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Implanting Numerous Hydrogen‐Bonding Networks in a Cu‐Porphyrin‐Based Nanosheet to Boost CH 4 Selectivity in Neutral‐Media CO 2 Electroreduction
Author(s) -
Wang YiRong,
Liu Ming,
Gao GuangKuo,
Yang YiLu,
Yang RuXin,
Ding HuiMin,
Chen Yifa,
Li ShunLi,
Lan YaQian
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202108388
Subject(s) - nanosheet , porphyrin , electrochemistry , catalysis , selectivity , materials science , electrocatalyst , hydrogen , nanotechnology , proton , chemistry , photochemistry , electrode , organic chemistry , physics , quantum mechanics
The exploration of novel systems for the electrochemical CO 2 reduction reaction (CO 2 RR) for the production of hydrocarbons like CH 4 remains a giant challenge. Well‐designed electrocatalysts with advantages like proton generation/transferring and intermediate‐fixating for efficient CO 2 RR are much preferred yet largely unexplored. In this work, a kind of Cu‐porphyrin‐based large‐scale (≈1.5 μm) and ultrathin nanosheet (≈5 nm) has been successfully applied in electrochemical CO 2 RR. It exhibits a superior FECH4of 70 % with a high current density (−183.0 mA cm −2 ) at −1.6 V under rarely reported neutral conditions and maintains FECH4>51 % over a wide potential range (−1.5 to −1.7 V) in a flow cell. The high performance can be attributed to the construction of numerous hydrogen‐bonding networks through the integration of diaminotriazine with Cu‐porphyrin, which is beneficial for proton migration and intermediate stabilization, as supported by DFT calculations. This work paves a new way in exploring hydrogen‐bonding‐based materials as efficient CO 2 RR catalysts.

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