超临界水中金属氢氧化物催化重油改质：氘示踪研究,Energy & Fuels

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超临界水中金属氢氧化物催化重油改质：氘示踪研究
Energy & Fuels ( IF 5.2 ) Pub Date : 2024-03-05 , DOI: 10.1021/acs.energyfuels.4c00100
Zhong Chen _{1,

2} , Qiao Chen _{1,

2} , Dongyuan Li ₃ , Yi Zhong _{1,

2} , Hongzhen Chen _{1,

2} , Wei Peng ₄

Affiliation

重油的转化迫在眉睫，因为大多数已勘探的化石石油储量和可再生的生物柴油原料都可以归类为重油。超临界水改质（SCWU）是一种绿色、有前景的重油转化技术，但纯水的供氢能力不足。该研究首次采用过渡金属氢氧化物（M-OH）来增强水的原位供氢能力。测试了 M-OH 以及一种后过渡金属 (Al) 和五种过渡金属 (Cr、Cu、Fe、Ni、Zn) 的相应金属氧化物纳米颗粒 (MO _n )。 SCWU条件选择为425 ℃、60 min、水油比4:1、催化剂油比1:10、水密度308 kg m ^–3。使用氧化氘 (D ₂ O) 代替 H ₂ O 作为氘示踪研究的反应介质。结果表明，不同的金属基MO _n纳米粒子对重烃裂解、气化、抑焦和D 加成反应表现出不同的效果。发现总体性能的顺序为NiO > Cr ₂ O ₃ > Fe ₂ O ₃ > CuO > Al ₂ O ₃ > ZnO。与MO _n相比，M-OH 通常可以提高油收率和H/C 比，同时降低焦炭收率。机理分析表明，水热条件下的M-OH分解行为是富油相中生成MO _n和晶格H ₂ O的主要原因。晶格H ₂ O不仅可以参与SCWU反应，而且可以抑制焦炭的形成。总之，M-OH是一种很有前途的催化剂，因为它结合了MO _n纳米粒子良好的分散性和催化活性以及水溶性无机金属盐（M-IAc）的低成本，但不会产生任何腐蚀性物质，例如来自 M-IAc 的无机酸。

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Metal Hydroxide-Catalyzed Heavy Oil Upgrading in Supercritical Water: Deuterium Tracing Study

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 (MO_n) of one post-transition metal (Al) and five transition metals (Cr, Cu, Fe, Ni, Zn) are tested. The SCWU conditions are selected as 425 °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 MO_n 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 MO_n, 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 MO_n 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 MO_n 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.

更新日期：2024-03-05

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