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Polymeric carbon nitride with frustrated Lewis pair sites for enhanced photofixation of nitrogen
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020-06-17 , DOI: 10.1039/d0ta03914d
Yue Ran 1, 2, 3, 4, 5 , Xuelian Yu 1, 2, 3, 4, 5 , Jianqiao Liu 1, 2, 3, 4, 5 , Jiayi Cui 1, 2, 3, 4, 5 , Jiangpeng Wang 1, 2, 3, 4, 5 , Lin Wang 1, 2, 3, 4, 5 , Yihe Zhang 1, 2, 3, 4, 5 , Xu Xiang 6, 7, 8, 9 , Jinhua Ye 10, 11, 12, 13, 14
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2020-06-17 , DOI: 10.1039/d0ta03914d
Yue Ran 1, 2, 3, 4, 5 , Xuelian Yu 1, 2, 3, 4, 5 , Jianqiao Liu 1, 2, 3, 4, 5 , Jiayi Cui 1, 2, 3, 4, 5 , Jiangpeng Wang 1, 2, 3, 4, 5 , Lin Wang 1, 2, 3, 4, 5 , Yihe Zhang 1, 2, 3, 4, 5 , Xu Xiang 6, 7, 8, 9 , Jinhua Ye 10, 11, 12, 13, 14
Affiliation
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The bottleneck of photocatalytic nitrogen fixation lies in the rate-limiting reductive activation of robust N
N triple bonds with high bond energy. Herein, polymeric carbon nitride with frustrated-Lewis-pairs was constructed by intercalation of electron-deficient boron (B) into metal-free carbon nitride. NH3-temperature programmed desorption (TPD) and pyridine-adsorption diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results demonstrated that B heteroatoms (Lewis acid) and proximal amino groups (Lewis base) were more likely to form frustrated Lewis pairs, which would capture, activate and reduce N2 to NH3 through a “pull–push” effect. Molybdenum-based oxide was further employed as a co-catalyst to improve the charge separation efficiency of site-engineered photocatalysts. The synergistic effect between intercalated B and defective MoO2 resulted in an 8-fold increased photoactivity of carbon nitride for N2 fixation. This work provides a new avenue for the rational design and engineering of frustrated Lewis pair sites on polymeric photocatalysts toward efficient N2 fixation.
中文翻译:
具有受阻路易斯对位的聚合碳氮化物,可增强氮的光固定性
光催化固氮的瓶颈在于
具有高键能的鲁棒N N三键的限速还原活化。在此,通过将缺电子的硼(B)嵌入无金属的氮化碳中,构造了具有沮丧的路易斯对的高分子氮化碳。NH 3-程序升温脱附(TPD)和吡啶吸附漫反射红外傅里叶变换光谱(DRIFTS)结果表明,B杂原子(路易斯酸)和近端氨基(路易斯碱)更可能形成受挫的路易斯对,捕获,活化N 2并将其还原为NH 3通过“推拉”效果。钼基氧化物还被用作助催化剂,以提高现场设计的光催化剂的电荷分离效率。插层B和有缺陷的MoO 2之间的协同作用导致氮化碳固定N 2的光活性增加了8倍。这项工作为合理设计和工程化高分子光催化剂上受挫的路易斯对位实现有效的N 2固定化提供了新途径。
更新日期:2020-07-07
![[triple bond, length as m-dash]](https://www.rsc.org/images/entities/char_e002.gif)
中文翻译:
![](https://scdn.x-mol.com/jcss/images/paperTranslation.png)
具有受阻路易斯对位的聚合碳氮化物,可增强氮的光固定性
光催化固氮的瓶颈在于
![[三重键,长度为m-破折号]](https://www.rsc.org/images/entities/char_e002.gif)