Tuning the synthesis of polymetallic-doped ZIF derived materials for efficient hydrogenation of furfural to furfuryl alcohol
Tuning the synthesis of polymetallic-doped ZIF derived materials for efficient hydrogenation of furfural to furfuryl alcohol
复制标题
调整多金属掺杂 ZIF 衍生材料的合成，以将糠醛有效氢化为糠醇
DOI：
10.1039/d0nr04098c
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发表时间：
2020
期刊：
影响因子：
6.7
通讯作者：
Zou Xiaoqin
中科院分区：
文献类型：
--
作者：
Fan Yafei;Li Shangjing;Wang Ying;Zhuang Changfu;Liu Xiaoteng;Zhu Guangshan;Zou Xiaoqin
采用多金属均相掺杂和自模板法制备了Cu、Co和Zn改性的N掺杂多孔炭（CuCo/Zn@NPC），作为糠醛加氢制糠醇的高性能非贵金属催化剂。在600 °C下处理后的CuCo/Zn@NPC-600催化剂显示出上级催化活性，在140 °C下使用H2时FF的转化率接近100%，FAL的选择性接近100%。在以异丙醇为氢供体的催化转移加氢反应中，FF的转化率达到95.8%，FAL的选择性为99.1%。结果表明，Zn掺杂使CuCo/Zn@NPC-600催化剂的产率比CuCo@NPC-600催化剂高37.3倍，比Cu掺杂的Co/Zn@NPC-600催化剂高2.3倍。CuCo/Zn@NPC-600催化剂的高活性主要是由于金属纳米颗粒的高度分散、Zn从前驱体模板中逃逸而形成的高级孔结构以及Cu和Co之间的协同效应。此外，CuCo/Zn@NPC-600催化剂在4次循环试验中表现出良好的FF加氢循环性能。采用均相掺杂和自模板策略的先进合成方法为制备有效的生物质基化合物加氢催化剂提供了启示。
Cu, Co and Zn modified N-doped porous carbons (CuCo/Zn@NPC) are prepared using a polymetallic homogeneous doping and self-templating method as high performance non-noble metal catalysts for the hydrogenation of furfural (FF) to furfuryl alcohol (FAL). The CuCo/Zn@NPC-600 catalyst after treatment at 600 °C shows a superior catalytic activity with nearly 100% conversion of FF and an almost 100% selectivity of FAL using H2 at 140 °C. Meanwhile in the catalytic transfer hydrogenation (CTH) using 2-propanol as a H-donor, the conversion of FF reaches 95.8% and the selectivity of FAL is 99.1%. The results show that the Zn dopant leads to 37.3 times higher yield on the CuCo/Zn@NPC-600 catalyst than that on CuCo@NPC-600, and 2.3 times higher than that on Co/Zn@NPC-600 with Cu dopants. The efficient activity of the CuCo/Zn@NPC-600 catalyst is mainly due to the highly dispersed metal nanoparticles, the advanced porous structure resulting from Zn escape from the precursor template, and the synergistic effect between Cu and Co. Furthermore, the CuCo/Zn@NPC-600 catalyst exhibits good recyclability in FF hydrogenation in four cycle tests. The advanced synthesis method using a homogeneous doping and self-templating strategy sheds light on preparing effective catalysts for hydrogenation of biomass-based compounds.