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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.
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1 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)
2 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)
3 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)
4 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)
5 University of Chinese Academy of Sciences, School of Physical Sciences, Beijing, China (GRID:grid.410726.6) (ISNI:0000 0004 1797 8419)
6 Hunan University, College of Materials Science and Engineering, Changsha, China (GRID:grid.67293.39)