Defect Engineering Metal‐Free Polymeric Carbon Nitride Electrocatalyst for Effective Nitrogen Fixation under Ambient Conditions,Angewandte Chemie International Edition

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Defect Engineering Metal‐Free Polymeric Carbon Nitride Electrocatalyst for Effective Nitrogen Fixation under Ambient Conditions
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-07-15 , DOI: 10.1002/anie.201806386
Chade Lv _{1,

2} , Yumin Qian ₁ , Chunshuang Yan _{1,

2} , Yu Ding ₁ , Yuanyue Liu ₁ , Gang Chen ₂ , Guihua Yu ₁

Affiliation

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⁻¹_cat., 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.

中文翻译：

缺陷工程无金属聚合氮化碳电催化剂，可在环境条件下有效固氮

在环境条件下的电催化氮还原反应（NRR）为将N ₂转化为NH ₃提供了有趣的画面。但是，电催化NRR主要依赖于金属基催化剂，在无金属催化剂上实现有效的N ₂活化方面仍然是一个巨大的挑战。在这里，我们报告了一种缺陷工程策略，以实现有效的NRR性能（NH ₃产量：8.09μgh ^-1 mg ^-1_cat。，法拉第效率：11.59％）在不含金属的聚合氮化碳（PCN）催化剂上。通过密度泛函理论计算可以说明，通过构建用于空间电子转移的双核末端键合结构，可以将二氮分子化学吸附在PCN的工程化氮空位上。此外，被吸附的N ₂的N-N键长显着增加，这对应于“强活化”系统将N ₂还原为NH ₃。这项工作还强调了缺陷工程对改善具有弱N ₂吸附和活化能力的电催化剂的重要性。

更新日期：2018-07-15

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