Lewis Acid Site-Promoted Single-Atomic Cu Catalyzes Electrochemical CO₂ Methanation

Abstract

Developing an efficient catalyst for the electrocatalytic CO 2 reduction reaction (CO 2 RR) is highly desired because of environmental and energy issues. Herein, we report a single-atomic-site Cu catalyst supported by a Lewis acid for electrocatalytic CO 2 reduction to CH 4 . Theoretical calculations suggested that Lewis acid sites in metal oxides (e.g., Al 2 O 3 , Cr 2 O 3 ) can regulate the electronic structure of Cu atoms by optimizing intermediate absorption to promote CO 2 methanation. Based on these theoretical results, ultrathin porous Al 2 O 3 with enriched Lewis acid sites was explored as an anchor for Cu single atoms; this modification achieved a faradaic efficiency (FE) of 62% at −1.2 V (vs RHE) with a corresponding current density of 153.0 mA cm −2 for CH 4 formation. This work demonstrates an effective strategy for tailoring the electronic structure of Cu single atoms for the highly efficient reduction of CO 2 into CH 4 . KEYWORDS: CO 2 RR, Lewis acid, Al 2 O 3 , single-atom Cu catalyst, CH 4

In situ construction of thiol-silver interface for selectively electrocatalytic CO2 reduction

“…Intensive consumption of traditional fossil fuels has been causing increased atmospheric carbon dioxide (CO 2 ), one of the main greenhouse gases, accounting for the continously going up of the global temperature [1][2][3]. Electrochemical catalysis provides a cost-effective and energy-efficient method for the mitigation of the environmental and energy concerns by directly converting CO 2 to valuable fuels and chemicals under ambient condition [4][5][6][7].…”

π-Adsorption promoted electrocatalytic acetylene semihydrogenation on single-atom Ni dispersed N-doped carbon

“…S2, ESI †). [26][27][28] The wavelet transform (WT) contour plot of SA-Ni-NC had only one intensity maximum at 5.6 ÅÀ1 , which was assigned to the Ni-N bonds rather than Ni-Ni scattering (8.2 ÅÀ1 ). These results clearly prove the dispersion of Ni-N 4 species in SA-Ni-NC (Fig.…”

Low‐dimensional material supported single‐atom catalysts for electrochemical CO2 reduction

“…In addition, they also demonstrated that the Lewis acid site in p‐Al 2 O 3 alters the electronic structure of Cu, which makes the single atom Cu more smoothly for producing CH 4 as the main product (Figure 5G,H). 95 In addition to LD metal oxide, the LD metal hydroxide is also used to support single atoms for ECR. Han et al 97 reported an a ‐Co(OH) 2 nanosheets supported Ir SAC for ECR, which shows the FE of CO could reach 97.6% with a TOF of 38,290 h −1 in aqueous electrolyte.…”

“…Color code: Cu, brick red; Al, purple; Cr, gray; O, red. Reproduced with permission 95 . Copyright 2021, American Chemical Society.…”