Pd single-atom monolithic catalyst: Functional 3D structure and unique chemical selectivity in hydrogenation reaction

Abstract

Regulating the selectivity of catalysts in selective hydrogenation reactions at the atomic level is highly desirable but remains a grand challenge. Here we report a simple and practical strategy to synthesize a monolithic single-atom catalyst (SAC) with isolated Pd atoms supported on bulk nitrogen-doped carbon foams (Pd-SAs/CNF). Moreover, we demonstrate that the single-atom Pd sites with unique electronic structure endow Pd-SAs/CNF with an isolated site effect, leading to excellent activity and selectivity in 4nitrophenylacetylene semi-hydrogenation reaction. In addition, benefiting from the great integrity and excellent mechanical strength, monolithic Pd-SAs/CNF catalyst is easy to separate from the reaction system for conducting the subsequent recycling. The cyclic test demonstrates the excellent reusability and stability of monolithic Pd-SAs/CNF catalyst. The discovery of isolated site effect provides a new approach to design highly selective catalysts. And the development of monolithic SACs provides new opportunities to advance the practical applications of single-atom catalysts.

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

“…This can be attributed to the linear combination of CO on Pd species with distinct electron deficiency in Pd–Zn dual sites and individual Pd sites in comparison with Pd–Pd sites. The varying decrease in electron density of Pd discloses the slight electron transfer from Pd to Zn atoms in Pd–Zn dual sites and the strong electron transfer from Pd to the carrier in individual Pd sites 56 – 59 .…”

The Electronic Metal–Support Interaction Directing the Design of Single Atomic Site Catalysts: Achieving High Efficiency Towards Hydrogen Evolution

“…[34,35] To realize the practical use of the single atomic site catalysts, several problems are needed to be considered, such as regulating the catalytic efficiency of metallic center, regulating the conductivity of basement and so on. [36][37][38][39][40][41][42] The interaction between metallic center and basement has also been noticed for a long time. [43][44][45] However, it hasnt been clearly figured out, which may act as an effective strategy to overcome the existing barriers of HER.…”

Single-atom catalysts: stimulating electrochemical CO2 reduction reaction in the industrial era

“…Previous work showed that most carbon-supported SACs with abundant nitrogen-doped are stable activated single-metal ions to form the homogeneous microcosmic structure of M-N x -C y . The universal methods for synthesizing carbon-supported SACs include molecular skeleton encapsulation, [34][35][36][37][38] impregnation and pyrolysis, [39][40][41] coordination regulation, [42][43][44] and thermal dispersion.…”