Gas‐Phase Dehydrogenation of Alkanes: C−H Activation by a Graphene‐Supported Nickel Single‐Atom Catalyst Model

Abstract

Ag as-phase anionic nickel(0) fluorenyl complex is shown to effect the dehydrogenation of linear,b ranched, and cyclic alkanes via CÀHa ctivation. It performs dehydrogenations via aC ÀHinsertion followed by b-hydride elimination. When given energy via collision-induced dissociation, the system is capable of second and thirdd ehydrogenations to form dienes and aromatics such as benzene.K inetic isotope effects and DFT calculations completed at the M06/6-311+ +G** level support the proposed mechanism. The metal complex can act as an experimental model for graphenesupported nickel single-atom catalysts and suggests that these catalysts are capable of alkane dehydrogenation via CÀH activation. Scheme 1. Gas-phase synthesis of complex I.

Few-Atom Pt Ensembles Enable Efficient Catalytic Cyclohexane Dehydrogenation for Hydrogen Production

“…Significantly, Campbell et al 23 examined the effect of ensemble size for this reaction on the Pt(111) single-crystal surface and demonstrated that it may require at least eight Pt atoms to convert cyclohexane into benzene. Recently, it was proposed that the gas-phase Ni fluorenyl complex (a Ni atom species), upon gaining energy via collision-induced dissociation, can catalyze the CDH reaction in an ion-trap mass spectrometer, 24 although it was far from a realistic heterogeneous catalytic reaction. With recent advances in catalyst fabrication and characterization, the field is better equipped to revisit these claims and, importantly, to refine the design principle of the metal catalyst using the knowledge gained recently at the atomic and molecular levels.…”

Multilayer Self‐Assemblies for Fabricating Graphene‐Supported Single‐Atomic Metal via Microwave‐Assisted Emulsion Micelle

“…[7] A few disordered anchoring sites were exposed on the surface of graphene, which may contribute to capturing the single-metal atoms. [8] Therefore, it is still highly urgent to develop a rapid and facile synthetic route for fabricating G-SAMs with controllable single-metal loading and distribution. [9] In nature, molecular self-assemblies and self-organizations have ubiquitously occurred in the formation of molecular crystals and protein folding.…”

Tuning the hybridization and charge polarization in metal nanoparticles dispersed over Schiff base functionalized SBA-15 enhances CO2 capture and conversion to formic acid

“…4b). [49][50][51] The peak at 2.7 Å can be assigned to the Ni-Pd bond in the sample conrming the alloy formation. 52 There is no metallic Ni-Ni bonding present in the samples as there is no indication of a Ni-Ni peak at 2.15 Å, further conrming that Ni does not crystallize as Ni metal.…”