Regulating coordination number in atomically dispersed Pt species on defect-rich graphene for n-butane dehydrogenation reaction

Abstract

Metal nanoparticle (NP), cluster and isolated metal atom (or single atom, SA) exhibit different catalytic performance in heterogeneous catalysis originating from their distinct nanostructures. To maximize atom efficiency and boost activity for catalysis, the construction of structure–performance relationship provides an effective way at the atomic level. Here, we successfully fabricate fully exposed Pt3 clusters on the defective nanodiamond@graphene (ND@G) by the assistance of atomically dispersed Sn promoters, and correlated the n-butane direct dehydrogenation (DDH) activity with the average coordination number (CN) of Pt-Pt bond in Pt NP, Pt3 cluster and Pt SA for fundamentally understanding structure (especially the sub-nano structure) effects on n-butane DDH reaction at the atomic level. The as-prepared fully exposed Pt3 cluster catalyst shows higher conversion (35.4%) and remarkable alkene selectivity (99.0%) for n-butane direct DDH reaction at 450 °C, compared to typical Pt NP and Pt SA catalysts supported on ND@G. Density functional theory calculation (DFT) reveal that the fully exposed Pt3 clusters possess favorable dehydrogenation activation barrier of n-butane and reasonable desorption barrier of butene in the DDH reaction.

Tailoring Single‐Atom Platinum for Selective and Stable Catalysts in Propane Dehydrogenation

“…Notably, this catalyst does not create a Pt−Sn alloy structure, implying the residual Pt ensembles, despite its high stability. As well as PDH, small Pt clusters exhibit excellent catalytic performance for the dehydrogenation of n ‐butane at 450 °C, which reflects the availability of Pt clusters for alkane dehydrogenation [8,65,66] …”

“…As well as PDH, small Pt clusters exhibit excellent catalytic performance for the dehydrogenation of n-butane at 450 °C, which reflects the availability of Pt clusters for alkane dehydrogenation. [8,65,66]…”

Single-atom catalysts for thermal- and electro-catalytic hydrogenation reactions

“…With maximum atom utilization, the development of SACs provides a promising approach to reasonable use of metal resources and achieving atomic economy, especially for noble-metal-based catalysts. [32][33][34][35][36] In terms of reactivity, SACs with fully exposed atoms possess more active sites, and the unsaturated coordination environment and charge transfer between single metal atoms and the support will effectively improve the intrinsic activity of active sites. 37,38 In this regard, a variety of synthetic methodologies have been developed for SACs.…”

A Label-Free Electrochemical Immunosensor for CEA Detection on a Novel Signal Amplification Platform of Cu2S/Pd/CuO Nanocomposites

“…Nanomaterials, such as graphene oxide, metal nanoparticles, and metal-organic frameworks (MOFs), are often used as a means of signal amplification to heighten the sensitivity of sensors because of their high specific surface area, prominent electron transfer ability, and excellent biocompatibility (Song et al, 2016;Farka et al, 2017). Among them, metal nanomaterials (Chen et al, 2021;Simsek and Wongkaew, 2021) have attracted strong attention because of their stronger electrical conductivity, excellent catalysis, larger specific surface area, and convenient control. Palladium nanoparticles (Pd NPs) have efficient catalytic activity toward hydrogen peroxide substrates (Edwards et al, 2014;Trujillo et al, 2021) and are excellent materials for the construction of immunosensors (Han et al, 2020).…”