<br>有缺陷的聚七嗪酰亚胺钾可防止自旋离域和空穴转移失活，实现高效太阳能转换和存储,Small

当前位置： X-MOL 学术 › Small › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

有缺陷的聚七嗪酰亚胺钾可防止自旋离域和空穴转移失活，实现高效太阳能转换和存储
Small ( IF 13.0 ) Pub Date : 2023-09-26 , DOI: 10.1002/smll.202304813
Li-Che Chueh, Tzu-Jen Lin, Hao-Cheng Lee, Jih-Jen Wu

通过在KSCN盐熔体中对合理设计的超分子配合物进行直接电离热处理，制备了缺陷七嗪环中部分中心氮原子被石墨碳原子取代的反位点缺陷聚七嗪酰亚胺钾（KPHI）。与没有反位点缺陷的KPHI相比，反位点缺陷的KPHI在H ₂析出反应(HER)中表现出显着改善的光催化和暗光催化性能。在空穴清除剂存在的情况下，反位点缺陷 KPHI 对 HER 表现出优异的光催化稳定性，持续 20 小时，而普通 KHPI 在 3 小时 HER 后观察到失活。此外，反位点缺陷KPHI中存储的光电子在黑暗中的H ₂产量增加了一个数量级以上。密度泛函理论计算表明，KPHI中的反位点缺陷单元不仅可以防止自旋离域，还可以抑制空穴转移的失活，有利于光电子存储和光催化活性。本研究的结果提供了对 KPHI 光物理和催化特性的深入了解，从而得出了通过在 KPHI 中纳入固有反位点缺陷来提高太阳能转换和存储性能的策略。

"点击查看英文标题和摘要"

Defective Potassium Poly(Heptazine Imide) Preventing Spin Delocalization and Hole Transfer Deactivation for Efficient Solar Energy Conversion and Storage

Anti-site defective potassium poly(heptazine imide) (KPHI) with the central nitrogen atoms partially replaced by graphitic carbon atoms in the flawed heptazine rings is prepared by direct ionothermal treatment of the rationally designed supramolecular complex in KSCN salt molten. Compared to the KPHIs without the anti-site defect, the anti-site defective KPHI demonstrates significantly improved photocatalytic and dark photocatalytic performances for H₂ evolution reaction (HER). In the presence of the hole scavenger, the anti-site defective KPHI exhibits superior photocatalytic stability for HER lasting 20 h, whereas the deactivation is observed from the ordinary KHPIs after 3 h HER. Moreover, the H₂ yield in the dark by the stored photoelectrons in the anti-site defective KPHI increases by more than an order of magnitude. Density functional theory calculations reveal that the anti-site defective unit in KPHI not only prevents spin delocalization but also inhibits the deactivation of hole transfer, which are beneficial to photoelectron storage and photocatalytic activity. The findings in this study provide insight into the photophysical and catalytic properties of KPHI, which conclude a strategy to improve the performances for solar energy conversion and storage by incorporating intrinsic anti-site defects in KPHI.

更新日期：2023-09-26

点击分享查看原文

点击收藏

公开下载

阅读更多本刊新发论文本刊介绍/投稿指南