Enriching Reaction Intermediates in Multishell Structured Copper Catalysts for Boosted Propanol Electrosynthesis from Carbon Monoxide

Abstract

Fine-tuned catalysts that alter the diffusion kinetics of reaction intermediates is of great importance for achieving high-performance multicarbon (C 2+ ) product generation in carbon monoxide (CO) reduction. Herein, we conduct a structural design based on Cu 2 O nanoparticles and present an effective strategy for enhancing propanol electrosynthesis from CO. The electrochemical characterization, operando Raman monitoring, and finite-element method simulations reveal that the multishell structured catalyst can realize the enrichment of C 1 and C 2 intermediates by nanoconfinement space, leading to the possibility of further coupling. Consequently, the multishell copper catalyst realizes a high Faraday efficiency of 22.22 ± 0.38% toward propanol at the current density of 50 mA cm −2 .

Cu-based catalyst designs in CO2 electroreduction: precise modulation of reaction intermediates for high-value chemical generation

“…80 Occasionally, to investigate the specific influence of a non-electrochemically active area factor, the ECSA values of both the experimental and control groups are adjusted in a manner nearly identical to control the active site variables. 70,81 The turnover number (TON), representing the product yield per unit catalyst, and turnover frequency (TOF), representing the product yield per unit catalyst over a specific time period, are additional parameters that can offer insights into catalyst utilization and stability. These two physical parameters are commonly employed to assess both the catalytic performance and the visible light harvesting capacity of catalysts in photocatalytic systems.…”

“…Additionally, the hierarchical structure of the catalyst influences the residence and reaction pathways of intermediates, as well as the kinetics of the protonation process. 81,146,161 Zhang et al developed multi-shelled CuO microboxes and investigated the effect of the hierarchical structure on active sites' exposure and the adsorption of carbonate intermediates. 162 They discovered that small and uniform multi-shelled CuO microboxes exhibited significantly improved performance in converting CO 2 into C 2 H 4 , which was attributed to the enrichment of *CO.…”

Multi‐Shell Copper Catalysts for Selective Electroreduction of CO2 to Multicarbon Chemicals

“…Previous studies of Cu catalysts briefly explored the confinement effect to a certain extent. [17] However, most of these studies have focused on porous structures at relatively low current densities. [17] Thorough examinations of investigations involving complicated structures and high current density are crucial for the future implementation of this technology.…”

Enrichment Strategies for Efficient CO2 Electroreduction in Acidic Electrolytes

“…Numerous studies indicate that increasing reactant and intermediate concentration boosts CO 2 RR [8] . This is mainly due to the high concentration of reactants and intermediates can enhance the probability of molecular collision and activation, thereby significantly accelerating the reaction rate and promoting selectivity [9] . As a result, enriching the reactants and intermediates in nearby active sites provides a promising avenue for enhancing the overall performance of acidic CO 2 RR.…”

“…[8] This is mainly due to the high concentration of reactants and intermediates can enhance the probability of molecular collision and activation, thereby significantly accelerating the reaction rate and promoting selectivity. [9] As a result, enriching the reactants and intermediates in nearby active sites provides a promising avenue for enhancing the overall performance of acidic CO 2 RR. Based on this, much work has been devoted to developing enrichment strategies in acidic CO 2 RR, thus a comprehensive and timely review is essential.…”