硼
催化作用
路易斯酸
氮气
无机化学
氨
化学
金属
吸附
法拉第效率
产量(工程)
过渡金属
碳纤维
材料科学
电化学
电极
有机化学
物理化学
冶金
复合材料
复合数
作者
Bin Chang,Lili Li,Danni Shi,Huaidong Jiang,Zizheng Ai,Shouzhi Wang,Yongliang Shao,Jianxing Shen,Yongzhong Wu,Yanlu Li,Xiaopeng Hao
标识
DOI:10.1016/j.apcatb.2020.119622
摘要
From a thermodynamic point of view, electrocatalytic nitrogen reduction reaction (NRR) is possible for the carbon-based metal-free catalysts, which are gradually becoming a class of potential alternatives to metal-based catalysts. However, the clarification of true active sites and corresponding exact catalytic mechanism of metal-free catalysts is urgently required. Taking full advantage of boron “Lewis acid”, a series of boron carbonitride (BCN) materials were designed and synthesized and the “Lewis acid catalysis” sites were tuned easily by adjusting the relative contents of boron and nitrogen atoms. Boron-enriched BCN exhibited outstanding NRR performance with an ammonia yield of −8.39 μg h−1.cm−2cat. (−41.9 μg h−1.mg−1cat.) and Faradaic efficiency of −9.87 %, together with excellent stability. Density functional theory calculations indicate that the boron sites of BCN enable the low energy barrier of the NRR rate-determining steps and the spontaneity of nitrogen adsorption. Our philosophy opens a new possible avenue to explore high-performance metal-free materials for nitrogen activation.
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