Single-Atom Ruthenium Catalytic Sites for Acetylene Hydrochlorination

J Phys Chem Lett. 2021 Aug 5;12(30):7350-7356. doi: 10.1021/acs.jpclett.1c01779. Epub 2021 Jul 29.

Abstract

The high cost of noble metal catalysts has been a major factor limiting their industrial applications. It is thus of strong interest to develop catalysts with minimum metal loading. Here, we designed and prepared a single-atom ruthenium catalyst through a cascade anchoring strategy to maximize the efficiency of Ru atoms for acetylene hydrochlorination. The single-atom catalyst supported on commercial activated carbon (AC) exhibits excellent catalytic activity with acetylene conversion of 95.4% at an acetylene gas hourly space velocity (GHSV) of 720 h-1 and almost no deactivation during a 600 h catalyst lifetime test. In conjunction with a series of experimental characterizations of the catalyst, including aberration-corrected scanning transmission electron microscopy (Ac-STEM), X-ray photoelectron spectroscopy (XPS), and extended X-ray absorption fine spectroscopy (EXAFS), density functional theory (DFT) study shows that RuN4 sites are likely responsible for acetylene hydrochlorination catalytic activity. This work provides a strategy to design efficient single-atom catalysts for acetylene hydrochlorination and helps us to gain deeper understanding of single-atom catalytic mechanisms.