Hydrodeoxygenation of non-edible bio-lipids to renewable hydrocarbons over mesoporous SiO2-TiO2 supported NiMo bimetallic catalyst
Hydrodeoxygenation of non-edible bio-lipids to renewable hydrocarbons over mesoporous SiO2-TiO2 supported NiMo bimetallic catalyst
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介孔SiO2-TiO2负载NiMo双金属催化剂将非食用生物脂质加氢脱氧为可再生碳氢化合物
DOI：
10.1016/j.apcata.2021.118475
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发表时间：
2022-02
期刊：
影响因子：
--
通讯作者：
Yuejin Liu（刘跃进）
中科院分区：
文献类型：
--
作者：
Lin Fu（付琳）;Wenxia Ba（巴文霞）;Yongfei Li（李勇飞）;Xin Li（黎新）;Jingxuan Zhao（赵敬璇）;Simiao Zhang（张思苗）;Yuejin Liu（刘跃进）
镍催化剂是脂肪酸加氢脱氧（HDO）的理想催化剂，但其HDO选择性较差。本文采用沉淀浸渍法制备了介孔Ni-Mo/SiO2-TiO 2催化剂，并将其用于月桂酸甲酯的加氢脱硫反应，月桂酸甲酯完全转化时正十二烷收率为96.3%。非食用生物油脂如麻风树油和废食用油也转化为n-C14+16+ 18烃，产率分别为94.3%和92.4%。此外，Ni-Mo/SiO2-TiO 2对酯基的HDO具有较强的化学选择性。实验结果表明，Mo的添加量和Ti/Si摩尔比对HDO选择性有显著影响。在部分还原的TiO 2表面形成的氧空位牢固地键合了Ni纳米粒子，活化了C双键O/C单键O键，改善了Ni纳米粒子的分散性，促进了R-COOCH 3 →R-CHO还原。Mo的加入使反应物的吸附构型由η1（C）-酰基转变为η2（C，O）-醛，促进了R-CH_2 OH中间体的形成。此外，丰富的布朗斯台德酸性位点（Mo 4 +-OH，Mo 6 +-OH，羟基）促进R-CH 2 OH到R-CH 3的HDO。
Ni-catalysts are promising candidate for fatty acid hydrodeoxygenation (HDO), but are limited by their quite poor HDO selectivity. Herein, a mesoporous Ni-Mo/SiO2-TiO2catalyst was prepared by precipitation and impregnation method and used for methyl laurate HDO, yielding 96.3% n-dodecane yield at full methyl laurate conversion. Non-edible bio-lipids such as jatropha oil and waste cooking oil also converted to n-C14+16+18hydrocarbons with yields of 94.3% and 92.4%, respectively. Besides, Ni-Mo/SiO2-TiO2shows strong chemoselectivity towards the HDO of ester groups. Experimental results showed that Mo-addition and Ti/Si molar ratio strongly influenced HDO selectivity. Oxygen vacancies formed on partial reduced TiO2surface securely bond Ni NPs and activate Cdouble bondO/Csingle bondO bonds, improving Ni NPs dispersion and promoting R–COOCH3→R–CHO reduction. Additional, Mo-addition switches reactant adsorption configuration from η1(C)-acyl to η2(C,O)-aldehyde, promoting the formation of R–CH2OH intermediate. Moreover, abundant Brønsted acidic sites (Mo4+–OH, Mo6+–OH, hydroxy groups) facilitate the HDO of R-CH2OH to R-CH3.
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