Defect Engineering Metal‐Free Polymeric Carbon Nitride Electrocatalyst for Effective Nitrogen Fixation under Ambient Conditions |
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| Authors: | Chade Lv Yumin Qian Chunshuang Yan Yu Ding Prof Yuanyue Liu Prof Gang Chen Prof Guihua Yu |
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| Institution: | 1. Materials Science and Engineering Program and Department of Mechanical Engineering, The University of Texas at Austin, Austin, TX, USA;2. MIIT Key Laboratory of Critical Materials Technology for, New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, P. R. China |
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| Abstract: | Electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions provides an intriguing picture for the conversion of N2 into NH3. However, electrocatalytic NRR mainly relies on metal‐based catalysts, and it remains a grand challenge in enabling effective N2 activation on metal‐free catalysts. Here we report a defect engineering strategy to realize effective NRR performance (NH3 yield: 8.09 μg h?1 mg?1cat., Faradaic efficiency: 11.59 %) on metal‐free polymeric carbon nitride (PCN) catalyst. Illustrated by density functional theory calculations, dinitrogen molecule can be chemisorbed on as‐engineered nitrogen vacancies of PCN through constructing a dinuclear end‐on bound structure for spatial electron transfer. Furthermore, the N?N bond length of adsorbed N2 increases dramatically, which corresponds to “strong activation” system to reduce N2 into NH3. This work also highlights the significance of defect engineering for improving electrocatalysts with weak N2 adsorption and activation ability. |
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| Keywords: | defect engineering electrocatalysis metal-free catalysts N2 activation nitrogen reduction reactions |
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