Importance of Zeolite Wettability for Selective Hydrogenation of Furfural over Pd@Zeolite Catalysts

Importance of Zeolite Wettability for Selective Hydrogenation of Furfural over Pd@Zeolite Catalysts
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沸石润湿性对于 Pd@沸石催化剂上糠醛选择性加氢的重要性

DOI:
10.1021/acscatal.7b03443
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发表时间:
2018-01
期刊:
影响因子:
12.9
通讯作者:
Feng-Shou Xiao
Feng-Shou Xiao
中科院分区:
化学1区
文献类型:
--
作者:
Chengtao Wang;Zhiqiang Liu;Liang Wang;Xue Dong;Jian Zhang;Guoxiong Wang;Shichao Han;Xiangju Meng;Anmin Zheng;Feng-Shou Xiao

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金属催化生物质分子的选择性氢化反应需求很大,但由于反应途径复杂,具有挑战性。在此,我们报告了一个有说服力的例子,通过分子筛微孔中分子的可控吸附,在Pd催化剂上实现了糠醛的选择性加氢。这一成功的关键是通过将硅烷醇官能化到沸石框架中,将Pd纳米颗粒固定在具有可控润湿性的硅烷-1沸石中(Pd@S-1-OH)。在以糠醛加氢为模型反应中,亲水性合适的Pd@S-1-OH催化剂对呋喃的形成表现出了非凡的选择性,在糠醛完全转化的情况下,呋喃的选择性高达99.9%,优于传统的基于沸石晶体的Pd纳米颗粒(Pd/S-1)和没有人工官能化硅醇基的S-1沸石固定Pd催化剂(Pd@S-1)。Pd@S-1-OH的非凡表现可以合理地归因于……
The metal-catalyzed selective hydrogenation of biomass-derived molecules is in great demand but is challenging due to the complex reaction pathways. Herein, we report a persuasive example for achieving selective hydrogenation of furfural over Pd catalysts by controllable sorption of molecules in zeolite micropores. The key to this success is fixation of Pd nanoparticles inside of silicalite-1 zeolite with controllable wettability (Pd@S-1-OH) by functionalizing silanol groups into the zeolite framework. In the hydrogenation of furfural as a model reaction, the Pd@S-1-OH catalyst with appropriate hydrophilicity exhibits extraordinary selectivity for the formation of furan, giving furan selectivity as high as >99.9% with a complete conversion of furfural, outperforming the conventional Pd nanoparticles supported on zeolite crystals (Pd/S-1) and S-1 zeolite fixed Pd catalysts without an artificially functionalized silanol group (Pd@S-1). The extraordinary performance of Pd@S-1-OH is reasonably attributed to t...