Activating the Ni‐Contenting Carbon Nanotube by Covalent Triazine Frameworks to Form Atomically Dispersed Ni Sites with Curvature Effect for Electrocatalytic CO 2 Reduction
N‐coordinated Ni sites (NiN x ) are effective catalysts for the electrochemical reduction of CO 2 to CO. In most researches, modulating the coordination environment of Ni atoms is focused on to improve electrochemical CO 2 reduction (ECR) performance. However, the influence of the carbon substrate...
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Published in | Small structures Vol. 5; no. 5 |
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Main Authors | , , , , , , |
Format | Journal Article |
Language | English |
Published |
01.05.2024
|
Online Access | Get full text |
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Summary: | N‐coordinated Ni sites (NiN
x
) are effective catalysts for the electrochemical reduction of CO
2
to CO. In most researches, modulating the coordination environment of Ni atoms is focused on to improve electrochemical CO
2
reduction (ECR) performance. However, the influence of the carbon substrate's structure on the intrinsic activity of NiN
x
is seldom investigated. The highly curved surface of carbon nanotubes (CNT) may provide a unique curvature effect on NiN
x
. It is found that the Ni residues in CNT can be atomized to form NiN
x
sites on the surface of CNT (Ni‐N/CNT@covalent triazine framework [CTF]) through high‐temperature pyrolysis, using a soluble CTF nanosheet as N precursor. The π‐conjugated and ultrathin 2D structure of CTF enables closer interfacial contact between CTF and CNT, which avoids the formation of a thick carbon layer to maximize the curvature effect. Theoretical data reveal that the NiN
3
configuration may act as a highly active ECR site, and the curvature effect from CNT can further tune the electronic structure of NiN
3
, thus improving the ECR kinetics. The Ni‐N/CNT@CTF‐based flow‐cell electrolyzer exhibits a j
CO
of 201 mA cm
−2
at −0.9 V with a high FE
CO
of 98%. |
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ISSN: | 2688-4062 2688-4062 |
DOI: | 10.1002/sstr.202300500 |