Facilitating nitrogen accessibility to boron-rich covalent organic frameworks via electrochemical excitation for efficient nitrogen fixation

Covalent organic frameworks with abundant active sites are potential metal-free catalysts for the nitrogen reduction reaction. However, the utilization ratio of active sites is restricted in an actual reaction process due to the limited nitrogen transport. Here, we demonstrate that facilitating the...

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Published inNature communications Vol. 10; no. 1; pp. 3898 - 9
Main Authors Liu, Sisi, Wang, Mengfan, Qian, Tao, Ji, Haoqing, Liu, Jie, Yan, Chenglin
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 29.08.2019
Nature Publishing Group
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Summary:Covalent organic frameworks with abundant active sites are potential metal-free catalysts for the nitrogen reduction reaction. However, the utilization ratio of active sites is restricted in an actual reaction process due to the limited nitrogen transport. Here, we demonstrate that facilitating the N 2 accessibility to boron-rich covalent organic frameworks through electrochemical excitation can achieve highly efficient nitrogen reduction activity. Simulations show that the boron sites are bonded with nitrogenous species under electrochemical condition and the resultant amorphous phase of covalent organic frameworks has much stronger affinity toward N 2 to enhance the molecule collision. Combined with experimental results, the excitation process is confirmed to be a virtuous cycle of more excited sites and stronger N 2 affinity, which continuously proceed until the whole system reaches the optimum reaction status. As expected, the electrochemically excited catalyst delivers significantly enhanced reaction activity, with a high Faradaic efficiency of 45.43%. Covalent organic frameworks are potential catalysts for nitrogen reduction, but limited nitrogen transport restricts the utilization ratio of active sites. Here, the authors demonstrate that electrochemical excitation of covalent organic frameworks can lead to efficient nitrogen reduction.
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ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-019-11846-x