Modulating the Electronic Structure of Single‐Atom Catalysts on 2D Nanomaterials for Enhanced Electrocatalytic Performance

Abstract

Single‐atom catalysts (SACs) on 2D nanomaterials have great potential as efficient and low‐cost electrocatalysts for clean energy technologies. The coordination environments, as well as the physicochemical properties of the 2D supports, play key roles in tuning the catalytic activity and reaction mechanism of the single‐atom centers. This review first summarizes the suitable synthetic strategies of single‐atom on different 2D supports. The methods that facilitate the formation of relative homogeneous structure and enable the regulation of the surrounding atomic environment of metal center are discussed. Furthermore, the recent progress of SACs for energy‐related electrochemical applications is reviewed, including oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO2 reduction reaction, and nitrogen reduction reaction. The strategies about modulation of the electronic structure of single‐atom for enhanced performance are highlighted, together with a discussion of the current issues and the prospects of this field.

Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

“…atoms from support materials or metal-metal bonds (Scheme 1). The electronic and geometric structures of central metal atoms could be adjustable by tailoring the coordination environment, which would change the absorption activity of reactants on metal atoms and thus influence the catalytic properties [5,[31][32][33][34]. A comprehensive review on modulating the local coordination of SACs and their related enhanced catalytic performance is timely important.…”

Transition metal-based catalysts for the electrochemical CO2reduction: from atoms and molecules to nanostructured materials

“…1). [33][34][35][36][37][38] A rational catalyst design primarily requires the elucidation of the structure-activity relationship. The present work will focus on the main reported strategies to control the structure, morphology and chemical composition at the atomic, molecular, supramolecular and nano levels, highlighting how these aspects affect the reactivity towards CO 2 RR.…”

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

“…The carbonaceous substrates (amorphous carbon, graphene, carbon nanotubes, g‐C 3 N 4 , etc.) not only have high electrical conductivity for fast electron transport, but also large specific surface area to prevent metal agglomeration via the strengthened metal‐support interaction . These interactions play a key role in tuning the charge density and the d orbital states of the metal active sites, enabling optimization of the adsorption energy for the intermediates on the metal surface.…”