increase in indium coverage to 0.3 ML led to stable InOx nanostructures under CO₂ hydrogenation conditions. These InO_x/Au(111) catalysts displayed a high selectivity (~ 80 %) towards CH₃OH production and an activity for CO₂ conversion that was at least 10 times larger than that of plain In₂O₃ or Cu(111) and Cu/ZnO(000$$\overline{1)}$$ benchmark catalysts. The results of AP-XPS show that InO_x/Au(111) produces methanol via methoxy intermediates. Inverse oxide/metal catalysts containing InOx open up a possibility for improving CO₂ → CH₃OH conversion in processes associated with the control of environmental pollution and the production of high value chemicals.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2477565

Report Number(s):: BNL-226336-2024-JAAM

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 22 Vol. 14; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Insights into the Surface Electronic Structure and Catalytic Activity of InOx/Au(111) Inverse Catalysts for CO2 Hydrogenation to Methanol

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Title: Insights into the Surface Electronic Structure and Catalytic Activity of InO_x/Au(111) Inverse Catalysts for CO₂ Hydrogenation to Methanol