<br>同型异质结：调整结晶富氮 C3N5 的庚嗪/三嗪相以实现多功能光催化应用,Materials Horizons

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同型异质结：调整结晶富氮 C3N5 的庚嗪/三嗪相以实现多功能光催化应用
Materials Horizons ( IF 12.2 ) Pub Date : 2023-09-21 , DOI: 10.1039/d3mh01115a
Sue-Faye Ng _{1,

2} , Joel Jie Foo _{1,

2} , Wee-Jun Ong _{1,

2,

3,

4,

5}

Affiliation

光催化技术作为通过水分解或化学合成实现可持续能源生产的一种手段已得到充分研究。最近，人们发现低C/N原子比的氮化碳同素异形体C ₃ N ₅与gC ₃ N ₄相比，由于其优异的电子性能和充足的N活性位点而具有很高的前景。切线而言，结晶 gC ₃ N ₄因其改进的电子传输和扩展的 π 共轭体系而成为潜在的候选者。本课题组首次成功采用一步熔盐焙烧法制备了新型富氮晶体C ₃ N ₅ ，并阐明了焙烧温度对七嗪/三嗪相的影响。 500 °C (CC3N5-500) 和 550 °C (CC3N5-550) 的煅烧温度会产生具有七嗪和三嗪相的结晶氮化碳，形成紧密的同型异质结，从而实现稳健的界面电荷分离。使用CC3N5-500实现了优异的光催化析氢速率（359.97 μmol h ^-1 ；表观量子效率（AQE）：420 nm处12.86%），比原始C ₃ N ₅高15倍。此外，CC3N5-500 在同步苯甲醇氧化和氢气生产以及 H ₂ O ₂生产方面表现出改进的活性（AQE：9.420 nm 处为 49%），表明其具有众多的光氧化还原能力。此外，最佳 CC3N5-500 在 3D 打印基板上的可回收性测试也显示，4 个循环（16 小时）后性能保持率为 92%。这凸显了晶体 C ₃ N ₅显着增强了各种多功能太阳能驱动应用的反应性能。因此，这些结果可以作为调整结晶度的二维无金属碳纳米材料的结构调整的指南，以实现增强的光催化作用。

"点击查看英文标题和摘要"

Isotype heterojunction: tuning the heptazine/triazine phase of crystalline nitrogen-rich C3N5 towards multifunctional photocatalytic applications

Photocatalytic technology has been well studied as a means to achieve sustainable energy generation through water splitting or chemical synthesis. Recently, a low C/N atomic ratio carbon nitride allotrope, C₃N₅, has been found to be highly prospective due to its excellent electronic properties and ample N-active sites compared to g-C₃N₄. Tangentially, crystalline g-C₃N₄ has also been a prospective candidate due to its improved electron transport and extended π-conjugated system. For the first time, our group successfully employed a one-step molten salt calcination method to prepare novel N-rich crystalline C₃N₅ and elucidate the effect of calcination temperature on the heptazine/triazine phase. Calcination temperatures of 500 °C (CC3N5-500) and 550 °C (CC3N5-550) lead to crystalline carbon nitride with both heptazine and triazine phases, forming an intimate isotype heterojunction for robust interfacial charge separation. An excellent photocatalytic hydrogen evolution rate (359.97 μmol h⁻¹; apparent quantum efficiency (AQE): 12.86% at 420 nm) was achieved using CC3N5-500, which was 15-fold higher than that of pristine C₃N₅. Furthermore, CC3N5-500 exhibited improved activity for simultaneous benzyl alcohol oxidation and hydrogen production, as well as H₂O₂ production (AQE: 9.49% at 420 nm), signifying its multitudinous photoredox capabilities. Moreover, the recyclability tests of the optimal CC3N5-500 on a 3D-printed substrate also showed a 92% performance retention after 4 cycles (16 h). This highlights that crystalline C₃N₅ significantly augmented the reaction performance for diverse multifunctional solar-driven applications. As such, these results serve as a guide toward the structural tuning of 2D metal-free carbon nanomaterials with tunable crystallinity toward achieving boosted photocatalysis.

更新日期：2023-09-21

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