Boosting Hydrogenation of CO <sub>2</sub> Using Cationic Cu Atomically Dispersed on 2D γ‐Al <sub>2</sub> O <sub>3</sub> Nanosheets
The continuous development of novel catalytic approaches is crucial for advancing efficient CO<sub>2</sub> hydrogenation processes. Drawing inspiration from single-atom catalysis and 2D materials, we designed a new 2D single-atom catalyst with excellent thermal stability by thermally treating Cu-adsorbed γ-AlOOH nanosheets, which yielded a Cu/γ-Al<sub>2</sub>O<sub>3</sub> catalyst with high activity in the hydrogenation of CO<sub>2</sub>-yielding methanol (CH<sub>3</sub>OH), dimethyl ether (DME), and CO as products. The active Cu sites are monodispersed and highly stable due to their cationic oxidation state and their substitution for pentacoordinated aluminum (Al<sup>P</sup>) sites on particle surfaces. This study demonstrates an efficient approach for achieving a high CO<sub>2</sub> hydrogenation rate (30.45 mol mol<sup>-1</sup> h<sup>-1</sup>) using a catalyst system that lacks metallic Cu centers, traditionally considered essential for H₂ dissociation, and employs what was previously thought to be an inert metal oxide (γ-Al<sub>2</sub>O<sub>3</sub>) for CO and CH<sub>3</sub>OH production. Ongoing mechanistic studies aim to elucidate the synergy between cationic Cu single atoms and γ-Al<sub>2</sub>O<sub>3</sub>, a Lewis acid support, in facilitating hydrogen (H<sub>2</sub>) activation and methanol formation.
Authors
- Honghong Shi (ORCID: https://orcid.org/0000-0002-9303-8344)
- Zihua Zhu (ORCID: https://orcid.org/0000-0001-5770-8462)
- Micah P. Prange (ORCID: https://orcid.org/0000-0002-0775-2024)
- Hai‐Lin Zhang (ORCID: https://orcid.org/0000-0002-7426-2885)
- Yifeng Zhu (ORCID: https://orcid.org/0000-0001-8965-5051)
- Oliver Y. Gutiérrez (ORCID: https://orcid.org/0000-0001-9163-4786)
- Duo Song (ORCID: https://orcid.org/0000-0002-5136-7959)
- János Szanyi (ORCID: https://orcid.org/0000-0002-8442-5465)
- Carolyn I. Pearce (ORCID: https://orcid.org/0000-0003-3098-1615)
- Kevin M. Rosso (ORCID: https://orcid.org/0000-0002-8474-7720)
- Xin Zhang (ORCID: https://orcid.org/0000-0003-4305-145X)
- Ying Chen
- Xiang Wang (ORCID: https://orcid.org/0000-0002-9629-3084)
- Ping Chen (ORCID: https://orcid.org/0000-0002-4527-4561)
- Yining Wang (ORCID: https://orcid.org/0000-0002-8180-1162)
- Ping Li (ORCID: https://orcid.org/0000-0002-2356-0962)
- Zhe-Ming Wang (ORCID: https://orcid.org/0000-0002-1986-4357)
Institutions
- Pacific Northwest National Laboratory (US)
- Environmental Molecular Sciences Laboratory (US)
- Institute of Process Engineering (CN)
- Institute of Physics (CN)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-04-17
- DOI
- https://doi.org/10.1002/anie.202505444
- Citations
- 7
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 3.62
Funders
- U.S. Department of Energy
- Battelle
- Office of Science
- Basic Energy Sciences
- Biological and Environmental Research
- Argonne National Laboratory
- Pacific Northwest National Laboratory