Abstract

Ambient-condition acetylene hydrogenation to ethylene (AC-AHE) is a promising process for ethylene production with minimal additional energy input, yet remains a great challenge due to the difficulty in the coactivation of acetylene and H2 at room temperature. Herein, we report a highly efficient AC-AHE process over robust sulfur-confined atomic Pd species on tungsten sulfide surface. The catalyst exhibits over 99% acetylene conversion with a high ethylene selectivity of 70% at 25 oC, and a record space-time yield of ethylene of 1123 molC2H4 molPd−1 h−1 under ambient conditions, which is nearly four times that of the typical Pd1Ag3/Al2O3 catalyst, and exhibiting superior stability of over 500 h. We demonstrate that the confinement of Pd-S coordination induces positively-charged atomic Pdδ+, which not only facilitates C2H2 hydrogenation but also promotes C2H4 desorption, thereby enabling a high conversion of C2H2 to C2H4 at room temperature while suppressing over-hydrogenation to C2H6.

Ambient-condition acetylene hydrogenation to ethylene (AC-AHE) is a promising process for ethylene production yet remains a challenge. Here the authors report a highly efficient AC-AHE process over robust sulfur-confined atomic Pd species on tungsten sulfide surface, achieving over 99% conversion and 70% selectivity, with a record-breaking ethylene yield and excellent stability exceeding 500 h at 25 °C.

Details

Title
Ambient-condition acetylene hydrogenation to ethylene over WS2-confined atomic Pd sites
Author
Zhang, Wangwang 1 ; Uwakwe, Kelechi 2 ; Hu, Jingting 3 ; Wei, Yan 4 ; Zhu, Juntong 5 ; Zhou, Wu 5   VIAFID ORCID Logo  ; Ma, Chao 6   VIAFID ORCID Logo  ; Yu, Liang 2   VIAFID ORCID Logo  ; Huang, Rui 4   VIAFID ORCID Logo  ; Deng, Dehui 3   VIAFID ORCID Logo 

 Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), College of Chemistry and Chemical Engineering, Xiamen, China (GRID:grid.12955.3a) (ISNI:0000 0001 2264 7233); Chinese Academy of Science, State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Dalian Institute of Chemical Physics, Dalian, China (GRID:grid.9227.e) (ISNI:0000000119573309) 
 Chinese Academy of Science, State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Dalian Institute of Chemical Physics, Dalian, China (GRID:grid.9227.e) (ISNI:0000000119573309); University of Chinese Academy of Sciences, Beijing, China (GRID:grid.410726.6) (ISNI:0000 0004 1797 8419) 
 Xiamen University, State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), College of Chemistry and Chemical Engineering, Xiamen, China (GRID:grid.12955.3a) (ISNI:0000 0001 2264 7233); Chinese Academy of Science, State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Dalian Institute of Chemical Physics, Dalian, China (GRID:grid.9227.e) (ISNI:0000000119573309); University of Chinese Academy of Sciences, Beijing, China (GRID:grid.410726.6) (ISNI:0000 0004 1797 8419) 
 Chinese Academy of Science, State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Dalian Institute of Chemical Physics, Dalian, China (GRID:grid.9227.e) (ISNI:0000000119573309) 
 University of Chinese Academy of Sciences, School of Physical Sciences, Beijing, China (GRID:grid.410726.6) (ISNI:0000 0004 1797 8419) 
 Hunan University, College of Materials Science and Engineering, Changsha, China (GRID:grid.67293.39) 
Pages
9457
Publication year
2024
Publication date
2024
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
3123172386
Copyright
© The Author(s) 2024. This work is published under http://creativecommons.org/licenses/by-nc-nd/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.