Al Promotion of In2O3 for CO2 Hydrogenation to Methanol

Liang Liu; Brahim Mezari; Nikolay A. Kosinov; Emiel J.M. Hensen

doi:10.1021/acscatal.3c04620

Al Promotion of In2O3 for CO2 Hydrogenation to Methanol

Liang Liu
, Brahim Mezari
, Nikolay A. Kosinov
, Emiel J.M. Hensen (Corresponding author)

Research output: Contribution to journal › Article › Academic › peer-review

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Abstract

In2O3 is a promising catalyst for the hydrogenation of CO2 to methanol, relevant to renewable energy storage in chemicals. Herein, we investigated the promoting role of Al on In2O3 using flame spray pyrolysis to prepare a series of In2O3−Al2O3 samples in a single step (0−20 mol % Al). Al promoted the methanol yield, with an optimum being observed at an Al content of 5 mol %. Extensive characterization showed that Al can dope into the In2O3 lattice (maximum ∼ 1.2 mol %), leading to the formation of more oxygen vacancies involved in CO2 adsorption and methanol formation. The rest of Al is present as small Al2O3 domains at the In2O3 surface, blocking the active sites for CO2 hydrogenation and contributing to higher CO selectivity. At higher Al content (≥10 mol %
Al), the particle size of In2O3 decreases due to the stabilizing effect of
Al2O3. Nevertheless, these smaller particles are prone to sintering during
CO2 hydrogenation since they appear to be more easily reduced. These findings show subtle effects of a structural promoter such as
Al on the reducibility and texture of In2O3 as a CO2 hydrogenation catalyst.

Original language	English
Pages (from-to)	15730-15745
Number of pages	16
Journal	ACS Catalysis
Volume	13
Issue number	24
DOIs	https://doi.org/10.1021/acscatal.3c04620
Publication status	Published - 15 Dec 2023

Funding

This work was supported by The Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC), an NWO Gravitation programme funded by the Ministry of Education, Culture and Science of the government of The Netherlands. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska Curie grant agreement No. 801359. Rim C. J. van de Poll is acknowledged for carrying out the TEM measurements. For TEM analysis (Titan microscopy), we acknowledge support from the Kavli Institute of Nanoscience, Delft University of Technology, and the Netherlands Electron Microscopy Infrastructure (NEMI), project number 184.034.014, part of the National Roadmap and financed by the Dutch Research Council (NWO).

Funders	Funder number
Netherlands Center for Multiscale Catalytic Energy Conversion
European Union's Horizon 2020 - Research and Innovation Framework Programme	801359
Kavli Nanoscience Institute, California Institute of Technology
Delft University of Technology	184.034.014
Ministerie van Onderwijs, Cultuur en Wetenschap
Nederlandse Organisatie voor Wetenschappelijk Onderzoek

Keywords

CO2 hydrogenation
In2O3
methanol
doping
aluminum
CO hydrogenation
In O

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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title = "Al Promotion of In2O3 for CO2 Hydrogenation to Methanol",

abstract = "In2O3 is a promising catalyst for the hydrogenation of CO2 to methanol, relevant to renewable energy storage in chemicals. Herein, we investigated the promoting role of Al on In2O3 using flame spray pyrolysis to prepare a series of In2O3−Al2O3 samples in a single step (0−20 mol \% Al). Al promoted the methanol yield, with an optimum being observed at an Al content of 5 mol \%. Extensive characterization showed that Al can dope into the In2O3 lattice (maximum ∼ 1.2 mol \%), leading to the formation of more oxygen vacancies involved in CO2 adsorption and methanol formation. The rest of Al is present as small Al2O3 domains at the In2O3 surface, blocking the active sites for CO2 hydrogenation and contributing to higher CO selectivity. At higher Al content (≥10 mol \% Al), the particle size of In2O3 decreases due to the stabilizing effect of Al2O3. Nevertheless, these smaller particles are prone to sintering during CO2 hydrogenation since they appear to be more easily reduced. These findings show subtle effects of a structural promoter such as Al on the reducibility and texture of In2O3 as a CO2 hydrogenation catalyst.",

keywords = "CO2 hydrogenation, In2O3, methanol, doping, aluminum, CO hydrogenation, In O",

author = "Liang Liu and Brahim Mezari and Kosinov, \{Nikolay A.\} and Hensen, \{Emiel J.M.\}",

year = "2023",

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doi = "10.1021/acscatal.3c04620",

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AU - Liu, Liang

AU - Mezari, Brahim

AU - Kosinov, Nikolay A.

AU - Hensen, Emiel J.M.

PY - 2023/12/15

Y1 - 2023/12/15

N2 - In2O3 is a promising catalyst for the hydrogenation of CO2 to methanol, relevant to renewable energy storage in chemicals. Herein, we investigated the promoting role of Al on In2O3 using flame spray pyrolysis to prepare a series of In2O3−Al2O3 samples in a single step (0−20 mol % Al). Al promoted the methanol yield, with an optimum being observed at an Al content of 5 mol %. Extensive characterization showed that Al can dope into the In2O3 lattice (maximum ∼ 1.2 mol %), leading to the formation of more oxygen vacancies involved in CO2 adsorption and methanol formation. The rest of Al is present as small Al2O3 domains at the In2O3 surface, blocking the active sites for CO2 hydrogenation and contributing to higher CO selectivity. At higher Al content (≥10 mol % Al), the particle size of In2O3 decreases due to the stabilizing effect of Al2O3. Nevertheless, these smaller particles are prone to sintering during CO2 hydrogenation since they appear to be more easily reduced. These findings show subtle effects of a structural promoter such as Al on the reducibility and texture of In2O3 as a CO2 hydrogenation catalyst.

AB - In2O3 is a promising catalyst for the hydrogenation of CO2 to methanol, relevant to renewable energy storage in chemicals. Herein, we investigated the promoting role of Al on In2O3 using flame spray pyrolysis to prepare a series of In2O3−Al2O3 samples in a single step (0−20 mol % Al). Al promoted the methanol yield, with an optimum being observed at an Al content of 5 mol %. Extensive characterization showed that Al can dope into the In2O3 lattice (maximum ∼ 1.2 mol %), leading to the formation of more oxygen vacancies involved in CO2 adsorption and methanol formation. The rest of Al is present as small Al2O3 domains at the In2O3 surface, blocking the active sites for CO2 hydrogenation and contributing to higher CO selectivity. At higher Al content (≥10 mol % Al), the particle size of In2O3 decreases due to the stabilizing effect of Al2O3. Nevertheless, these smaller particles are prone to sintering during CO2 hydrogenation since they appear to be more easily reduced. These findings show subtle effects of a structural promoter such as Al on the reducibility and texture of In2O3 as a CO2 hydrogenation catalyst.

KW - CO2 hydrogenation

KW - In2O3

KW - methanol

KW - doping

KW - aluminum

KW - CO hydrogenation

KW - In O

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DO - 10.1021/acscatal.3c04620

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JO - ACS Catalysis

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ER -

Al Promotion of In2O3 for CO2 Hydrogenation to Methanol

Abstract

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Keywords

UN SDGs

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