Decentralized and sustainable methanol synthesis from co2 hydrogenation over cu-based catalysts

Hu, Zonggao 2025. Decentralized and sustainable methanol synthesis from co2 hydrogenation over cu-based catalysts. PhD Thesis, Cardiff University. Item availability restricted.

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Abstract

To prepare a novel, efficient low-Cu-content supported Cu-based catalyst for decentralized and sustainable methanol synthesis from CO2 hydrogenation, a γ-Al2O3 supported Cu catalyst was prepared via sol-immobilization. This catalyst exhibited high activity but low methanol selectivity. Subsequently, the influence of Zn, three introduction routes, and a range of Zn/Cu ratios were investigated, and the resultant Cu-Zn catalysts showed different properties and thereby distinct performances. The different sources of γ-Al2O3 with different specific surface areas were also compared, and larger specific surface areas were not the critical factor in achieving high-performance Cu-Zn-based CO2-tomethanol catalysts. Single-site catalysts remain largely unexplored in CO2 hydrogenation to methanol. UiO-66 was used as the host material for Cu-based single-site catalysts. The significant effects of synthetic conditions (temperatures, the amount of acetic acid as a modulator, ligand-to-metal ratios) on the crystallinity, size, morphologies, defects of UiO-66 were confirmed. Two selected octahedral UiO-66 with different defects were employed to prepare Cu-based single-site catalysts by impregnation followed by thermal reduction, and the Cu/UiO-66 with less defects showed better catalytic performance than the Cu/UiO-66 with more defects and other four UiO-66-based Cu nanocatalysts obtained by different thermal treatment routes. UiO-66 can serve as a template to generate atypical octahedral ZrO2 by thermal decomposition. The Cu-Zn nanocatalysts supported on the UiO-66-derived tZrO2 were synthesized by sol-immobilization, and exhibited outstanding methanol productivity comparable to those of the optimized CuZn/γ-Al2O3 and the commercial Cu/ZnO/Al2O3 catalyst. The t-ZrO2 with a larger specific surface area, prepared via precipitation, supported Cu-Zn catalyst demonstrated much lower methanol productivity at a comparable CuZn loading.

Item Type:	Thesis (PhD)
Date Type:	Completion
Status:	Unpublished
Schools:	Schools > Chemistry
Date of First Compliant Deposit:	14 October 2025
Last Modified:	14 Oct 2025 14:30
URI:	https://orca.cardiff.ac.uk/id/eprint/181656

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