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Low-Temperature Hydrogenation of CO2 to Methanol in Water on ZnO-Supported CuAu Nanoalloys

Mosrati, Jawaher ; Ishida, Tamao ; Mac, Hung ; Al-Yusufi, Mohammed ; Honma, Tetsuo ; Parliniska-Wojtan, Magdalena ; Kobayashi, Yasuhiro ; Klyushin, Alexander LU ; Murayama, Toru and Abdel-Mageed, Ali M. (2023) In Angewandte Chemie - International Edition 62(51).
Abstract

Optimizing processes and materials for the valorization of CO2 to hydrogen carriers or platform chemicals is a key step for mitigating global warming and for the sustainable use of renewables. We report here on the hydrogenation of CO2 in water on ZnO-supported CuAu nanoalloys, based on ≤7 mol % Au. CuxAuy/ZnO catalysts were characterized using 197Au Mössbauer, in situ X-ray absorption (Au LIII- and Cu K-edges), and ambient pressure X-ray photoelectron (APXP) spectroscopic methods together with X-ray diffraction and high-resolution electron microscopy. At 200 °C, the conversion of CO2 showed a significant increase by 34 times (from 0.1 to 3.4 %) upon increasing... (More)

Optimizing processes and materials for the valorization of CO2 to hydrogen carriers or platform chemicals is a key step for mitigating global warming and for the sustainable use of renewables. We report here on the hydrogenation of CO2 in water on ZnO-supported CuAu nanoalloys, based on ≤7 mol % Au. CuxAuy/ZnO catalysts were characterized using 197Au Mössbauer, in situ X-ray absorption (Au LIII- and Cu K-edges), and ambient pressure X-ray photoelectron (APXP) spectroscopic methods together with X-ray diffraction and high-resolution electron microscopy. At 200 °C, the conversion of CO2 showed a significant increase by 34 times (from 0.1 to 3.4 %) upon increasing Cu93Au7 loading from 1 to 10 wt %, while maintaining methanol selectivity at 100 %. Limited CO selectivity (4–6 %) was observed upon increasing temperature up to 240 °C but associated with a ≈3-fold increase in CO2 conversion. Based on APXPS during CO2 hydrogenation in an H2O-rich mixture, Cu segregates preferentially to the surface in a mainly metallic state, while slightly charged Au submerges deeper into the subsurface region. These results and detailed structural analyses are topics of the present contribution.

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author
; ; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
APXPS, CO Reduction in Water, Cuau Nanoalloys, Green Methanol, Mössbauer Spectroscopy
in
Angewandte Chemie - International Edition
volume
62
issue
51
article number
e202311340
publisher
John Wiley & Sons Inc.
external identifiers
  • scopus:85176408772
  • pmid:37856669
ISSN
1433-7851
DOI
10.1002/anie.202311340
language
English
LU publication?
yes
id
8409c01f-5a32-4615-b849-1d75d0bb651b
date added to LUP
2024-01-11 10:03:32
date last changed
2024-11-23 04:21:45
@article{8409c01f-5a32-4615-b849-1d75d0bb651b,
  abstract     = {{<p>Optimizing processes and materials for the valorization of CO<sub>2</sub> to hydrogen carriers or platform chemicals is a key step for mitigating global warming and for the sustainable use of renewables. We report here on the hydrogenation of CO<sub>2</sub> in water on ZnO-supported CuAu nanoalloys, based on ≤7 mol % Au. Cu<sub>x</sub>Au<sub>y</sub>/ZnO catalysts were characterized using <sup>197</sup>Au Mössbauer, in situ X-ray absorption (Au L<sub>III</sub>- and Cu K-edges), and ambient pressure X-ray photoelectron (APXP) spectroscopic methods together with X-ray diffraction and high-resolution electron microscopy. At 200 °C, the conversion of CO<sub>2</sub> showed a significant increase by 34 times (from 0.1 to 3.4 %) upon increasing Cu<sub>93</sub>Au<sub>7</sub> loading from 1 to 10 wt %, while maintaining methanol selectivity at 100 %. Limited CO selectivity (4–6 %) was observed upon increasing temperature up to 240 °C but associated with a ≈3-fold increase in CO<sub>2</sub> conversion. Based on APXPS during CO<sub>2</sub> hydrogenation in an H<sub>2</sub>O-rich mixture, Cu segregates preferentially to the surface in a mainly metallic state, while slightly charged Au submerges deeper into the subsurface region. These results and detailed structural analyses are topics of the present contribution.</p>}},
  author       = {{Mosrati, Jawaher and Ishida, Tamao and Mac, Hung and Al-Yusufi, Mohammed and Honma, Tetsuo and Parliniska-Wojtan, Magdalena and Kobayashi, Yasuhiro and Klyushin, Alexander and Murayama, Toru and Abdel-Mageed, Ali M.}},
  issn         = {{1433-7851}},
  keywords     = {{APXPS; CO Reduction in Water; Cuau Nanoalloys; Green Methanol; Mössbauer Spectroscopy}},
  language     = {{eng}},
  month        = {{12}},
  number       = {{51}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Angewandte Chemie - International Edition}},
  title        = {{Low-Temperature Hydrogenation of CO<sub>2</sub> to Methanol in Water on ZnO-Supported CuAu Nanoalloys}},
  url          = {{http://dx.doi.org/10.1002/anie.202311340}},
  doi          = {{10.1002/anie.202311340}},
  volume       = {{62}},
  year         = {{2023}},
}