Stabilizing Cu⁰–Cu⁺ sites by Pb-doping for highly efficient CO₂ electroreduction to C₂ products

Abstract

The electrochemical CO2 reduction reaction (CO2RR) can convert CO2 to C2 hydrocarbons and oxygenates over Cu-based catalysts, which has great potential to store renewable energy and close the carbon cycle....

Critical Role of Cu Nanoparticle-Loaded Cu(100) Surface Structures on Structured Copper-Based Catalysts in Boosting Ethanol Generation in CO2 Electroreduction

“…Therefore, it is suggested that the unique flower-like micro/nanostructure of Cu-F-M and Cu-F catalysts may not only provide a larger electrochemically active surface area but also induce the formation of CuNPs@Cu(110) surface structures during electrochemical activation, thereby improving CO 2 conversion and increasing selectivity to specific products (e.g., ethanol) in the eCO 2 RR. , As a result, the Cu-F-M catalyst exhibits a significantly higher selectivity of C 2+ products (including ethanol) in the eCO 2 RR (Figure b), in comparison to the Cu-P-M catalyst. On the other hand, previous studies have highlighted the key role of Cu + species in enhancing *CO adsorption and C–C coupling to facilitate the generation of C 2+ products in the eCO 2 RR. − Interestingly, despite both the collapse of flower-like morphology and the absence of Cu + species (Figures S9 and S11) on the spent Cu-F-M after stability evaluation, the spent Cu-F-M electrocatalyst with remaining CuNPs@Cu(100) surface structures (Figures S12–14) still exhibits high ethanol selectivity. The above results sufficiently demonstrate that CuNPs@Cu(100) surface structures in the Cu-F-M catalyst play a decisive role in promoting the production of C 2+ products in the eCO 2 RR.…”

Active hydrogen-controlled CO₂/N₂/NO_x electroreduction:From mechanism understanding to catalyst design

“…[40][41][42] Currently, a wide range of products has been produced through diverse reaction systems, including CO, formic acid, CH 4 , CH 3 OH, ethylene, ethane, ethanol and other C 2+ products. [43][44][45][46][47] As is shown in Figure 1B, after being absorbed onto electrode surface, the CO 2 molecule is then transformed into CO 2 ˙− or * CO intermediates over different electrode materials. 48 These two intermediates could directly desorb from the electrode to yield the 2-electron transfer products, CO and HCOOH.…”

Enhancing CO2 Electroreduction Performance through Si-Doped CuO: Stabilization of Cu+/Cu0 Sites and Improved C2 Product Selectivity

“…31,32 Previous work proposed the significance of localized interface bonding between active sites and support, facilitating the stabilization of highly reactive, coordinatively unsaturated cations. 25,29−31 Especially, some studies have incorporated pblock metals such as Gd, 33 Pb, 34 and Sn 35 to stabilize Cu + species, significantly improving CO 2 reduction performance. Among various supports, silicon (Si) oxide stands out for its exceptional ability to stabilize reaction intermediates and transition states, courtesy of its influence on solvent dynamics.…”

“…In Cu-based catalyst, the reactivity and catalytic efficacy are profoundly influenced by the structural and chemical attributes of the surface and interfaces, which are the primary locales for CO 2 electroreduction. − When CuO x are juxtaposed onto the other oxides, the resulting oxide–oxide interface markedly impacts their structural integrity and catalytic behavior. , Previous work proposed the significance of localized interface bonding between active sites and support, facilitating the stabilization of highly reactive, coordinatively unsaturated cations. ,− Especially, some studies have incorporated p-block metals such as Gd, Pb, and Sn to stabilize Cu + species, significantly improving CO 2 reduction performance. Among various supports, silicon (Si) oxide stands out for its exceptional ability to stabilize reaction intermediates and transition states, courtesy of its influence on solvent dynamics.…”