Gesesse Getaneh Diress, Wang Cong, Chang Bor Kae, Tai Shih-Hsuan, Beaunier Patricia, Wojcieszak Robert, Remita Hynd, Colbeau-Justin Christophe, Ghazzal Mohamed Nawfal
Institut de chimie Physique, UMR 8000 CNRS, Université Paris-Saclay, 91405, Orsay, France.
Nanoscale. 2020 Apr 3;12(13):7011-7023. doi: 10.1039/c9nr09891g.
Engineering photocatalysts based on gold nanoparticles (AuNPs) has attracted great attention for the solar energy conversion due to their multiple and unique properties. However, boosting the photocatalytic performance of plasmonic materials for H2 generation has some limitations. In this study, we propose a soft-chemistry method for the preparation of a strong metal-support interaction (SMSI) to enhance the photocatalytic production of H2. The TiO2 thin overlayer covering finely dispersed AuNPs (forming an SMSI) boosts the photocatalytic generation of hydrogen, compared to AuNPs deposited at the surface of TiO2 (labelled as a classical system). The pathway of the charge carriers' dynamics regarding the system configuration is found to be different. The photogenerated electrons are collected by AuNPs in a classical system and act as an active site, while, unconventionally, they are injected back in the titania surface for an SMSI photocatalyst making the system highly efficient. Additionally, the adsorption energy of methanol, theoretically estimated using the density functional theory (DFT) methodology, is lower for the soft-chemistry SMSI photocatalyst accelerating the kinetics of photocatalytic hydrogen production. The SMSI obtained by soft-chemistry is an original concept for highly efficient photocatalytic materials, where the photon-to-energy conversion remains a major challenge.
基于金纳米颗粒（AuNPs）的工程光催化剂因其多种独特性能，在太阳能转换方面备受关注。然而，提高等离子体材料用于制氢的光催化性能存在一些局限性。在本研究中，我们提出一种软化学方法来制备强金属-载体相互作用（SMSI），以提高光催化产氢量。与沉积在TiO2表面的AuNPs（标记为经典体系）相比，覆盖精细分散AuNPs的TiO2薄覆盖层（形成SMSI）可促进光催化产氢。发现关于体系构型的电荷载流子动力学途径有所不同。在经典体系中，光生电子被AuNPs收集并作为活性位点，而对于SMSI光催化剂，光生电子则反常地注入到二氧化钛表面，使体系高效运行。此外，使用密度泛函理论（DFT）方法理论估算得出，软化学SMSI光催化剂的甲醇吸附能较低，从而加速了光催化产氢的动力学过程。通过软化学获得的SMSI是高效光催化材料的一个原创概念，其中光子到能量的转换仍然是一个重大挑战。
