Ultra-thin ZrO2 overcoating on CuO-ZnO-Al2O3 catalyst by atomic layer deposition for improved catalytic performance of CO2 hydrogenation to dimethyl ether

Fan, Xiao; Jin, Baitang; He, Xiaoqing; Li, Shiguang; Liang, Xinhua

doi:10.1088/1361-6528/acc036

Ultra-thin ZrO₂ overcoating on CuO-ZnO-Al₂O₃ catalyst by atomic layer deposition for improved catalytic performance of CO₂ hydrogenation to dimethyl ether

Journal Article · Mon Mar 20 00:00:00 EDT 2023 · Nanotechnology

DOI:https://doi.org/10.1088/1361-6528/acc036· OSTI ID:1962454

Fan, Xiao ^[1]; Jin, Baitang ^[1]; He, Xiaoqing ^[2]; Li, Shiguang ^[3]; ^[4]

Missouri Univ. of Science and Technology, Rolla, MO (United States)
Univ. of Missouri, Columbia, MO (United States)
Gas Technology Institute, Des Plaines, IL (United States)
Missouri Univ. of Science and Technology, Rolla, MO (United States); Washington Univ., St. Louis, MO (United States)

An ultra-thin overcoating of zirconium oxide (ZrO₂) film on CuO-ZnO-Al₂O₃ (CZA) catalysts by atomic layer deposition (ALD) was proved to enhance the catalytic performance of CZA/HZSM-5 (H form of Zeolite Socony Mobil-5) bifunctional catalysts for hydrogenation of CO₂ to dimethyl ether (DME). Under optimal reaction conditions (i.e. 240 °C and 2.8 MPa), the yield of product DME increased from 17.22% for the bare CZA/HZSM-5 catalysts, to 18.40% for the CZA catalyst after 5 cycles of ZrO₂ ALD with HZSM-5 catalyst. All the catalysts modified by ZrO₂ ALD displayed significantly improved catalytic stability of hydrogenation of CO₂ to DME reaction, compared to that of CZA/HZSM-5 bifunctional catalysts. The loss of DME yield in 100 h of reaction was greatly mitigated from 6.20% (loss of absolute value) to 3.01% for the CZA catalyst with 20 cycles of ZrO₂ ALD overcoating. Characterizations including hydrogen temperature programmed reduction, x-ray powder diffraction, and x-ray photoelectron spectroscopy revealed that there was strong interaction between Cu active centers and ZrO₂.

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Research Organization:: Gas Technology Institute, Des Plaines, IL (United States)

Sponsoring Organization:: USDOE Advanced Research Projects Agency - Energy (ARPA-E); National Science Foundation (NSF)

Grant/Contract Number:: AR0000806; CBET 2306177

OSTI ID:: 1962454

Alternate ID(s):: OSTI ID: 1959272; OSTI ID: 2418410

Journal Information:: Nanotechnology, Vol. 34, Issue 23; ISSN 0957-4484

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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Ultra-thin ZrO2 overcoating on CuO-ZnO-Al2O3 catalyst by atomic layer deposition for improved catalytic performance of CO2 hydrogenation to dimethyl ether

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