Facilitating Nitrogen Accessibility to Boron-rich Covalent Organic Frameworks Via Electrochemical Excitation for Efficient Nitrogen Fixation

Overview

Journal Nat Commun

Specialty Biology

Date 2019 Aug 31

PMID 31467283

Citations 13

Authors

Sisi Liu

Mengfan Wang

Tao Qian

Haoqing Ji

Jie Liu

Chenglin Yan

Affiliations

Soon will be listed here.

Abstract

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 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 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 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%.

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