XAS/DRIFTS/MS spectroscopy for time-resolved operando study of integrated carbon capture and utilisation process

Hongman Sun, Chunfen Wang, Shuzhuang Sun, Antonio T. Lopez, Youhe Wang, Jingbin Zeng, Zhen Liu, Zifeng Yan, Christopher M.A. Parlett*, Chunfei Wu

*Corresponding author for this work

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Abstract

An integrated carbon capture and utilization (ICCU) process present an ideal solution to address anthropogenic carbon dioxide (CO2) emissions from fossil fuel-driven electricity production, allowing for capturing and subsequent utilization of CO2 instead of current release into the atmosphere. Effective dual-functional materials (DFMs), through the combination of CO2 sorbents and catalysts, can not only capture CO2 but also convert it into higher-value chemicals, such as CH4 or CO, under isothermal conditions within a single reactor are highly desirable for ICCU processes. In this study, we investigate the mechanism of ICCU over 10 %NiCaO by the time-resolved operando XAS/DRIFTS/MS and the influence of a reduction pretreatment on the process and the products formed. During the 1st stage of the ICCU process (carbon capture), CaO adsorbs CO2 resulting in bicarbonate, carbonate, and formate species formation. At the same time, the Ni catalytic active species are oxidized by CO2, leading to the formation of NiO and CO. However, pre-treating the same DFM under hydrogen, during heating to operating temperature, resulted in a switch to CH4 production, suggesting the presence of high levels of surface adsorbed H2. During the 2nd stage of ICCU (CO2 conversion), the NiO generated during capture is reduced by H2 to metallic Ni, which facilitates the reduction of bicarbonates, carbonates, and formats, via H2 dissociation, to produce and liberate gaseous CO. Thus, both adsorption and catalytic sites are regenerated for the subsequent ICCU cycle.

Original languageEnglish
Article number121622
JournalSeparation and Purification Technology
Volume298
Early online date05 Jul 2022
DOIs
Publication statusPublished - 01 Oct 2022

Bibliographical note

Funding Information:
This project has received funding from the National Natural Science Foundation of China (22102215), Fundamental Research Funds for the Central Universities (21CX06013A) and Key Project of China National Key R&D Plan (2018YFE0118200). This work was financially supported by State Key Laboratory of Heavy Oil Processing, European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement (823745). The authors acknowledge the Diamond Light Source for the awarding of beamtime on the I20-EDE beamline (SP23645-1) and UK Catalysis Hub for access and support to the facilities and equipment for the operando XAS/DRIFTS measurements.

Funding Information:
This project has received funding from the National Natural Science Foundation of China (22102215), Fundamental Research Funds for the Central Universities (21CX06013A) and Key Project of China National Key R&D Plan (2018YFE0118200). This work was financially supported by State Key Laboratory of Heavy Oil Processing, European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement (823745). The authors acknowledge the Diamond Light Source for the awarding of beamtime on the I20-EDE beamline (SP23645-1) and UK Catalysis Hub for access and support to the facilities and equipment for the operando XAS/DRIFTS measurements.

Publisher Copyright:
© 2022 The Authors

Keywords

  • CaO
  • Dual-functional materials
  • Integrated carbon capture and utilisation
  • Mechanism
  • Operando XAS/DRIFTS/MS

ASJC Scopus subject areas

  • Analytical Chemistry
  • Filtration and Separation

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