Li Xiaoyu, Cheng Jinling, Hou Huaming, Meira Debora M, Liu Lichen
Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing 100084, China.
National Energy Center for Coal to Clean Fuels, Synfuels China Co., Ltd., Huairou District, Beijing 101407, China.
JACS Au. 2024 Feb 6;4(2):666-679. doi: 10.1021/jacsau.3c00732. eCollection 2024 Feb 26.
Reactant-induced structural evolutions of heterogeneous metal catalysts are frequently observed in numerous catalytic systems, which can be associated with the formation or deactivation of active sites. In this work, we will show the structural transformation of subnanometer Pt clusters in pure-silica MFI zeolite structure in the presence of CO, O, and/or HO and the catalytic consequences of the Pt-zeolite materials derived from various treatment conditions. By applying the appropriate pretreatment under a reactant atmosphere, we can precisely modulate the size distribution of Pt species spanning from single Pt atoms to small Pt nanoparticles (1-5 nm) in the zeolite matrix, resulting in the desirably active and stable Pt species for CO oxidation. We also show the incorporation of Fe into the zeolite framework greatly promotes the stability of Pt species against undesired sintering under harsh conditions (up to 650 °C in the presence of CO, O, and moisture).
在众多催化体系中,经常观察到反应物诱导的非均相金属催化剂的结构演变,这可能与活性位点的形成或失活有关。在这项工作中,我们将展示在CO、O和/或H₂O存在下,纯硅MFI沸石结构中亚纳米级Pt簇的结构转变,以及源自各种处理条件的Pt-沸石材料的催化后果。通过在反应物气氛下进行适当的预处理,我们可以精确调节沸石基质中从单个Pt原子到小Pt纳米颗粒(1-5 nm)的Pt物种的尺寸分布,从而得到用于CO氧化的理想活性和稳定的Pt物种。我们还表明,将Fe引入沸石骨架可大大提高Pt物种在苛刻条件下(在CO、O和水分存在下高达650°C)抵抗不期望烧结的稳定性。