| Li、Au掺杂对GaN/ZnO异质结光解水制氢性能的调控 |
| Regulation of photocatalytic hydrogen production performance in GaN/ZnO heterojunction through doping with Li and Au |
|
| 摘要: 以提高GaN/ZnO异质结光解水制氢性能为目标，采用第一性原理方法研究了Li和Au元素掺杂GaN/ZnO异质结的电子结构、光学性质和光催化性能。电子结构计算表明GaN/ZnO异质结为直接带隙半导体，异质结类型为Z型，带隙为1.41 eV，能有效促进载流子分离。Li、Au掺杂后的各结构中除Li替位Zn结构外，均具有磁性。光学性质分析的结果表明，掺杂Li、Au元素可以提高体系的吸收系数，其中Li替位Zn后异质结具有较大的光吸收系数，同时具有较大的功函数(7.37 eV)和界面电势差(2.55 V)，表明其可见光利用率较高，界面结构稳定且具有较大的内建电场，可以更有效地促进电子与空穴的迁移从而减小电子-空穴对的结合。Bader电荷分析表明掺杂元素Li和Au均失去电子。电子从GaN层向ZnO层转移，在界面处形成了一个有效的内电场。Li替位 Zn和 Au同时替位近位的 Ga和 Zn所对应的 2种结构的层与层之间转移的电子较多，说明其界面电势差较大且拥有较高的光生载流子迁移速率。光解水制氢性能分析表明，ZnO薄膜、GaN/ZnO异质结、Li替位 Ga以及 Li同时替位远位的 Ga和 Zn四种体系在 pH=0时，满足光解水制氢的条件。GaN薄膜、ZnO薄膜和 Li同时替位远位的 Ga和 Zn三种体系在pH=7时满足光解水制氢的条件。 |
| 关键词: 第一性原理方法 GaN/ZnO异质结 电子结构 磁特性 光解水制氢 |
| 基金项目: 陕西省自然科学基金(No.2023-JC-YB-028)和西安石油大学研究生创新和实践能力培养计划项目(No.YCS23113093)资助。 |
| Abstract: This paper aims to improve hydrogen production through photolysis water performance of GaN/ZnO heterojunction by doping Li and Au. First principles methods were used to investigate the electronic structures, optical properties, and photocatalytic performance of Li and Au doping GaN/ZnO heterojunction. The electronic structure calculation shows that the GaN/ZnO heterojunction is a direct band-gap semiconductor, and the heterojunction type is a Z-type heterojunction with a band gap of 1.41 eV, which can effectively promote carrier separation. The structures doped with Li and Au are magnetic except for the Li substitution Zn structure. The results of optical property analysis show that the doping of Li and Au can improve the absorption coefficient of the system, and the heterojunction after Li substitution Zn has a large optical absorption coefficient, a large work function (7.37 eV), and an interface potential difference (2.55 V), indicating that the visible light utilization rate is high, the interface structure is stable and has a large built-in electric field, which can more effectively promote the migration of electrons and holes and reduce the binding of electron-hole pairs. The Bader charge analysis shows that the doped elements Li and Au lose electrons. The electrons are transferred from the GaN layer to the ZnO layer, forming an effective internal electric field at the interface. More electrons are transferred between the two structural layers of Ga and Zn, which are substituted by Li and Au, indicating that the interfacial potential difference is large and has a high migration rate of photogenerated carriers. The analysis of the performance of photolysis of water to hydrogen production shows that the four systems of ZnO film, GaN/ZnO heterojunction, Li substitution Ga, and Ga and Zn with simultaneous displacement of Li meet the conditions for hydrogen production by photolysis at pH=0. The GaN film, ZnO film, and Ga and Zn systems with a simultaneous displacement of Li meet the conditions for hydrogen production by photolysis of water at pH=7. |
| Keywords: first principles method GaN/ZnO heterojunction electronic structure magnetic property hydrogen production through photolysis water |
| 投稿时间：2024-06-28 修订日期：2025-01-20 |
| 摘要点击次数: 341 |
| 全文下载次数: 52 |
| 温俊青,王若琦,张建民.Li、Au掺杂对GaN/ZnO异质结光解水制氢性能的调控[J].无机化学学报,2025,41(5):923-938. |
| 查看全文 查看/发表评论 下载PDF阅读器 |
| Support information: |
|
|
|
|
|
|
