Mesopore-Augmented Electrochemical CO₂ Reduction on Nitrogen-Doped Carbon

TY - JOUR

T1 - Mesopore-Augmented Electrochemical CO2 Reduction on Nitrogen-Doped Carbon

AU - Han, Xu

AU - Zhang, Ting

AU - Biset-Peiró, Martí

AU - Roldan, Alberto

AU - Ceccato, Marcel

AU - Lock, Nina

AU - Pedersen, Steen Uttrup

AU - Morante, Joan Ramon

AU - Arbiol, Jordi

AU - Daasbjerg, Kim

N1 - © 2024 Wiley‐VCH GmbH.

PY - 2024/11/22

Y1 - 2024/11/22

N2 - The electrochemical carbon dioxide reduction reaction (eCO2RR) using nitrogen-doped carbon (N-C) materials offers a promising and cost-effective approach to global carbon neutrality. Regulating the porosity of N-C materials can potentially increase the catalytic performance by suppressing the concurrence of the hydrogen evolution reaction (HER). However, the augmentation of porosity usually alters the active sites or the chemical composition of catalysts, resulting in intertwined influences of various structural factors and catalytic performance. In this study, incorporating secondary carbon sources into the metal-organic framework (MOF) precursor through nanocasting aimed to selectively enhance the mesoporous structure, allowing for deciphering this effect from other changes in the catalyst composition. Consequently, the developed N-C catalyst exhibited a significant surface area with abundant mesopores, leading to a maximum Faradaic efficiency (FE) for carbon monoxide (CO) of 95% at -0.50 V versus the reversible hydrogen electrode (vs. RHE). Furthermore, the FE for CO is enhanced across a wide potential range, surpassing previously reported metal-free N-C eCO2RR catalysts. The investigation reveals that constructing mesoporous structures can induce excellent CO2 catalysis by enhancing the accessibility of active sites while establishing an elevated local pH at these sites.

AB - The electrochemical carbon dioxide reduction reaction (eCO2RR) using nitrogen-doped carbon (N-C) materials offers a promising and cost-effective approach to global carbon neutrality. Regulating the porosity of N-C materials can potentially increase the catalytic performance by suppressing the concurrence of the hydrogen evolution reaction (HER). However, the augmentation of porosity usually alters the active sites or the chemical composition of catalysts, resulting in intertwined influences of various structural factors and catalytic performance. In this study, incorporating secondary carbon sources into the metal-organic framework (MOF) precursor through nanocasting aimed to selectively enhance the mesoporous structure, allowing for deciphering this effect from other changes in the catalyst composition. Consequently, the developed N-C catalyst exhibited a significant surface area with abundant mesopores, leading to a maximum Faradaic efficiency (FE) for carbon monoxide (CO) of 95% at -0.50 V versus the reversible hydrogen electrode (vs. RHE). Furthermore, the FE for CO is enhanced across a wide potential range, surpassing previously reported metal-free N-C eCO2RR catalysts. The investigation reveals that constructing mesoporous structures can induce excellent CO2 catalysis by enhancing the accessibility of active sites while establishing an elevated local pH at these sites.

KW - CO electroreduction

KW - CO generation

KW - mesopores

KW - metal–organic frameworks (MOFs)

KW - nitrogen-doped carbon (N–C)

UR - http://www.scopus.com/inward/record.url?scp=85209724053&partnerID=8YFLogxK

U2 - 10.1002/smll.202406883

DO - 10.1002/smll.202406883

M3 - Journal article

C2 - 39575471

SN - 1613-6810

JO - Small (Weinheim an der Bergstrasse, Germany)

JF - Small (Weinheim an der Bergstrasse, Germany)

IS - 2406883

M1 - 2406883

ER -