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Integrated carbon capture and utilization: Synergistic catalysis between highly dispersed Ni clusters and ceria oxygen vacancies

Sun, H; Zhang, Y; Wang, C; Isaacs, MA; Osman, AI; Wang, Y; Rooney, D; ... Wu, C; + view all (2022) Integrated carbon capture and utilization: Synergistic catalysis between highly dispersed Ni clusters and ceria oxygen vacancies. Chemical Engineering Journal , 437 , Article 135394. 10.1016/j.cej.2022.135394. Green open access

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Abstract

Integrated carbon capture and utilization (ICCU) presents an ideal solution to address anthropogenic carbon dioxide (CO2) emissions from industry and energy sectors, facilitating CO2 capture and subsequent utilization through conversion into high-value chemicals, as opposed to current release into the atmosphere. Herein, we report the synergistic coupling of porous CaO, as a sorbent for CO2 capture, and Ni doped CeO2 nanorods, as catalytic sites for CO2 reduction. It is found that ceria is shown to possess the capacity for CO2 utilization, however, critically it only results in the generation of CO due to the weak CO-ceria bonding. The addition of Ni active sites gives rise to CH4 being the predominant product, via the strong interaction between Ni species and CO, which facilitates further reduction. Through tuning Ni loadings, we have evaluated the role of catalytic active site size, with a Ni loading of only 0.5 wt% providing optimal performance through the formation of sub-nanometer sized clusters. This near-atomic active site dispersion gives rise to CH4 productivity and selectivity of 1540 mmol g−1 Ni and 85.8%, respectively, with this optimal combination of catalyst and sorbent demonstrating high stability over 10 cycles of ICCU process. These observations in parallel with the synergistic coupling of earth-abundant, low-cost materials (CaO and Ni) will have broad implications on the design and implementation of high efficiency, cost-effective ICCU materials and processes.

Type: Article
Title: Integrated carbon capture and utilization: Synergistic catalysis between highly dispersed Ni clusters and ceria oxygen vacancies
Open access status: An open access version is available from UCL Discovery
DOI: 10.1016/j.cej.2022.135394
Publisher version: https://doi.org/10.1016/j.cej.2022.135394
Language: English
Additional information: © 2022 The Authors. Published by Elsevier B.V. under a Creative Commons license (https://creativecommons.org/licenses/by/4.0/).
Keywords: Sub-nanometer catalysts, Oxygen vacancies, Carbon capture, Methane, CeO2
UCL classification: UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL
URI: https://discovery.ucl.ac.uk/id/eprint/10154687
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