在掺氮碳-氧化铝杂化支撑钴催化剂上催化生物油升级,选择性生产高价值燃料。

IF 9.7 1区 环境科学与生态学 Q1 AGRICULTURAL ENGINEERING Bioresource Technology Pub Date : 2024-06-29 DOI:10.1016/j.biortech.2024.131059
Qin Peng, Xia Jiang, Guangmei Cao, Tianqiao Xie, Ziheng Jin, Lingling Xie, Fengli Gan, Shenggui Ma, Mingming Peng
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引用次数: 0

摘要

生物质快速热解产生的生物油可以通过催化加氢脱氧(HDO)升级为汽油和柴油替代品。在此,通过混凝浴技术建立了新型氮掺杂碳氧化铝杂化支撑钴(Co/NCAn,n = 1、2.5、5)催化剂。优化后的 Co/NCA2.5 催化剂的愈创木酚转化率为 100%,对环己烷的选择性高(93.6%),脱氧度极高(97.3%)。其中,Co 和 NC 之间更强的结合能和更大的电荷转移促进了环己醇的形成,密度泛函理论计算揭示了这一点。此外,适量的路易斯酸位点增强了环己醇中 C-O 键的裂解,最终导致了对环己烷的显著选择性。最后,Co/NCA2.5 催化剂对粗生物油 HDO 中的高热值碳氢化合物燃料也表现出卓越的选择性(93.1%)。这项研究为掺杂 N 的氧化铝杂化催化剂用于高效 HDO 反应提供了理论依据。
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Selective production of high-value fuel via catalytic upgrading of bio-oil over nitrogen-doped carbon-alumina hybrid supported cobalt catalysts.

Bio-oil derived from biomass fast pyrolysis can be upgraded to gasoline and diesel alternatives by catalytic hydrodeoxygenation (HDO). Here, the novel nitrogen-doped carbon-alumina hybrid supported cobalt (Co/NCAn, n = 1, 2.5, 5) catalyst is established by a coagulation bath technique. The optimized Co/NCA2.5 catalyst presented 100 % conversion of guaiacol, high selectivity to cyclohexane (93.6 %), and extremely high deoxygenation degree (97.3 %), respectively. Therein, the formation of cyclohexanol was facilitated by stronger binding energy and greater charge transfer between Co and NC which was unraveled by density functional theory calculations. In addition, the appropriate amount of Lewis acid sites enhanced the cleavage of the C-O bond in cyclohexanol, finally resulting in a remarkable selectivity for cyclohexane. Finally, the Co/NCA2.5 catalyst also exhibited excellent selectivity (93.1 %) for high heating value hydrocarbon fuel in crude bio-oil HDO. This work provides a theoretical basis on N dopants collaborating alumina hybrid catalysts for efficient HDO reaction.

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来源期刊
Bioresource Technology
Bioresource Technology 工程技术-能源与燃料
CiteScore
20.80
自引率
19.30%
发文量
2013
审稿时长
12 days
期刊介绍: Bioresource Technology publishes original articles, review articles, case studies, and short communications covering the fundamentals, applications, and management of bioresource technology. The journal seeks to advance and disseminate knowledge across various areas related to biomass, biological waste treatment, bioenergy, biotransformations, bioresource systems analysis, and associated conversion or production technologies. Topics include: • Biofuels: liquid and gaseous biofuels production, modeling and economics • Bioprocesses and bioproducts: biocatalysis and fermentations • Biomass and feedstocks utilization: bioconversion of agro-industrial residues • Environmental protection: biological waste treatment • Thermochemical conversion of biomass: combustion, pyrolysis, gasification, catalysis.
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