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.

Construction of Pd-Zn dual sites to enhance the performance for ethanol electro-oxidation reaction

“…The development of highly active and low-cost electrocatalysts for the ethanol oxidation reaction (EOR) lays at the heart of DEFCs 16 – 25 . Down-sizing of metal nanoparticles into individual metal sites is commonly regarded as an efficient approach to enhance the performance and cost-effectiveness of electrocatalysts, but may be improper for specific reactions catalyzed by multiple sites or peculiar active centers 26 – 31 . For now, alloying of Pd with base metals (M) like Zn, Ni, Sn, Co, Cu, Ge, etc.…”

Metallic Iron Nanocatalysts for the Selective Acetylene Hydrogenation under Industrial Front-End Conditions

“…The effects of morphology, − support interaction, − inorganic ,− and organic − selectivity modifiers, and bi- and trimetallic palladium catalysts − have been closely analyzed and optimized. Another approach under investigation is the further optimization of more abundantly available alternatives such as nickel, − copper, ,, and gold − as catalysts for selective acetylene hydrogenation in order to compete with the palladium-based catalysts. Over the last decades nanoparticles have been the focus of both approaches and many studies in general. , Various results can be optimized , through nanoparticle size, , morphology, − surface modification of organic ligands, − and support-based interactions. , Most recent deployments on acetylene hydrogenation include Pt–Sn bimetallic nanoparticles confined in mesoporous silica walls, Pd on fiberglass or in microporous carbon tubes, gold nanoparticles supported on Ce–Zr oxides, Cu 2 O nanocubes, and many more.…”

Influence of surface defects on activity and selectivity: a quantitative study of structure sensitivity of Pd catalysts for acetylene hydrogenation

“…9 An ideal catalyst for acetylene hydrogenation should be able to avoid the stepwise hydrogenation of acetylene to ethane. 10,11 Although the emerging non-noble Ni-based 10,12 and Cu-based 13 catalysts are showing convincing potentials, Pd-based catalysts are still the most commonly used in industries for acetylene hydrogenation and extensively studied from both experimental [14][15][16][17][18] and theoretical perspectives. [19][20][21][22][23][24] Interestingly, the activity and selectivity patterns of pure Pd catalysts vary significantly; in some cases, Pd was reported to possess considerable selectivity towards ethene, while other studies showed that Pd primarily promotes the production of ethane.…”