Metal Oxides Mediated Subtractive Manufacturing of Two-Dimensional Carbon Nitride for High Efficiency and High Yield Photocatalytic H2 Evolution.
Metal Oxides Mediated Subtractive Manufacturing of Two-Dimensional Carbon Nitride for High Efficiency and High Yield Photocatalytic H2 Evolution.
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DOI：
10.1021/acsnano.9b04443
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发表时间：
2019-09
期刊：
影响因子：
17.1
通讯作者：
Hui Xu;X. She;Ting Fei;Yanhua Song;Daobin Liu;Hongping Li;Xiaofei Yang;Jinman Yang;Hua-ming L
中科院分区：
文献类型：
--
作者：
Hui Xu;X. She;Ting Fei;Yanhua Song;Daobin Liu;Hongping Li;Xiaofei Yang;Jinman Yang;Hua-ming L
g-C3 N4是一种很有前途的可见光驱动的光催化剂，但其光催化性能的实现主要受到光生载流子分离效率低和电荷转移动力学缓慢的限制。二维（2D）g-C3 N4可以显著提高电荷产生、转移和分离效率。二维g-C3 N4基Z型异质结构可以进一步增强载流子分离，同时提高氧化还原能力，从而进一步提高光催化性能。在这里，我们报告了一个过渡金属氧化物（TMO）介导的减成制造过程中的大规模合成2D g-C3 N4和同时形成2D/2D TMO/g-C3 N4 Z-计划异质结。TMO用作催化剂以促进本体g-C3 N4在潮湿空气存在下的水解反应，形成2D g-C3 N4。所得的2D/2D TMO/g-C3 N4催化剂，特别是2D/2D Co 3 O 4/g-C3 N4，由于电子-空穴对复合的抑制和增强的氧化还原能力而表现出高效率和高产率的光催化放氢。2D/2D Co 3 O 4/g-C3 N4在λ > 400 nm范围内光催化放氢速率约为370 μmol h-1。2D/2D Co 3 O 4/g-C3 N4催化剂在405 nm处的外量子效率（EQE）达到53.6%，是g-C3 N4基催化剂中最高的。
The g-C3N4 is a promising viable-light-driven photocatalyst for H2 evolution reaction, however, the achievement of the high photocatalytic performance is primarily limited by the low separation efficiency of the photogenerated charge carriers and partly restricted by the slow kinetics of charge transfer. Two-Dimensional (2D) g-C3N4 can significantly improve the charge generation, transfer, and separation efficiencies. 2D g-C3N4 based Z-scheme heterostructure can further enhance charge carriers separation and simultaneously increase the redox ability thereby further boosting the photocatalytic performance. Here, we report a transition metal oxide (TMO) mediated subtractive manufacturing process towards large scale synthesis of 2D g-C3N4 and the simultaneous formation of 2D/2D TMO/g-C3N4 Z-scheme heterojunction. The TMOs serve as catalysts to facilitate the hydrolysis reaction of the bulk g-C3N4 in the presence of moist air, forming 2D g-C3N4. The resulting 2D/2D TMO/g-C3N4 catalysts, particularly 2D/2D Co3O4/g-C3N4, exhibits high efficiency and high yield photocatalytic H2 evolution due to suppression of electron-hole pair recombination and enhanced redox ability. The 2D/2D Co3O4/g-C3N4 photocatalyzes H2 evolution with a rate of ~370 μmol h-1 within λ > 400 nm. The external quantum efficiency (EQE) of 2D/2D Co3O4/g-C3N4 at λ = 405 nm reached 53.6%, which is among the highest for g-C3N4-based catalysts.