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Construction of electron donor–acceptor Z-scheme heterojunction for boosting photocatalytic H2 production
Applied Surface Science ( IF 6.7 ) Pub Date : 2023-05-27 , DOI: 10.1016/j.apsusc.2023.157625
Xinlei Zhang, Xuehua Wang, Guicun Li, Lei Wang, Jianfeng Huang, Alan Meng, Zhenjiang Li

Enhancing the solar energy conversion of metal-free graphitic carbon nitride (g-C3N4) based photocatalyst remains a great challenge. Herein, a novel Z-scheme heterojunction photocatalyst is constructed by in-situ anchoring Pt6 NCs on carbon self-doping g-C3N4 (CCN/Pt6 NCs) for boosting photocatalytic H2 evolution activity. Remarkably, the optimized CCN/Pt6 NCs photocatalyst exhibits high H2 evolution rate of 6.32 mmol·h−1·g−1 and 36.25 mmol·h−1·g−1, which is ≈150.5 and ≈412 times than that of pristine CN under visible light (λ > 420 nm) and full solar spectrum irradiation, respectively, outperforming majority of the reported g-C3N4-based photocatalysts. Systematic characterizations have revealed that CCN with delocalized electrons and larger the work function is deemed to be a preferable electron-acceptor. Meanwhile, Pt6 NCs with appropriate HOMO-LUMO level is regarded as an electron-donor. Theoretical and experimental works reveal that the favorable photocatalytic performance of CCN/Pt6 NCs heterojunction is mainly attributed to the giant internal electric field induced donor–acceptor interaction, which achieves Z-scheme charge transfer mechanism. This work opens up new insights for rational fabrication of metal-free g-C3N4 based photocatalysts to boost the solar energy conversion.



中文翻译:

构建电子供体-受体 Z 型异质结促进光催化产氢

提高基于无金属石墨碳氮化物(gC 3 N 4)的光催化剂的太阳能转化仍然是一个巨大的挑战。在此,通过将 Pt 6 NCs原位锚定在碳自掺杂 gC 3 N 4 (CCN/Pt 6 NCs) 上,构建了一种新型 Z 型异质结光催化剂,以提高光催化 H 2释放活性。值得注意的是,优化后的 CCN/Pt 6 NCs 光催化剂表现出6.32 mmol·h -1 ·g -1和 36.25 mmol·h -1 ·g -1的高 H 2释放速率,分别是原始 CN 在可见光(λ > 420 nm)和全太阳光谱照射下的 ≈150.5 和 ≈412 倍,优于大多数已报道的基于 gC 3 N 4催化剂。系统表征表明,具有离域电子和较大功函数的 CCN 被认为是一种优选的电子受体。同时,具有适当HOMO-LUMO能级的Pt 6 NCs被认为是电子供体。理论和实验工作表明,CCN/Pt 6具有良好的光催化性能NCs异质结主要归因于巨大的内部电场诱导的供体-受体相互作用,实现了Z型电荷转移机制。这项工作为合理制备非金属 gC 3 N 4基光催化剂以促进太阳能转化开辟了新思路。

更新日期:2023-05-27
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