Ambient-condition acetylene hydrogenation to ethylene over WS<sub>2</sub>-confined atomic Pd sites.

Zhang, Wangwang; Uwakwe, Kelechi; Hu, Jingting; Wei, Yan; Zhu, Juntong; Zhou, Wu; Ma, Chao; Yu, Liang et al. · Nat Commun · 2024

basic_science · Level V

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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 H<sub>2</sub> 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 <sup>o</sup>C, and a record space-time yield of ethylene of 1123 mol<sub>C2H4</sub> mol<sub>Pd</sub><sup>-1</sup> h<sup>-1</sup> under ambient conditions, which is nearly four times that of the typical Pd<sub>1</sub>Ag<sub>3</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst, and exhibiting superior stability of over 500 h. We demonstrate that the confinement of Pd-S coordination induces positively-charged atomic Pd<sup>δ+</sup>, which not only facilitates C<sub>2</sub>H<sub>2</sub> hydrogenation but also promotes C<sub>2</sub>H<sub>4</sub> desorption, thereby enabling a high conversion of C<sub>2</sub>H<sub>2</sub> to C<sub>2</sub>H<sub>4</sub> at room temperature while suppressing over-hydrogenation to C<sub>2</sub>H<sub>6</sub>.