Rational Design of Heterogeneous Dual-Atom Catalysts for CO₂ Electroreduction Reactions

Abstract

One of the strategies to mitigate the concentration of CO 2 in the atmosphere and reduce the global warming effect is to capture CO 2 and convert it to synthetic fuels and fine chemicals. Although CO 2 is structurally and chemically stable, the electrochemical transformation has attracted much attention because it offers mild reaction conditions regarding temperature, pressure, and process controllability. Among various electrocatalysts, dualatom catalysts (DACs) have been extensively developed in the past few years due to their unique features for the electrochemical reactions of small molecules. The catalytic activity of DACs in the electrochemical CO 2 reduction reaction (eCO 2 RR) has surpassed single-atom catalysts (SACs) by providing a higher metal loading, two active sites (cf. one active site for SACs), a synergistic effect of adjacent metal atoms, the possibility of tuning the electronic state (adjusting the d-band center), and more possible configuration modes (side-on and side-bridge) for adsorption of CO 2 (cf. only end-on and end-bridge modes for SACs). As a result, both higher reactivity and selectivity in eCO 2 RR can be achieved by breaking scaling relationships with more possible interactions between intermediates and active sites. This review highlights and discusses the recent progress in applying homo-and heteronuclear DACs for eCO 2 RR focusing on the synthesis, characterization, and electrochemical catalytic performance.

Deep learning of electrochemical CO2 conversion literature reveals research trends and directions

“…In comparison to SACs, they have not only a similar ability to utilize almost 100% of the catalyst atoms but also much enhanced electronic property, improved activity, and selectivity. 57 Upon examining the 3153 literature we collected, it was verified that there are 7 papers focusing on dual-atom catalysts. We searched Web of Science for dual-atom catalysts to collect the most recent developments in the field.…”

Hollow carbon-based materials for electrocatalytic and thermocatalytic CO2 conversion

“…However, some important aspects still need to be further investigated: (1) the coordination environment has great impact on the electronic structure of SACs, so unveiling the relationship between the coordination number or connecting heteroatom type of SACs and eCO 2 RR activity is important; (2) at present, most of the SACs syntheses are still at the laboratory stage; a universal approach for large-scale SACs production is required to meet the demands of practical applications; 119 (3) some studies suggest that single-atom site conguration only shows high reactivity in the primary reaction process and is inadequate for the subsequent catalytic reaction steps involving multiple electron transfer and intermediate conversion, accordingly, developing novel catalysts with dual atomic sites may overcome this limitation. 120,121 2.2.3 Metal nanoparticles modication. Metal nanoparticles (NPs) modied HSC material as active and reusable catalysts have attracted wide interest in the eld of catalytic CO 2 reduction, in which metal NPs act as the active sites.…”

Highly efficient CO2 electrochemical reduction on dual metal (Co–Ni)–nitrogen sites

“…This concept is further explored in recent comprehensive reviews, highlighting the advancements and potential of DASCs in various applications. 24–29 Nitrogenated carbon-based DASCs have demonstrated advantages in improving CO 2 ECR performance. 30 For example, the N-bridged Co–N–Ni bimetallic catalyst achieves a CO faradaic efficiency of 96.4%, significantly higher than Co–N 4 at 61.5% and Ni–N 4 at 45.0%, respectively.…”