期刊
CHEMICAL ENGINEERING JOURNAL
卷 437, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.135394
关键词
Sub-nanometer catalysts; Oxygen vacancies; Carbon capture; Methane; CeO2
资金
- European Unions Horizon 2020 research and innovation programme under the Marie Sklo-dowska-Curie Grant [823745]
- FundamentalResearch Funds for the Central Universities [21CX06013A]
- National Natural Science Foundation of China [22025206, 21961130378, 22102215]
- Newton Advanced Fellowships [NAF\R1\191267]
- Ministry of Science and Technology of the Peoples Republic of China [2018YFE0117300]
- Key Projects of China National Key RD Plan [2018YFE0118200]
Integrated carbon capture and utilization (ICCU) presents an ideal solution for addressing CO2 emissions from industry and energy sectors. The coupling of porous CaO and Ni doped CeO2 nanorods facilitates CO2 capture and reduction, leading to high performance and stability. This has significant implications for the design and implementation of efficient and cost-effective ICCU materials and processes.
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 subnanometer 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.
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