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<p>Methanol synthesis via non-thermal plasma (NTP) catalytic CO<sub>2</sub> hydrogenation provides a sustainable approach to chemical and fuel production with potential in carbon emissions reduction. However, the underlying mechanisms remain unclear. Here we evaluate the mechanism of NTP-catalytic CO<sub>2</sub> hydrogenation over Cu–Zn/ZSM-5 through operando X-ray absorption spectroscopy, diffuse reflectance infrared Fourier transform spectroscopy and in situ X-ray pair distribution function. We found that Zn enhances Cu dispersion and reducibility, as well as forming active Cu/ZnO interfacial sites. Beyond the conventional formate pathway on metallic Cu, these interfaces enable an additional CO hydrogenation route, enhancing methanol yield. NTP also promotes gas-phase CO<sub>2</sub> dissociation to CO, bypassing the reverse water–gas shift step required in thermal catalysis. No Cu/Zn alloy formation was observed, underscoring the importance of metallic Cu and Cu/ZnO interfaces under NTP conditions. Furthermore, NTP stabilizes reduced Cu species, preventing re-oxidation and ensuring sustained catalytic activity. These findings advance the mechanistic understanding of NTP-assisted catalysis.</p><p></p>

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Unveiling active sites and the cooperative role of non-thermal plasma and copper–zinc catalysts in the hydrogenation of CO2 to methanol

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月13日

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  • Shanshan Xu,
  • Matthew E. Potter,
  • Raquel Simancas,
  • Lucy Costley-Wood,
  • Boya Qiu,
  • Xuzhao Liu,
  • Cristina Stere,
  • M. Asunción Molina,
  • Danial Farooq,
  • Floriana Tuna,
  • Dingyue Zhang,
  • Shuanglin Zhang,
  • Huanhao Chen,
  • Shengzhe Ding,
  • Xinrui Wang,
  • Sarayute Chansai,
  • Matthew Lindley,
  • Sarah J. Haigh,
  • Armando Ibraliu,
  • Lan Lan,
  • Piu Chawdhury,
  • Mariyam Bi,
  • Otis Leahair,
  • Yilai Jiao,
  • Min Hu,
  • Qiang Liu,
  • Toru Wakihara,
  • Xiaolei Fan,
  • Andrew M. Beale,
  • Christopher Hardacre

摘要

Methanol synthesis via non-thermal plasma (NTP) catalytic CO2 hydrogenation provides a sustainable approach to chemical and fuel production with potential in carbon emissions reduction. However, the underlying mechanisms remain unclear. Here we evaluate the mechanism of NTP-catalytic CO2 hydrogenation over Cu–Zn/ZSM-5 through operando X-ray absorption spectroscopy, diffuse reflectance infrared Fourier transform spectroscopy and in situ X-ray pair distribution function. We found that Zn enhances Cu dispersion and reducibility, as well as forming active Cu/ZnO interfacial sites. Beyond the conventional formate pathway on metallic Cu, these interfaces enable an additional CO hydrogenation route, enhancing methanol yield. NTP also promotes gas-phase CO2 dissociation to CO, bypassing the reverse water–gas shift step required in thermal catalysis. No Cu/Zn alloy formation was observed, underscoring the importance of metallic Cu and Cu/ZnO interfaces under NTP conditions. Furthermore, NTP stabilizes reduced Cu species, preventing re-oxidation and ensuring sustained catalytic activity. These findings advance the mechanistic understanding of NTP-assisted catalysis.