In-situ synthesis of NiMo@SAPO-11 under mild conditions for the hydrodeoxygenation of triolein

IF 4.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2025-04-02 DOI:10.1016/j.mcat.2025.115076
Dejiang Zheng, Lu Li, Shitao Yu
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Abstract

Economical and sulphur-free Ni catalysts are attractive alternatives to hydrodeoxygenation (HDO) of fats and oils for the production of diesel-range paraffins, but are prone to decarbonylation/decarboxylation (DCOx) reactions. Metal oxide decorated nickel catalysts exhibit remarkably high catalytic activity, which can modify the nickel catalyzed deoxygenation reaction pathway. Herein, a series of NiMo@SAPO-11 catalysts with different Ni/Mo mass ratio were prepared using an in-situ synthesis under mild conditions (100 °C, 12 h). The as-synthesized bimetallic NiMo nanocatalyst with a Ni/Mo mass ratio of 3:1 showed an excellent catalytic HDO activity with 100 % conversion of triolein and 86.5 % selectivity of octadecane. Combined with experimental results and density functional calculations, it was demonstrated that oxygen vacancies derived from MoOx considerably favored the adsorption and activation of substrates. An efficient selective HDO process for fats and oils has been achieved by direct deoxygenation of hydroxyl/carbonyl functional groups.

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温和条件下原位合成NiMo@SAPO-11对三油酸的加氢脱氧
经济且无硫的镍催化剂是脂肪和油加氢脱氧(HDO)生产柴油级石蜡的有吸引力的替代品,但容易发生脱碳/脱羧(DCOx)反应。金属氧化物修饰的镍催化剂具有非常高的催化活性,可以修饰镍催化的脱氧反应途径。本文在温和条件下(100℃,12 h)原位合成制备了一系列不同Ni/Mo质量比的NiMo@SAPO-11催化剂。合成的Ni/Mo质量比为3:1的双金属NiMo纳米催化剂具有优异的HDO催化活性,三油醇转化率为100%,十八烷选择性为86.5%。结合实验结果和密度泛函计算,证明了MoOx产生的氧空位极大地有利于底物的吸附和活化。通过直接脱氧羟基/羰基官能团,实现了油脂的高效选择性HDO工艺。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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