Single‐Site Pd Coupling with Jahn–Teller Active Cu as Pair Sites for Simultaneous Activation of Alkyne and Hydrogen Toward Efficient Semihydrogenation
Abstract
Abstract Single‐site pairs are promising in achieving high selectivity and activity in alkyne semihydrogenation, but its applicability is limited by the insufficient activity because pair sites cannot adsorb and activate alkyne. Here, we couple single‐site Pd with Jahn–Teller active Cu atoms of Cu‐doped Fe 2 O 3 to construct a highly active and stable single‐site Pd‐Cu pairs. The Jahn–Teller active Cu possesses elongated axial orbitals, and the strong electronic coupling between Pd and Cu further contributes to their unoccupied axial d orbitals, which helps Pd‐Cu pair to cooperatively activate C 2 H 2 molecule, unlike ordinary single‐site pairs where only H 2 is activated. As a result, this catalyst exhibits state‐of‐the‐art performance, with > 99.99% conversion and 95.5% selectivity as well as excellent stability with negligible performance decay after 300‐h test in purifying acetylene of ethylene stream. Both in situ spectra and theoretical results indicate two H addition steps occur on Pd and Cu sites in sequence. This work opens an avenue for constructing highly efficient single‐site pairs for selective hydrogenation and beyond.
Article Details
Authors (9)
Jingyun Jiang
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry‐Education Platform for Energy Storage Tianjin University Tianjin 300072 China
Mengxian Yu
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry‐Education Platform for Energy Storage Tianjin University Tianjin 300072 China
Chengxiang Shi
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry-Education Platform for Energy Storage
Zhen‐Feng Huang
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry‐Education Platform for Energy Storage Tianjin University Tianjin 300072 China
Xiangwen Zhang
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry-Education Platform for Energy Storage
Lun Pan
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry-Education Platform for Energy Storage
Ruijie Gao
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry-Education Platform for Energy Storage
Jinlong Gong
School of Chemical Engineering and Technology, Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin University
Ji‐Jun Zou
Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Institute of Molecular Plus, National Industry‐Education Platform for Energy Storage Tianjin University Tianjin 300072 China