Boosting Hydrogenation of CO2 Using Cationic Cu Atomically Dispersed on 2D γ‐Al2O3 Nanosheets

Chen, Ping; Zhu, Yifeng; Zhang, Hailin; Prange, Micah P.; Song, Duo; Szanyi, Janos; Wang, Yining; Chen, Ying; Wang, Xiang; Gutiérrez, Oliver Y.; Zhu, Zihua; Wang, Zheming; Pearce, Carolyn I.; Li, Ping; Rosso, Kevin M.; Shi, Honghong; Zhang, Xin

doi:10.1002/anie.202505444

Title: Boosting Hydrogenation of CO₂ Using Cationic Cu Atomically Dispersed on 2D γ‐Al₂O₃ Nanosheets

Journal Article · Thu Apr 17 00:00:00 UTC 2025 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202505444 · OSTI ID:3028485

Chen, Ping ^[1]; Zhu, Yifeng ^[1]; Zhang, Hailin ^[2];

^[1]; Song, Duo ^[1]; Szanyi, Janos ^[1]; Wang, Yining ^[1];

^[1]; Wang, Xiang ^[1]; Gutiérrez, Oliver Y. ^[1];

^[1];

^[1]; Pearce, Carolyn I. ^[1]; Li, Ping ^[3];

^[1]; Shi, Honghong ^[1]; Zhang, Xin ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Chinese Academy of Sciences (CAS), Beijing (China)
Chinese Academy of Sciences (CAS), Beijing (China)

The continuous development of novel catalytic approaches is crucial for advancing efficient CO₂ 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-Al₂O₃ catalyst with high activity in the hydrogenation of CO₂-yielding methanol (CH₃OH), 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^P) sites on particle surfaces. This study demonstrates an efficient approach for achieving a high CO₂ hydrogenation rate (30.45 mol mol⁻¹ h⁻¹) 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-Al₂O₃) for CO and CH₃OH production. Ongoing mechanistic studies aim to elucidate the synergy between cationic Cu single atoms and γ-Al₂O₃, a Lewis acid support, in facilitating hydrogen (H₂) activation and methanol formation.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (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); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; AC05-76RL01830

OSTI ID:: 3028485

Report Number(s):: PNNL-SA-208548

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 25 Vol. 64; ISSN 1521-3773; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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2D catalyst
CO2 Hydrogenation
Cu/γ-Al2O3
Methanol
Single-Atom Catalysis

Title: Boosting Hydrogenation of CO2 Using Cationic Cu Atomically Dispersed on 2D γ‐Al2O3 Nanosheets

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Title: Boosting Hydrogenation of CO₂ Using Cationic Cu Atomically Dispersed on 2D γ‐Al₂O₃ Nanosheets