Ni/support-CaO bifunctional combined materials for integrated CO2 capture and reverse water-gas shift reaction: Influence of different supports

Shuzhuang Sun, Chen Zhang, Shaoliang Guan, Shaojun Xu*, Paul T. Williams, Chunfei Wu

*Corresponding author for this work

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Abstract

Integrated CO2 capture and utilisation (ICCU) is a promising strategy for restricting carbon emissions and achieving carbon neutrality. Bifunctional combined materials (BCMs), containing adsorbents and active catalysts, are widely applied in this process. Producing syngas via reverse water–gas shift reaction (RWGS) and integrating with Fischer-Tropsch (F-T) synthesis is an attractive and valuable CO2 utilisation route. This work investigated a series of Ni/support-CaO BCMs (supports = ZrO2, TiO2, CeO2 and Al2O3) for the integrated CO2 capture and RWGS (ICCU-RWGS) process. The Ni/support-CaO BCMs were prepared by physically mixing various metal oxide supports loaded Ni with sol–gel derived CaO. The ICCU-RWGS performance (CO2 conversion, CO yield and CO generation rate) of these BCMs followed the order during tested conditions (550–750 °C): Ni/CeO2-CaO > Ni/TiO2-CaO > Ni/ZrO2-CaO > Ni/Al2O3-CaO. A comprehensive characterisation of Ni/support materials showed that Ni/CeO2 had the characteristics of stronger basicity, optimal Ni dispersion and improved NiO reducibility, which led to the outperforming ICCU-RWGS activity over Ni/CeO2-CaO (e.g. 56.1% CO2 conversion, 2.68 mmol g−1 CO yield and ∼100% CO selectivity at 650 °C). Furthermore, the Ni/CeO2-CaO BCM showed a stable, yet, self-optimising catalytic performance during the cyclic ICCU-RWGS reaction over 20 cycles. The TEM characterisation suggested that was ascribed to the volume expansion and shrinkage of CaO in the cyclic adsorption–desorption altering the distance between the adsorbent and Ni/CeO2, resulting in an enhanced CO2 conversion during the cycle.

Original languageEnglish
Article number121604
JournalSeparation and Purification Technology
Volume298
Early online date04 Jul 2022
DOIs
Publication statusPublished - 01 Oct 2022

Bibliographical note

Funding Information:
The authors gratefully acknowledge financial support from the China Scholarship Council (reference number: 201906450023). This project has received funding from the European Union's Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 823745. The UK Catalysis Hub is kindly thanked for the resources and support provided via our membership of the UK Catalysis Hub Consortium and funded by EPSRC grant: EP/R026939/1, EP/R026815/1, EP/R026645/1, EP/R027129/1 or EP/M013219/1(biocatalysis). The XPS data collection was performed at the EPSRC National Facility for XPS (‘HarwellXPS’), operated by Cardiff University and UCL, under contract No. PR16195.

Funding Information:
The authors gratefully acknowledge financial support from the China Scholarship Council (reference number: 201906450023 ). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No 823745 . The UK Catalysis Hub is kindly thanked for the resources and support provided via our membership of the UK Catalysis Hub Consortium and funded by EPSRC grant: EP/R026939/1, EP/R026815/1, EP/R026645/1, EP/R027129/1 or EP/M013219/1(biocatalysis). The XPS data collection was performed at the EPSRC National Facility for XPS (‘HarwellXPS’), operated by Cardiff University and UCL, under contract No. PR16195.

Publisher Copyright:
© 2022 The Authors

Keywords

  • Bifunctional combined materials
  • Integrated CO capture and utilisation
  • Reverse water-gas shift reaction

ASJC Scopus subject areas

  • Analytical Chemistry
  • Filtration and Separation

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