Promoting Hydrodeoxygenation of Inedible Biolipids Via Coking and Sintering Resistant Co-Loaded ZrO2–SiO2 Dual-Support Catalyst

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2025-07-11 DOI:10.1007/s10562-025-05108-3

Jiaqi Yan, Haojie Zhang, Jing Guo, Zhiyong Yang, Yongfei Li

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引用次数: 0

Abstract

Deoxygenation of various fatty acid methyl esters (FAMEs) and inedible biolipids to diesel-range alkanes was investigated over an efficient dual-supported Co-based catalyst (Co/Zr_n–SiO₂). The combination of SiO₂ and ZrO₂ dual-support improves the catalytic performance and reduces the apparent activation energy of the Co-based catalyst, with three advantages: (i) both the high surface area of SiO₂ and the encapsulating effect of ZrO₂ favor the formation of smaller Co nanoparticles and fine dispersion, which in turn reduces coke deposition; (ii) incorporating oxyphilic Zr increases the content of Co⁰ while also improving the electron density of Co and the ratio of oxygen deficient (O_D), which is favorable for the dissociation of H₂ and adsorption of C=O/C–O bonds; (iii) hydroxyl-rich SiO₂ and abundant ZrO_x−O_D−Co interfaces synergistically promote the hydrodeoxygenation (HDO) and suppress the decarbonylation (–CO)/decarboxylation (–COO) pathways, effectively preventing carbon loss. The Co/Zr_0.25–SiO₂ with 10 wt% Co and 0.25 Zr/Si molar ratio is used for the deoxygenation of methyl palmitate, yielding 97.6% selectivity towards diesel-range alkanes, with 85.1% hexadecane at full MP conversion. Complex inedible biolipids such as jatropha oil and waste cooking oil can be easily transformed into diesel-range alkanes with a selectivity of 93.9% and 91.6%, respectively. Furthermore, the catalyst shows stable recyclability in the current catalytic deoxygenation system.

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通过抗焦化和烧结共负载ZrO2-SiO2双负载催化剂促进不可食用生物脂的加氢脱氧

研究了多种脂肪酸甲酯（FAMEs）和不可食用生物脂在高效双负载Co基催化剂（Co/ Zrn-SiO2）上脱氧制柴油烷烃。SiO2和ZrO2双载体的组合提高了Co基催化剂的催化性能，降低了Co基催化剂的表观活化能，具有以下三个优点：(1)SiO2的高表面积和ZrO2的包封作用有利于形成更小的Co纳米颗粒和精细分散，从而减少了焦炭的沉积；（ii）加入亲氧性的Zr增加了Co0的含量，同时提高了Co的电子密度和缺氧率（OD），有利于H2的解离和C=O/C - O键的吸附；（iii）富含羟基的SiO2和丰富的ZrOx - OD -CO界面协同促进氢脱氧（HDO），抑制脱羰(-CO)/脱羧（-COO）途径，有效防止碳损失。Co/ Zr0.25-SiO2 （Co质量分数为10 wt%， Zr/Si质量分数为0.25）用于棕榈酸甲酯的脱氧，对柴油烷烃的选择性为97.6%，对十六烷的选择性为85.1%。麻疯树油和废食用油等复杂的不可食用生物脂可以很容易地转化为柴油级烷烃，选择性分别为93.9%和91.6%。此外，该催化剂在现有的催化脱氧体系中表现出稳定的可回收性。

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.