Quasi-Phthalocyanine Conjugated Covalent Organic Frameworks with Nitrogen-Coordinated Transition Metal Centers for High-Efficiency Electrocatalytic Ammonia Synthesis.
basic_science · Level V
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- Record sourced from PubMed, PMID 34935367.
- Also identified by DOI 10.1021/acs.nanolett.1c04009.
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Abstract
Developing high-performance nitrogen reduction reaction (NRR) electrocatalysts is an ongoing challenge. Herein, we report a pyrolysis-free synthetic method for introducing ordered quasi-phthalocyanine N-coordinated transition metal (Ti, Cu, or Co) centers into a conjugated two-dimensional (2D) covalent organic framework (COF) for enhanced NRR performance. Detailed experiments and characterizations revealed that the NRR activity of Ti-COF was clearly better than that of Cu-COF and Co-COF, because of the superior abilities of Ti metal centers in activating inert N<sub>2</sub> molecules and suppressing the hydrogen evolution reaction (HER). The resulting Ti-COF exhibits a high NH<sub>3</sub> yield of 26.89 μg h<sup>-1</sup> mg<sup>-1</sup><sub>cat.</sub> and a Faradaic efficiency of 34.62% for NRR. Density functional theory (DFT) calculations verify that Ti-COF can effectively adsorb and activate N<sub>2</sub> molecules and inhibit HER compared with Cu-COF, Co-COF, and pristine COF catalysts. This work opens a new avenue for developing 2D-COF materials that contain abundant coordinated transition metal centers toward electrocatalytic NRR.