Recent advances in the design of single-atom electrocatalysts by defect engineering

Abstract

Single-atom catalysts (SACs) with isolated metal atoms dispersed on supports have attracted increasing attention due to their maximum atomic utilization and excellent catalytic performance in various electrochemical reactions. However, SACs with a high surface-to-volume ratio are fundamentally less stable and easily agglomerate, which weakens their activity. In addition, another issue that restricts the application of SACs is the low metal loading. Defect engineering is the most effective strategy for the precise synthesis of nanomaterials to catch and immobilize single atoms through the modulation of the electronic structure and coordination environment. Herein, in this mini-review, the latest advances in designing SACs by defect engineering have been first highlighted. Then, the heteroatom doping or intrinsic defects of carbon-based support and anion vacancies or cation vacancies of metal-based supports are systematically evaluated. Subsequently, the structure-activity relationships between a single-atom coupled defect structure and electrocatalytic performance are illustrated by combining experimental results and theoretical calculations. Finally, a perspective to reveal the current challenges and opportunities for controllable preparation, in situ characterization, and commercial applications is further proposed.

Electrocatalytic oxidation of 5‐hydroxymethylfurfural for sustainable 2,5‐furandicarboxylic acid production—From mechanism to catalysts design

“…Crystal defect refers to the periodic repeated arrangement of particles deviating from the crystal structure 74 . It is well known that crystal defects are usually classified into point, line, surface, and bulk defects 75,76 .…”

“…Crystal defect refers to the periodic repeated arrangement of particles deviating from the crystal structure. 74 It is well known that crystal defects are usually classified into point, line, surface, and bulk defects. 75,76 Among them, point defects, including vacancy, gap, and impurity defects, have a critical impact on the functional properties of materials and are widely used in various application scenarios of catalysis.…”

Ni Single Atoms Embedded in Graphene Nanoribbon Sieves for High‐Performance CO2 Reduction to CO

“…[6][7][8] Especially, the Ni SACs, which are capable of selectively and efficiently reducing CO 2 to CO, have shown great potential for the CO 2 RR. [9][10][11] Theoretical researches have proved that the CO 2 RR activity of Ni SACs originates from the Ni-N 4 -C active center, in which the Ni atom are stabilized by four nitrogen atoms and embed in a carbon substrate. [12,13] The carbon substrate, as the host material, significantly affects the catalytic performance for the CO 2 RR.…”

“…[ 6–8 ] Especially, the Ni SACs, which are capable of selectively and efficiently reducing CO 2 to CO, have shown great potential for the CO 2 RR. [ 9–11 ]…”

Editorial: Defect chemistry in electrocatalysis

“…This special Research Topic includes four reviews and one original research. Defect engineering on carbon-based and metal-based single-atom electrocatalysts was highlighted by (Li et al, 2022b) along with the discussions of their characterization. Defective Noble metal and non-noble metal catalysts for electrocatalytic oxygen reduction reaction were discussed and summarized by (Mao et al, 2022) Based on experimental results and theoretical calculations, they clarified the structure-activity relationships between defect engineering and catalytic performance.…”