Atomically dispersed Lewis acid sites boost 2-electron oxygen reduction activity of carbon-based catalysts

Abstract

Elucidating the structure-property relationship is crucial for the design of advanced electrocatalysts towards the production of hydrogen peroxide (H2O2). In this work, we theoretically and experimentally discovered that atomically dispersed Lewis acid sites (octahedral M–O species, M = aluminum (Al), gallium (Ga)) regulate the electronic structure of adjacent carbon catalyst sites. Density functional theory calculation predicts that the octahedral M–O with strong Lewis acidity regulates the electronic distribution of the adjacent carbon site and thus optimizes the adsorption and desorption strength of reaction intermediate (*OOH). Experimentally, the optimal catalyst (oxygen-rich carbon with atomically dispersed Al, denoted as O-C(Al)) with the strongest Lewis acidity exhibited excellent onset potential (0.822 and 0.526 V versus reversible hydrogen electrode at 0.1 mA cm−2 H2O2 current in alkaline and neutral media, respectively) and high H2O2 selectivity over a wide voltage range. This study provides a highly efficient and low-cost electrocatalyst for electrochemical H2O2 production.

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

“…However, it has received little attention in the electrocatalytic CO 2 RR, possibly because of its insulating properties. Herein, we indeed find that loading Cu SA onto commercial Al 2 O 3 and Cr 2 O 3 Lewis acids 44 can significantly improve the activity of CO 2 methanation, and the samples with stronger Lewis acidity perform better. Moreover, when Cu SAs are supported by ultrathin, porous Al 2 O 3 , the resulting catalyst exhibits a high selectivity of 62% toward CH 4 with a corresponding current density of 153.0 mA cm −2 at −1.2 V (vs RHE).…”

Computational Screening of Single-Metal-Atom Embedded Graphene-Based Electrocatalysts Stabilized by Heteroatoms

“…It has already been reported that Co-N-C is a good catalyst for ORR through previous DFT computational screening studies and experimental validation ( Zheng et al, 2016 ). Using O-dopant as a heteroatom has been reported for an O-C(Al) catalyst synthesized by using isomorphic metal-organic framework MIL-53(Al, Ga) ( Yang et al, 2020 ) or a multiwalled carbon nanotube catalyst ( Jiang et al, 2019 ). Moreover, the role of O-dopant heteroatoms has been elucidated in Co-NG(O) catalysts ( Jung et al, 2020 ).…”

Gd-doped CuBi2O4/CuO heterojunction film photocathodes for photoelectrochemical H2O2 production through oxygen reduction

“…As a kind of valuable chemicals and potential energy carriers, H2O2 has widely been used in chemical industrial, green synthesis, environmental treatment, and fuel cell technology [16]. The annual global production of H2O2 will increase to 6 million tons by 2024 [17]. At present, most of H2O2 is synthesized at an industrial scale through a well-established anthraquinone oxidation process.…”