College of Science, Inner Mongolia Agricultural University, Hohhot 010018, China.
Inner Mongolia Key Laboratory of Soil Quality and Nutrient Resource & Key Laboratory of Agricultural Ecological Security and Green Development at Universities of Inner Mongolia Autonomous, Hohhot 010018, China.
ACS Appl Mater Interfaces. 2023 Jun 28;15(25):30161-30169. doi: 10.1021/acsami.3c03451. Epub 2023 Jun 19.
Plasmonic Au nanoparticles (NPs) employing localized surface plasmon resonance excitation have exhibited superior visible light absorption for many organic transformations. In this work, we prepared a ternary composite catalyst comprising plasmonic Au NPs and a 2D/2D TiO-CN heterojunction via a photoreduction method of chloroauric acid in the presence of TiO-CN. The introduction of plasmonic nanogold particles embedded onto the TiO surface of the TiO-CN heterojunction can significantly improve the photocatalytic performance during photooxidation of benzyl alcohol to benzaldehyde under mild conditions (1 bar air, white LED irradiation at ambient temperature). The productivity over Au/TiO-CN (0.25 mmol g h) is found to be ∼5.6, 8.3, and 8.2-fold of these over the Au/TiO, TiO-CN, and CN-Au-TiO heterojunctions, respectively. Trapping experiments and electron spin resonance (ESR) spectroscopy confirm that the superoxide (O) and hydroxyl radicals (OH) act as the reactive oxygen species during photooxidation. Furthermore, the experimental results combined with density functional theory calculations reveal that the chemisorbed benzyl alcohol population, surface oxygen vacancies, and lifetime of photoexcited electrons and holes are largely improved by plasmonic Au NPs. This study on nanogold composites provides some hints for developing new efficient and practical photocatalysts.
采用局域表面等离激元共振激发的等离子体 Au 纳米粒子（NPs）在许多有机转化中表现出优异的可见光吸收。在这项工作中，我们通过在 TiO-CN 存在下用光还原氯金酸的方法制备了包含等离子体 Au NPs 和二维/二维 TiO-CN 异质结的三元复合催化剂。将等离子体纳米金颗粒嵌入到 TiO-CN 异质结的 TiO 表面上，可以显著提高在温和条件下（1 巴空气，环境温度下的白色 LED 照射）光氧化苯甲醇为苯甲醛的光催化性能。发现 Au/TiO-CN（0.25mmol g h）的产率分别是 Au/TiO、TiO-CN 和 CN-Au-TiO 异质结的 5.6、8.3 和 8.2 倍。捕获实验和电子自旋共振（ESR）光谱证实，超氧阴离子（O）和羟基自由基（OH）在光氧化过程中作为活性氧物质。此外，实验结果结合密度泛函理论计算表明，等离子体 Au NPs 大大提高了化学吸附的苯甲醇浓度、表面氧空位以及光激发电子和空穴的寿命。这项关于纳米金复合材料的研究为开发新的高效实用光催化剂提供了一些启示。
