Catalytic mechanism and activity of N2 reduction on boron-decorated crystalline carbon nitride
Catalytic mechanism and activity of N2 reduction on boron-decorated crystalline carbon nitride
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DOI：
10.1088/2053-1583/ac953a
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发表时间：
2022-09
期刊：
影响因子：
5.5
通讯作者：
Meifang Zheng;Xu Cai;Yi Li;K. Ding;Yong-Fan Zhang;Wenkai Chen;Chenghua Sun;Wei-hui Lin
中科院分区：
文献类型：
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作者：
Meifang Zheng;Xu Cai;Yi Li;K. Ding;Yong-Fan Zhang;Wenkai Chen;Chenghua Sun;Wei-hui Lin
开发高效、低成本和生态友好的固氮催化剂至关重要，并为传统的Haber-Bosch工艺提供了替代方法。然而，目前对热还原固氮催化剂的研究主要集中在含金属催化剂上，对热还原过程的微观机理研究还很有限。本文探索了一种经济的无金属硼原子修饰的聚三嗪酰亚胺（B/PTI），一种结晶氮化碳，作为一种优良的热固氮催化剂，并提出了N2热还原反应（NTRR）的底物-氢机理。我们的研究结果表明，底物氢作为氢源可以促进加氢过程的活化势垒为0.56 eV，显着低于已报道的NTRR催化剂。重要的是，B/PTI表现出与Fe、Ru和Ti催化剂相当的高转换频率。我们的工作为NTRR机理提供了新的见解，并为可持续的氨合成提供了替代解决方案。
The development of efficient, low-cost, and eco-friendly catalysts for nitrogen fixation is essential and provides an alternative method to the traditional Haber–Bosch process. However, studies on thermal catalyst of nitrogen fixation mainly focus on metal-containing, and the microscopic mechanism of thermal reduction process is still limited. Herein, we explored an economic metal-free boron atom decorated poly(triazine imide) (B/PTI), a crystalline carbon nitride, as an excellent thermal catalyst of nitrogen fixation and proposed a substrate-hydrogen mechanism for the N2 thermal reduction reaction (NTRR). Our results reveal that the substrate hydrogen as the hydrogen source can promote the hydrogenation process with activation barrier of 0.56 eV, significantly lower than that of reported NTRR catalysts. Importantly, the B/PTI exhibits high turnover frequency, which is comparable to Fe, Ru, and Ti catalysts. Our work offers new insights into NTRR mechanism and provides an alternative solution for the sustainable ammonia synthesis.