Designing Direct Z-Scheme Heterojunctions Enabled by Edge-Modified Phosphorene Nanoribbons for Photocatalytic Overall Water Splitting,The Journal of Physical Chemistry Letters

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Designing Direct Z-Scheme Heterojunctions Enabled by Edge-Modified Phosphorene Nanoribbons for Photocatalytic Overall Water Splitting
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2021-12-23 , DOI: 10.1021/acs.jpclett.1c03527
Yunzhi Gao ₁ , Cenfeng Fu ₁ , Wei Hu ₁ , Jinlong Yang ₁

Affiliation

Direct Z-scheme photocatalyst possess promising potential to utilize solar radiation for photocatalytic overall water splitting; however, the design and characterization remain challenging. Here, we construct and verify a direct Z-scheme heterojunction using edge-modified phosphorene-nanoribbons (X-PNRs, where X = OH and OCN) with first-principles ground-state and excited-state density functional theory (DFT) calculations. The ground-state calculations provide fundamental properties such as geometric structure and band alignment. The linear-response time-dependent DFT (LR-TDDFT) calculations exhibit the photogenerated charge distribution and demonstrate the generation of interlayer excitons in heterojunctions, which are advantageous to the electron–hole recombination in Z-scheme heterojunctions. The ultrafast charge transfer at the interface studied by time-dependent ab initio nonadiabatic molecular dynamics (NAMD) simulations indicates that interlayer electron–hole recombination is prior to intralayer recombination for the OH/OCN-PNRs heterojunction, showing the characteristics of a Z-scheme heterojunction. Therefore, our computational work provides a universal strategy to design direct Z-scheme heterojunction photocatalysts for overall water splitting.

中文翻译：

设计由边缘改性磷烯纳米带实现的直接 Z 型异质结，用于光催化整体水分解

直接Z型光催化剂具有利用太阳辐射进行光催化全水分解的广阔潜力；然而，设计和表征仍然具有挑战性。在这里，我们使用具有第一性原理基态和激发态密度泛函理论 (DFT) 计算的边缘改性磷烯纳米带 (X-PNR，其中 X = OH 和 OCN) 构建并验证了直接 Z 型异质结。基态计算提供了基本属性，例如几何结构和能带对齐。线性响应时间相关的 DFT (LR-TDDFT) 计算展示了光生电荷分布，并证明了异质结中层间激子的产生，这有利于 Z 型异质结中的电子-空穴复合。通过时间相关的从头算非绝热分子动力学 (NAMD) 模拟研究的界面处的超快电荷转移表明，对于 OH/OCN-PNRs 异质结，层间电子-空穴复合先于层内复合，显示出 Z 方案的特征异质结。因此，我们的计算工作提供了一种通用策略来设计用于整体水分解的直接 Z 型异质结光催化剂。

更新日期：2022-01-13

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