| 苗瑞霞,牛佳美,晏杰,贾小坛.金属掺杂对β-Ga2O3光催化分解水制氢性能的影响[J].分子催化,2025,39(1):76-84 |
| 金属掺杂对β-Ga2O3光催化分解水制氢性能的影响 |
| Impact of Metal Doping on the Photocatalytic Water Splitting Performance of β-Ga2O3 for Hydrogen Production |
| 投稿时间：2024-12-11 修订日期：2025-01-03 |
| DOI：10.16084/j.issn1001-3555.2025.01.008 |
| 中文关键词: 光催化 β-Ga2O3 掺杂 光学性质 |
| 英文关键词:photocatalysis β-Ga2O3 doping optical properties |
| 基金项目:国家自然科学基金(51302215, 62105260, 12004303)[National Natural Science Foundation of China (51302215, 62105260, 12004303)]. |
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| 中文摘要: |
| β-Ga2O3以其较高的导带底(Conduction Band Minimum, CBM)和较低的价带顶(Valence Band Maximum, VBM), 赋予其光生电子和空穴较强的还原与氧化能力, 但其宽禁带和高载流子复合率限制了在光催化中的应用. 金属离子掺杂被认为是提升光催化性能的有效途径. 本文基于第一性原理系统研究了Sr、Ba、V、Nb、Ta等二十种元素掺杂对β-Ga2O3光催化性能的影响, 研究发现: Sr、Nb、Ta、Mn、Fe、Zn、Hg七种元素掺杂β-Ga2O3后, 材料除能保持合适的带边位置外, 还具有更高的电子空穴分离效率以及更低的形成能, 表明这些元素的引入可有效提升β-Ga2O3光催化效率; Nb、Ta掺杂可显著增强材料在红外光区的吸收, Mn、Fe掺杂则显著提升材料在紫外和可见光区的吸收能力, 其中, Nb在0.5 eV处光吸收系数高达1.38×105 cm–1, Mn、Fe掺杂在3 eV处光吸收系数可达1×105 cm–1, 在不同波段均呈现出良好的光吸收能力. 此外, Hg掺杂表现出跨红外至深紫外的宽波段增强效果, Hg掺杂后, 电子空穴相对有效质量高达109, 说明Hg掺杂显著提升载流子分离能力, 同时由于其在宽波段显著增强的光吸收效果, 因此, Hg可作为β-Ga2O3在光催化制氢中理想的金属掺杂元素, 以上研究结果为β-Ga2O3光催化分解水制氢研究提供了价值参考. |
| 英文摘要: |
| β-Ga2O3, with its high conduction band minimum (CBM) and low valence band maximum (VBM), endows photogenerated electrons and holes with strong reductive and oxidative capabilities. However, its photocatalytic applications are limited for its wide bandgap and fast carrier recombination. Metal ion doping has been considered as an effective approach to enhance the photocatalytic performance. In this study, the effects of doping twenty elements, including Sr, Ba, V, Nb, and Ta et al, on the photocatalytic performance of β-Ga2O3 are investigated based on first-principles calculations. The results are as follows: doping Sr, Nb, Ta, Mn, Fe, Zn and Hg, not only maintains appropriate band edge positions but also exhibits higher electron-hole separation efficiency and lowers formation energies, indicating that these dopants can effectively enhance the photocatalytic efficiency of β-Ga2O3; Nb and Ta doping significantly enhances infrared light absorption, while Mn and Fe doping both improves ultraviolet and visible light absorption of β-Ga2O3. Specifically, absorption coefficient of β-Ga2O3 with Nb doping achieves an as high as 1.38×105 cm-1 at 0.5 eV, and Mn and Fe doping reaches a high absorption coefficient of 1×105 cm–1 at 3 eV, demonstrating excellent light absorption in their respective wavelength ranges. Furthermore, Hg doping shows enhancement on broad absorption spectrum, from infrared to deep ultraviolet; β-Ga2O3 with Hg doping exhibits an electron-hole relative effective mass as high as 109, indicating that Hg dopant can significantly improving carrier separation efficiency. Meanwhile, owing to its remarkable effect of enhancing light absorption in a wide wavelength range, Hg can be used as an ideal dopant for β-Ga2O3 in photocatalytic hydrogen production. These results provide valuable references for the study of β-Ga2O3 in photocatalytic water splitting and hydrogen generation. |
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