Atomic Pd on Graphdiyne/Graphene Heterostructure as Efficient Catalyst for Aromatic Nitroreduction

Abstract

With the maximum atom-utilization efficiency, single atom catalysts (SACs) have attracted great research interest in catalysis science recently. To address the following key challenges for the further development of SACs: i) how to stabilize and avoid the aggregation of SACs, ii) how to enhance the specific surface area and conductivity of supports, and iii) how to achieve scalable mass production with low cost, a SAC consisting of single Pd atoms anchored on well-designed graphdiyne/graphene (GDY/G) heterostructure (Pd 1 /GDY/G) is synthesized. Pd 1 /GDY/G exhibits high catalytic performance, as demonstrated by the reduction reaction of 4-nitrophenol. Furthermore, density functional theory calculation indicates that graphene in the GDY/G heterostructure plays a key role in the enhancement of catalytic efficiency owing to the electron transfer process, deriving from the gap between the Fermi level of graphene and the conduction band minimum of GDY. The GDY/G heterostructure is a promising support for the preparation of extremely efficient and stable SACs, which can be used in a broad range of future industrial reactions.

Size‐Dependent Activity and Selectivity of Atomic‐Level Copper Nanoclusters during CO/CO2 Electroreduction

“…[11] Thes light hypsochromic shift for the Gb ands on Cu/GDY reveals the charge transfer from Cu to GDY. [13d] The decreasing intensity ratio of Da nd Gb ands for Cu/GDYat increasing loading conditions indicates agradually diminished amount of defects in Cu/GDY, [18] which should be ascribed to the nearly perfect reaction of the copper precursor with aryne monomer.Furthermore,the obvious peaks at 2170.6 cm À1 and 1974.8 cm À1 for Cu 45.2 /GDYc onfirm the formation of conjugated diyne linkers (-CCÀCC-). X-ray photoelectron spectroscopy (XPS) in Figure 2a shows identical peaks at ca.…”

Crystal Facet Induced Single‐Atom Pd/CoxOy on a Tunable Metal–Support Interface for Low Temperature Catalytic Oxidation

“…According to Figure 5d, Pd/Co x O y ‐I maintains the activity at 60 °C within 118 h in dry condition without any decay. In particular, by comparison to those of reported single‐atom Pd catalysts elsewhere, [ 9,37–40 ] as‐synthesized Pd/Co x O y ‐I catalyst exceeds most acceptable levels by four times or more (Table S3, Supporting Information). The terrific catalyst durability of the catalysts is reflected by the strong adhesion on substrate and stable interaction between Pd atoms and Co x O y nanoarrays.…”

Graphdiyne‐Supported Atomic Catalysts: Synthesis and Applications

“…In this method, liquid-exfoliated graphene was utilized as the template for the epitaxy growth of few-layered high-quality GDY. [28] Then, Pd(NO 3 ) 2 was utilized as a precursor and reacted with GDY/G at 373 K. After being reduced by NaBH 4 , Pd/GDY/G was obtained. The structure and composition were characterized before the catalytic reaction.…”