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Ga-doped Cu/H-nanozeolite-Y catalyst for selective hydrogenation and hydrodeoxygenation of lignin-derived chemicals
Green Chemistry ( IF 9.8 ) Pub Date : 2018-06-18 , DOI: 10.1039/c8gc00629f
Deepak Verma 1, 2, 3, 4, 5 , Rizki Insyani 1, 2, 3, 4 , Handi Setiadi Cahyadi 1, 2, 3, 4 , Jaeyong Park 2, 3, 4, 5 , Seung Min Kim 4, 6, 7, 8 , Jae Min Cho 2, 3, 4, 9 , Jong Wook Bae 2, 3, 4, 9 , Jaehoon Kim 1, 2, 3, 4, 5
Affiliation  

The development of an efficient non-sulfided and non-precious catalyst for selective hydrogenation (HD) and hydrodeoxygenation (HDO) of biomass-derived feedstocks to produce fuels and chemicals is of great interest. In this study, a highly efficient bimetallic Ga-doped Cu/H-nanozeolite-Y (Cu/HNZY) catalyst was developed for selective HD and HDO of lignin-derived species (vanillin, acetovanillone, and cinnamaldehyde) under mild conditions (120–180 °C, 1 MPa H2). The HNZY support exhibited a mesoporous structure with a large external surface area, which can facilitate reactant adsorption. Ga doping not only increased the Cu dispersion and Lewis acidity, but produced low coordinated Ga species (e.g., Ga+ and (GaH2)+), which could enhance the HDO activity. As a result, at 160 °C for 2 to 5 h, complete conversion of vanillin and acetovanillone into their decarbonylated species (creosol and 4-ethylguiuacol) with high selectivity (>99%) could be achieved at a low H2 initial pressure of 1 MPa. In addition, when cinnamaldehyde was converted over Ga-doped Cu/HNZY at 180 °C, selective HD and HDO followed by cyclization formed high amounts of indane and its derivatives, which have a variety of applications in pharmaceutical and agricultural industries. This could open a new possibility for lignin-to-drug intermediates.

中文翻译:

Ga掺杂的Cu / H-纳米沸石-Y催化剂用于木质素衍生化学品的选择性加氢和加氢脱氧

对于用于衍生自生物质的原料的选择性加氢(HD)和加氢脱氧(HDO)以生产燃料和化学品的有效的非硫化且非贵重的催化剂的开发引起了极大的兴趣。在这项研究中,开发了一种高效的双金属Ga掺杂的Cu / H-纳米沸石-Y(Cu / HNZY)催化剂,用于在温和条件下(120- 180°C,1 MPa H 2)。HNZY载体表现出具有大的外表面积的中孔结构,这可以促进反应物的吸附。Ga掺杂不仅增加了Cu的分散度和路易斯酸度,而且产生了低配位的Ga物种(例如Ga +和(GaH 2+),可以增强HDO的活性。结果,在160°C下2至5 h,可以在低的H 2初始压力下,以高选择性(> 99%)将香兰素和乙酰香草醛完全转化为脱羰基物质(甲酚和4-乙基癸二酚)。 1兆帕 另外,当肉桂醛在180°C的条件下通过Ga掺杂的Cu / HNZY转化时,选择性HD和HDO随后环化形成大量的茚满及其衍生物,在制药和农业工业中具有多种应用。这可能为木质素-药物中间体开辟新的可能性。
更新日期:2018-07-16
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