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

DOI: 10.1016/j.cej.2022.135394

Authors: Hongman Sun (China University of Petroleum; Queen's University of Belfast) , Yu Zhang (China University of Petroleum) , Chunfen Wang (China University of Petroleum) , Mark A. Isaacs (University College London; Harwell XPS, Research Complex at Harwell) , Ahmed I. Osman (Queen's University Belfast) , Yehong Wang (Dalian Institute of Chemical Physics, Chinese Academy of Sciences) , David Rooney (Queen's University Belfast) , Youhe Wang (China University of Petroleum) , Zifeng Yan (China University of Petroleum) , Christopher M. A. Parlett (University of Manchester; Diamond Light Source; The University of Manchester at Harwell; UK Catalysis Hub, Research Complex at Harwell) , Feng Wang (Dalian Institute of Chemical Physics, Chinese Academy of Sciences) , Chunfei Wu (Queen's University Belfast)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Chemical Engineering Journal , VOL 437

State: Published (Approved)
Published: June 2022
Diamond Proposal Number(s): 19850

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.

Journal Keywords: Sub-nanometer catalysts; Oxygen vacancies; Carbon capture; Methane; CeO2

Diamond Keywords: Carbon Capture and Storage (CCS)

Subject Areas: Chemistry, Materials, Environment


Instruments: B18-Core EXAFS

Added On: 01/03/2022 09:46

Discipline Tags:

Earth Sciences & Environment Climate Change Physical Chemistry Catalysis Chemistry Materials Science Chemical Engineering Engineering & Technology

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS)