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 -