Highly Selective Carbon Dioxide Electroreduction on Structure-Evolved Copper Perovskite Oxide toward Methane Production

Abstract

Electrochemical carbon dioxide (CO 2 ) conversion is promising to balance the carbon cycle for human society. However, an efficient electrocatalyst is the key to determine the selective conversion of CO 2 toward valuable products. We report herein an efficient La 2 CuO 4 perovskite catalyst for electrochemical CO 2 reduction. A high Faradaic efficiency of 56.3% with a partial current density of 117 mA cm −2 is achieved for methane production over this perovskite catalyst at −1.4 V (vs RHE). The results demonstrate that the structural evolution of La 2 CuO 4 perovskite takes place simultaneously during the cathodic CO 2 reduction process. Theoretical investigations further unravel that the emerging Cu/La 2 CuO 4 interface accounts for the CO 2 methanation behaviors. This work provides an effective perovskite electrocatalyst for ambient CO 2 methanation and offers a valuable understanding of the structure evolution and surface reconstruction of precatalysts in catalytic reactions for energy-relevant technologies.

Facile Synthesis of Sub‐Nanometric Copper Clusters by Double Confinement Enables Selective Reduction of Carbon Dioxide to Methane

“…Thus, it is highly attractive to develop efficient and selective CO 2 RR electrocatalysts. Although Cu‐based electrocatalysts possess overwhelming advantages in regard to generate hydrocarbons than other metals, they still suffer from unsatisfactory selectivity towards specified hydrocarbons, such as CH 4 , which is an extensively used fuel. Recent density‐functional theory (DFT) calculations reveal a size‐dependent CO 2 RR performance on metallic Cu clusters, and the small‐sized Cu cluster with 13 atoms is more favorable for the generation of CH 4 , compared with other bigger clusters ranging from 55 to 561 atoms and bulk Cu .…”

Seeing is Believing: In Situ/Operando Optical Microscopy for Probing Electrochemical Energy Systems

“…Energy storage plays a crucial role in the future sustainable energy systems, considering the needs to balance the output fluctuations of renewable energy sources and support the prosperities of electronic devices and electric transportation. [ 1,2 ] Of various storage methods, electrochemical storage are a choice to meet the various energy demands of the society. [ 3,4 ] Over the past decades, great efforts have been made to optimize electrochemical energy systems (EESs) in terms of energy and power densities, lifespan, safety and costs, which are dependent on their internal physico‐chemical processes such as redox reactions, ion transports, formation of interstitial interfaces, degradation of components and by‐substances generation.…”

Facile Synthesis of Sub‐Nanometric Copper Clusters by Double Confinement Enables Selective Reduction of Carbon Dioxide to Methane

“…[2] Thus, it is highly attractive to develop efficient and selective CO 2 RR electrocatalysts. Although Cu-based electrocatalysts possess overwhelming advantages in regard to generate hydrocarbons than other metals, [3] they still suffer from unsatisfactory selectivity towards specified hydrocarbons, [4] such as CH 4 , which is an extensively used fuel. Recent density-functional theory (DFT) calculations reveal a size-dependent CO 2 RR performance on metallic Cu clusters, and the small-sized Cu cluster with 13 atoms is more favorable for the generation of CH 4 , compared with other bigger clusters ranging from 55 to 561 atoms and bulk Cu.…”