Ultrasmall Cu Nanoparticles Supported on Crystalline, Mesoporous ZnO for Selective CO ₂ Hydrogenation

Journal Article · Wed Dec 20 00:00:00 EST 2023 · ChemCatChem

DOI:https://doi.org/10.1002/cctc.202301077· OSTI ID:2246983

Hu, Mingzhen ^[1]; Lu, Xingxu ^[2]; Zhu, Chunxiang ^[2]; Yang, Tiangang ^[1]; Tan, Haiyan ^[3]; Jin, Lei ^[1]; Kerns, Peter ^[1]; Meng, Michael ^[1]; Suib, Steven L. ^[4]; Gao, Puxian ^[5]; He, Jie  ^[6]

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1. Department of Chemistry University of Connecticut Storrs, Connecticut 06269 USA
2. Department of Materials Science and Engineering University of Connecticut Storrs, Connecticut 06269 USA
3. Institute of Materials Science University of Connecticut Storrs, Connecticut 06269 USA
4. Department of Chemistry University of Connecticut Storrs, Connecticut 06269 USA, Department of Materials Science and Engineering University of Connecticut Storrs, Connecticut 06269 USA, Institute of Materials Science University of Connecticut Storrs, Connecticut 06269 USA
5. Department of Materials Science and Engineering University of Connecticut Storrs, Connecticut 06269 USA, Institute of Materials Science University of Connecticut Storrs, Connecticut 06269 USA
6. Department of Chemistry University of Connecticut Storrs, Connecticut 06269 USA, Institute of Materials Science University of Connecticut Storrs, Connecticut 06269 USA

Abstract Converting CO ₂ to value‐added chemicals, e. g ., CH ₃ OH, is highly desirable in terms of the carbon cycling while reducing CO ₂ emission from fossil fuel combustion. Cu‐based nanocatalysts are among the most efficient for selective CO ₂ ‐to‐CH ₃ OH transformation; this conversion, however, suffers from low reactivity especially in the thermodynamically favored low temperature range. We herein report ultrasmall copper (Cu) nanocatalysts supported on crystalline, mesoporous zinc oxide nanoplate (Cu@ m ZnO) with notable activity and selectivity of CO ₂ ‐to‐CH ₃ OH in the low temperature range of 200–250 °C. Cu@ m ZnO nanoplates are prepared based on the crystal‐crystal transition of mixed Cu and Zn basic carbonates to mesoporous metal oxides and subsequent hydrogen reduction. Under the nanoconfinement of mesopores in crystalline ZnO frameworks, ultrasmall Cu nanoparticles with an average diameter of 2.5 nm are produced. Cu@ m ZnO catalysts have a peak CH ₃ OH formation rate of 1.13 mol h ⁻¹ per 1 kg under ambient pressure at 246 °C, about 25 °C lower as compared to that of the benchmark catalyst of Cu−Zn−Al oxides. Our new synthetic strategy sheds some valuable insights into the design of porous catalysts for the important conversion of CO ₂ ‐to‐CH ₃ OH.

• Sponsoring Organization: USDOE
• Grant/Contract Number: EE0008423
• OSTI ID: 2246983
• Journal Information: ChemCatChem, Journal Name: ChemCatChem Vol. 16 Journal Issue: 3; ISSN 1867-3880
• Publisher: Wiley Blackwell (John Wiley & Sons)
• Country of Publication: Germany
• Language: English