A Synthesis Strategy of Double-Atom Catalysts on a Carbon Surface

Abstract

Highly active double-atom catalysts (DACs) for electrochemical reactions hold promise to enable sustainable energy conversion and storage. However, fabricating stable DACs remains challenging due to the lack of a fundamental understanding of the formation and stabilization mechanisms of DACs. Here, we present a systematic investigation of the feasibility of forming DACs on a defective carbon surface, through density functional theory calculations, from which an effective synthesis strategy of DACs is proposed. Such a synthesis strategy is validated by molecular dynamics simulations of the process of the formation of a stable array of Pt–Au DACs on a defective carbon surface. Results from this study offer a mechanistic understanding and quantitative guidance for the rational selection of transition metals and optimal synthesis conditions to fabricate DACs with desirable electrocatalyst activity in emerging energy applications.

Bimetallic Sites for Catalysis: From Binuclear Metal Sites to Bimetallic Nanoclusters and Nanoparticles

“…The formation of binuclear bimetallic sites on carbon support can also be achieved by a subsequent anchoring strategy . The metal atoms anchored primarily on the support can serve as the binding sites for the secondary metal atoms during the high-temperature pyrolysis process through the formation of metal–metal bonding, which facilitates the selective generation of binuclear bimetallic sites.…”

“…The formation of binuclear bimetallic sites on carbon support can also be achieved by a subsequent anchoring strategy. 74 The metal atoms anchored primarily on the support can serve as the binding sites for the secondary metal atoms during the hightemperature pyrolysis process through the formation of metal− metal bonding, which facilitates the selective generation of binuclear bimetallic sites. Taking Co-MOF material comprising isolated Co atoms in the MOF matrix as the starting material, binuclear Co−Fe species are formed after the introduction of Fe precursor into the Co-MOF and subsequent high-temperature pyrolysis treatment.…”

Ligand Assisted Thermal Atomization of Palladium Clusters: An Inspiring Approach for the Rational Design of Atomically Dispersed Metal Catalysts

“…Like what has been found in ADCs basing on other elements, many researchers noticed that Pd based NCCs and Pd based SACs work differently within the scope of catalytic direction [10e] and chemical activity [11] . However, the transformation between Pd‐NCC and Pd‐SAC always requires extremely high annealing temperature (above 700 °C) and sometimes dangerous reducing atmosphere (such as H 2 , CO and CH 4 ) [12] because of the high formation energy of Pd nanoclusters [13] . Besides, suffering from coking and sintering, it is a common phenomenon that the Pd nanoclusters aggregate into large nanoparticles after going through high temperature treatments [14] .…”

Machine learning enabled rational design of atomic catalysts for electrochemical reactions

“…, low loading and isolated active site). 10–14 In short, the development of ACs can facilitate atomic economy in the application of renewable energy conversion technologies, leading to maximum atom-utilization efficiency.…”

“…They not only inherit the advantages of SACs (e.g., ultimate atomic utilization, high activity, and selectivity) but also introduce a synergistic effect to break the theoretical limit of SACs and overcome the drawbacks of SACs (e.g., low loading and isolated active site). [10][11][12][13][14] In short, the development of ACs can facilitate atomic economy in the application of renewable energy conversion technologies, leading to maximum atom-utilization efficiency.…”