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	Metal Hydroxide-Catalyzed Heavy Oil Upgrading in Supercritical Water: Deuterium Tracing Study
	Chen, Zhong1,2; Chen, Qiao1,2; Li, Dongyuan3; Zhong, Yi1,2; Chen, Hongzhen1,2; Peng, Wei4
	2024-03-05
摘要	Conversion of heavy oil is urgent as most of the explored fossil oil reserves and renewable raw biodiesel can be categorized as heavy oil. Supercritical water upgrading (SCWU) is a green and promising technology for heavy oil conversion, but the hydrogen-donating capacity of pure water is inadequate. This study adopts transition-metal hydroxide (M-OH) to enhance the in situ hydrogen-donating capacity of water for the first time. Both M-OH and the corresponding metal oxide nanoparticle (MOn) of one post-transition metal (Al) and five transition metals (Cr, Cu, Fe, Ni, Zn) are tested. The SCWU conditions are selected as 425 degrees C, 60 min, water-to-oil ratio of 4:1, catalyst-to-oil ratio of 1:10, and water density of 308 kg m(-3). Deuterium oxide (D2O) instead of H2O is used as the reaction medium for a deuterium tracing study. Results indicate that the different metal-based MOn nanoparticles display various effects on heavy hydrocarbon cracking, gasification, coke suppression, and D addition reactions. The overall performance is found to be on the order of NiO > Cr2O3 > Fe2O3 > CuO > Al2O3 > ZnO. Compared to MOn, M-OH can generally improve the oil yield and H/C ratio and reduce the coke yield simultaneously. The mechanism analysis suggests that the M-OH decomposition behavior under hydrothermal conditions is the primary cause by which MOn and lattice H2O are generated in the oil-rich phase. The lattice H2O can not only take part in SCWU reactions but also suppress coke formation. In conclusion, M-OH is a promising catalyst as it combines the good dispersibility and catalytic activity of MOn nanoparticles and the low cost of water-soluble inorganic metal salts (M-IAc) but does not result in any corrosive species, such as inorganic acid from M-IAc.
DOI	10.1021/acs.energyfuels.4c00100
发表期刊	ENERGY & FUELS
ISSN	0887-0624
卷号	38期号:7页码:5738-5750
通讯作者	Chen, Zhong(chenzhong@cigit.ac.cn)
收录类别	SCI
WOS记录号	WOS:001180388800001
语种	英语