Hou Jian, Lartey Jemima A, Lee Chang Yeon, Kim Jun-Hyun
School of Intelligent Manufacturing, Luoyang Institute of Science and Technology, Luoyang, 471023, China.
Department of Chemistry, Illinois State University, Normal, IL, 61790-4160, USA.
Sci Rep. 2024 Jan 16;14(1):1352. doi: 10.1038/s41598-024-51695-3.
Validating the direct photocatalytic activity of colloidal plasmonic nanoparticles is challenging due to their limited stability and needed support materials that can often contribute to the chemical reactions. Stable gold nanoparticles (AuNPs) with tunable sizes are prepared across porous polymer particles without any chemical bonds where the resulting composite particles exhibit intense surface plasmon resonances (SPRs) in the visible region. These composite particles are then tested as photocatalysts under a broadband solar-simulated light source to examine the contribution degree of photothermal heating and SPR coming from the incorporated AuNPs in the C-C bond forming homocoupling reaction. Generally, the thermal and photothermal heating are the main driving force to increase the reactivity of relatively smaller AuNPs (~ 44 nm in diameter) with a narrower SPR band. However, the SPR-induced catalytic activity is much greater for the composite particles containing larger AuNPs (~ 87 nm in diameter) with a broader SPR. As the polymer particle matrix does not influence the catalytic activity (e.g., inducing charge delocalization and/or separation), the unique SPR role of the colloidal AuNPs in the catalytic reaction is assessable under light irradiation. This study experimentally demonstrates the possibility of evaluating the direct contribution of SPRs to photocatalytic chemical reactions.
由于胶体等离子体纳米颗粒稳定性有限且需要能经常参与化学反应的支撑材料,因此验证其直接光催化活性具有挑战性。在没有任何化学键的情况下,在多孔聚合物颗粒上制备了尺寸可调的稳定金纳米颗粒(AuNP),所得复合颗粒在可见光区域表现出强烈的表面等离子体共振(SPR)。然后,在宽带太阳模拟光源下将这些复合颗粒作为光催化剂进行测试,以研究在形成C-C键的均偶联反应中,光热加热和来自掺入的AuNP的SPR的贡献程度。一般来说,热加热和光热加热是提高相对较小的AuNP(直径约44nm)反应活性的主要驱动力,其SPR带较窄。然而,对于含有较大AuNP(直径约87nm)且SPR较宽的复合颗粒,SPR诱导的催化活性要大得多。由于聚合物颗粒基质不影响催化活性(例如,诱导电荷离域和/或分离),因此在光照下可评估胶体AuNP在催化反应中独特的SPR作用。本研究通过实验证明了评估SPR对光催化化学反应直接贡献的可能性。