Selective hydrogenation of 1,3-butadiene catalyzed by a single Pd atom anchored on graphene: the importance of dynamics
Selective hydrogenation of 1,3-butadiene catalyzed by a single Pd atom anchored on graphene: the importance of dynamics
复制标题
锚定在石墨烯上的单个 Pd 原子催化 1,3-丁二烯的选择性氢化：动力学的重要性
DOI：
10.1039/c8sc00776d
复制
发表时间：
2018-07-21
期刊：
影响因子：
8.4
通讯作者：
Guo, Hua
中科院分区：
文献类型：
--
作者：
Feng, Yingxin;Zhou, Linsen;Guo, Hua
The active-site structure, reaction mechanism, and product seLectivity of the industrially important selective hydrogenation of 1,3-butadiene are investigated using first principles for an emerging single-atom Pd catalyst anchored on graphene. Density functional theory calculations suggest that the mono-pi-adsorbed reactant undergoes sequential hydrogenation by Pd-activated H-2. Importantly, the high seLectivity towards 1-butene is attributed to the post-transition-state dynamics in the second hydrogenation step, which Leads exclusively to the desorption of the product. This dynamical event prevails despite the existence of energetically preferred 1-butene adsorption on Pd, which would eventually Lead to complete hydrogenation to butane and be thus inconsistent with experimental observations. This insight underscores the importance of dynamics in heterogeneous catalysis, which has so far been underappreciated.
