Chemoselective hydrodeoxygenation of palmitic acid to diesel-like hydrocarbons over Ni/MoO2@Mo2CTx catalyst with extraordinary synergic effect
Chemoselective hydrodeoxygenation of palmitic acid to diesel-like hydrocarbons over Ni/MoO2@Mo2CTx catalyst with extraordinary synergic effect
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DOI：
10.1016/j.cej.2019.123472
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发表时间：
2020-07
影响因子：
15.1
通讯作者：
Junmei Liang;Tao Chen;Jiapeng Liu;Qicheng Zhang;W. Peng;Yang Li;Feng-bao Zhang;Xiaobin Fan
中科院分区：
文献类型：
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作者：
Junmei Liang;Tao Chen;Jiapeng Liu;Qicheng Zhang;W. Peng;Yang Li;Feng-bao Zhang;Xiaobin Fan
脂质化学选择性加氢脱氧（HDO）生成类柴油烃是生物质向生物燃料转化的重要过程。本文设计了一种新型镍基催化剂（Ni/MoO2@Mo2CTx），在棕榈酸的HDO中具有优异的催化性能。为了减轻ni基催化剂中C原子的损失，采用了Mo2CTxMXene的部分氧化作为新型载体。结果表明，十六烷/十五烷（C16/C15）的催化活性和选择性比在Ni/MoO2@Mo2CTxcatalyst上得到了提高，棕榈酸HDO的主要产物是C16，具有较高的碳原子经济性。这种促进的催化性能可能归因于金属Ni， Mo2CTxMXene以及moo2活性位点的协同作用。棕榈酸（-COOH）在初始阶段通过Ni/MoO2@Mo2CTxcatalyst可转化为十六烷醛（-CHO）和十六烷醇（-CH2OH）。金属Ni进一步通过脱羰（DCO）途径裂解C-C键，使十六醛氢化成c15。mo2ct氧化得到的moo2纳米粒子加速了十六醇C-O键的断裂，通过加氢-脱水途径提高了c16的选择性。
Chemoselective hydrodeoxygenation (HDO) of lipids to diesel-like hydrocarbons is important for biomass to biofuel conversion. Here we design a new Ni-based catalyst (Ni/MoO2@Mo2CTx) with extraordinary catalytic performance in the HDO of palmitic acid. To relieve the loss of C atom for Ni-based catalyst, partial oxidation of Mo2CTxMXene was used as a novel support. As a result, the catalytic activity and selectivity ratio of hexadecane/pentadecane (C16/C15) were enhanced over Ni/MoO2@Mo2CTxcatalyst, and the major product of palmitic acid HDO is C16, demonstrating a high C atom economy. This facilitated catalytic performance may be ascribed to the synergic effect of metal Ni, Mo2CTxMXene as well as MoO2active sites. The palmitic acid (–COOH) can convert into hexadecanal (–CHO) and hexadecanol (–CH2OH) over Ni/MoO2@Mo2CTxcatalyst in the initial stage. The metal Ni further contributes to the hydrogenation of the hexadecanal to C15with the cleavage of C–C bonds by decarbonylation (DCO) route. MoO2nanoparticles obtained from Mo2CTxoxidation accelerate the scission of C–O bonds of the hexadecanol to improve the selectivity of C16by hydrogenation-dehydration route.