Multifunctional Pd@UiO-66 Catalysts for Continuous Catalytic Upgrading of Ethanol to n-Butanol
Multifunctional Pd@UiO-66 Catalysts for Continuous Catalytic Upgrading of Ethanol to n-Butanol
复制标题
用于乙醇连续催化升级为正丁醇的多功能Pd@UiO-66催化剂
DOI：
10.1021/acscatal.8b04014
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发表时间：
2018-12-01
期刊：
影响因子：
12.9
通讯作者：
Li, Xiaonian
中科院分区：
文献类型：
--
作者：
Jiang, Dahao;Fang, Geqian;Li, Xiaonian
将UIO-66负载的纳米钯(Pd@UIO-66)催化剂用于乙醇连续催化改质为正丁醇的高效、稳定催化剂。最好的Pd@UiO-66催化剂在较低的温度(523K)和压力(2 Mpa)下进行了200h的长期评价，乙醇转化率为49.8%，正丁醇的选择性为48.6%，正丁醇产率为24.2%。Pd@UIO-66催化剂的高活性和高选择性主要归因于高度分散的Pd纳米粒子和UIO-66上的配位不饱和的Zr中心分别作为脱氢/加氢和Aldol缩合的活性中心的紧密协同作用，而催化剂的高稳定性主要归因于Pd纳米粒子与Zr-6节点的静电吸引和UIO-66空穴的限制作用。
UiO-66-encapsulated nanopalladium (Pd@UiO-66) catalysts were used as highly efficient and stable catalysts for continuous catalytic upgrading of ethanol to n-butanol. The best Pd@UiO-66 catalyst exhibited 49.8% of ethanol conversion, 48.6% of selectivity toward n-butanol, and thereby 24.2% of n-butanol yield at relatively low temperature (523 K) and pressure (2 MPa) during a 200 h long-term evaluation. The high catalytic activity and selectivity of Pd@UiO-66 catalyst are primarily ascribed to the close synergy of highly dispersed Pd nanoparticles and coordinatively unsaturated Zr sites on Zr-6 nodes of UiO-66, as active centers for dehydrogenation/hydrogenation and aldol condensation, respectively; however, the high stability of the catalyst is mainly attributed to the electrostatic attraction of Pd nanoparticles with Zr-6 nodes and the confinement effect of the cavities of UiO-66.