Inverse ZrO2/Cu as a highly efficient methanol synthesis catalyst from CO2 hydrogenation

Congyi Wu, Lili Lin (), Jinjia Liu, Jingpeng Zhang, Feng Zhang, Tong Zhou, Ning Rui, Siyu Yao, Yuchen Deng, Feng Yang, Wenqian Xu, Jun Luo, Yue Zhao, Binhang Yan, Xiao-Dong Wen (), José A. Rodriguez () and Ding Ma ()
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Congyi Wu: College of Chemistry and Molecular Engineering and College of Engineering and BIC-ESAT Peking University
Lili Lin: College of Chemistry and Molecular Engineering and College of Engineering and BIC-ESAT Peking University
Jinjia Liu: Chinese Academy of Sciences
Jingpeng Zhang: Tsinghua University
Feng Zhang: State University of New York at Stony Brook
Tong Zhou: Tianjin University of Technology
Ning Rui: Brookhaven National Laboratory
Siyu Yao: Brookhaven National Laboratory
Yuchen Deng: College of Chemistry and Molecular Engineering and College of Engineering and BIC-ESAT Peking University
Feng Yang: College of Chemistry and Molecular Engineering and College of Engineering and BIC-ESAT Peking University
Wenqian Xu: Argonne National Laboratory, Argonne
Jun Luo: Tianjin University of Technology
Yue Zhao: College of Chemistry and Molecular Engineering and College of Engineering and BIC-ESAT Peking University
Binhang Yan: Tsinghua University
Xiao-Dong Wen: Chinese Academy of Sciences
José A. Rodriguez: Brookhaven National Laboratory
Ding Ma: College of Chemistry and Molecular Engineering and College of Engineering and BIC-ESAT Peking University

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract Enhancing the intrinsic activity and space time yield of Cu based heterogeneous methanol synthesis catalysts through CO2 hydrogenation is one of the major topics in CO2 conversion into value-added liquid fuels and chemicals. Here we report inverse ZrO2/Cu catalysts with a tunable Zr/Cu ratio have been prepared via an oxalate co-precipitation method, showing excellent performance for CO2 hydrogenation to methanol. Under optimal condition, the catalyst composed by 10% of ZrO2 supported over 90% of Cu exhibits the highest mass-specific methanol formation rate of 524 gMeOHkgcat−1h−1 at 220 °C, 3.3 times higher than the activity of traditional Cu/ZrO2 catalysts (159 gMeOHkgcat−1h−1). In situ XRD-PDF, XAFS and AP-XPS structural studies reveal that the inverse ZrO2/Cu catalysts are composed of islands of partially reduced 1–2 nm amorphous ZrO2 supported over metallic Cu particles. The ZrO2 islands are highly active for the CO2 activation. Meanwhile, an intermediate of formate adsorbed on the Cu at 1350 cm−1 is discovered by the in situ DRIFTS. This formate intermediate exhibits fast hydrogenation conversion to methoxy. The activation of CO2 and hydrogenation of all the surface oxygenate intermediates are significantly accelerated over the inverse ZrO2/Cu configuration, accounting for the excellent methanol formation activity observed.

Date: 2020
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DOI: 10.1038/s41467-020-19634-8

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