Adsorption Site Regulation to Guide Atomic Design of Ni–Ga Catalysts for Acetylene Semi‐Hydrogenation

Abstract

Atomic regulation of metal catalysts has emerged as an intriguing yet challenging strategy to boost product selectivity. Here, we report a density functional theory‐guided atomic design strategy for the fabrication of a NiGa intermetallic catalyst with completely isolated Ni sites to optimize acetylene semi‐hydrogenation processes. Such Ni sites show not only preferential acetylene π‐adsorption, but also enhanced ethylene desorption. The characteristics of the Ni sites are confirmed by multiple characterization techniques, including aberration‐corrected high‐resolution scanning transmission electron microscopy and X‐ray absorption spectrometry measurements. The superior performance is also confirmed experimentally against a Ni5Ga3 intermetallic catalyst with partially isolated Ni sites and against a Ni catalyst with multi‐atomic ensemble Ni sites. Accordingly, the NiGa intermetallic catalyst with the completely isolated Ni sites shows significantly enhanced selectivity to ethylene and suppressed coke formation.

Hydroxyl improving the activity, selectivity and stability of supported Ni single atoms for selective semi-hydrogenation

“…However, Ni metal can oligomerize hydrocarbon reactants, which subsequently reduces catalytic selectivity in acetylene hydrogenation towards ethylene. [10][11][12] Improved selectivity for acetylene hydrogenation towards ethylene can be achieved by alloying Ni with inactive metals, such as Zn, [13][14][15][16][17] Cu, [18][19][20] Au, [21][22][23] Ga [24][25][26] and Sn, 27,28 to form bimetallic particles. Nevertheless, the resulting bimetallic catalysts with the presence of an extended ensemble are not free from the formation of ethane and oligomers.…”

Constructing RuCoOx/NC Nanosheets with Low Crystallinity within ZIF‐9 as Bifunctional Catalysts for Highly Efficient Overall Water Splitting

“…Hydrogen is a promising secondary energy in the construction of multiple energy supply system, due to the advantages of wide sources, high energy density, flexibility, and rich application scenarios [1,2] . The conversion of electric energy to hydrogen via electrocatalytic water splitting has become an important direction in the new energy technology revolution [3–5] .…”

Pd‐Nanocomposites Formed by Calcination of [Pd(2‐pymo)2]n Framework as Catalysts of Phenylacetylene Semihydrogenation in Water

“…[8] Catalytic transformations of terminal alkynes are intensively studied due to their technological importance. [22,23] Semihydrogenation of phenylacetylene to styrene is an important process in the olefin industry because phenylacetylene can inhibit styrene polymerization. [24] Therefore the concentration of phenylacetylene should be reduced to < 10 ppm.…”