Structural rule of N-coordinated single-atom catalysts for electrochemical CO₂ reduction

Abstract

Metal single-atom catalysts (SACs) on nitrogen-doped carbons exhibit an attractive prospect in catalysis. However, how to quickly collocate various metal centers with diversified N-coordination topologic structures to maximize the catalytic...

Emerging materials for electrochemical CO2reduction: progress and optimization strategies of carbon-based single-atom catalysts

“…7d). 189 The results demonstrated that TM SACs on GN 2 with the least N coordination achieved excellent CO 2 RR catalytic activity and selectivity.…”

Oriented design of triple atom catalysts for electrocatalytic nitrogen reduction with the genetic-algorithm-based global optimization method driven by first principles calculations

“…Here, the cohesive energy (E c ) of metals, which only depends on the metal itself and can directly describe the binding strength of metal centers, is selected as the descriptor to assess the activity of catalysts for the NRR, which has been successfully used to understand the transition metal single-atom catalysts. 26 The detailed E c of transition metals are listed in Table S6. † 3.2.1 Activity trends.…”

“…That is to say, the stronger binding strength (i.e., more negative E c ) of active metal centers corresponds to the usually stronger adsorption of intermediates. 26 With these obtained relationships, we can then gain the free energy change (DG i , see calculation details in the table) of each elementary step of the NRR on the SAS, DAS and TAS, respectively. Accordingly, the curves of the limiting potential (U NRR ¼ ÀDG i(max) ) of the NRR on the SAS, DAS and TAS, that are oen used to evaluate the intrinsic activity of electrocatalysts, can be built up (Fig.…”

“…For example, Sun et al, Qiao et al and Wang et al investigated the activity trends of single-atom catalysts for the NRR and CO 2 RR, respectively, that guide their rational design. [24][25][26] However, owing to the single-atom structural feature (SAS), the ideal catalytic ability of single-atom catalysts could be restricted by the limited coordination ability of the metal center. 27 To achieve higher catalytic performance, a strategy to explore double-and triple-atom structures (DASs and TASs) as the active centers has been put forward, which could more exibly tune the adsorption strength and break the scaling relationships of different intermediates on single-atom catalysts.…”

First-principles study of CO2 hydrogenation to formic acid on single-atom catalysts supported on SiO2

“…Guo et al realized low-temperature CO 2 methanation over CeO 2 -supported Ru single-atoms, with a turnover frequency of 7.41 × 10 −3 s −1 at 463 K. 16 Recently, transition metal single-atoms anchored on graphene and silicomolybdic were reported to show excellent CO 2 electroreduction activity. 17,18…”