Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2021-09-01 , DOI: 10.1016/j.apcatb.2021.120674 Enxin Cui 1 , Haibin Li 1 , Chen Zhang 1 , Dan Qiao 1 , Manoj B. Gawande 2 , Chen-Ho Tung 1 , Yifeng Wang 1, 3
A conventional plasmonic Ag-AgCl photocatalyst consists of Ag nanoparticles (AgNPs) and AgCl. Here, we converted a small amount of Ag+ on the surfaces of AgCl particles into single-atom Ag(0) (SAAg). SAAg was characterized with high-angle annular dark field aberration corrected (HAADF AC)-STEM and quantified with electron spin resonance (ESR). The obtained AgEG/Mg(OH)2 material was efficient and afforded excellent selectivity control between hydrodehalogenation and deiodination-borylation under visible light irradiation. SAAg acted as the 1e−-reducing site of the photocatalyst and its loading is linearly correlated with the initial reaction rate. While the quantity of SAAg was only 6.0 × 10–8 mol g−1, the TOF of SAAg reached 1.4 × 104 h−1. The oxidation state of SAAg retained 0 in both the resting and the working states. This study suggests SAAg may be an effective cocatalyst in general for reductive dehalogenation of organic halides.
中文翻译:
一种含有银(0)单原子的先进等离子体光催化剂,用于芳基碘化物的选择性硼酸化
传统的等离子体 Ag-AgCl 光催化剂由 Ag 纳米粒子 (AgNPs) 和 AgCl 组成。在这里,我们将AgCl 颗粒表面上的少量 Ag +转化为单原子 Ag(0) (SAAg)。SAAg 以高角度环形暗场像差校正 (HAADF AC)-STEM 为特征,并通过电子自旋共振 (ESR) 进行量化。所获得的Ag EG /Mg(OH) 2材料是有效的,并且在可见光照射下在加氢脱卤和脱碘-硼酰化之间提供了极好的选择性控制。SAAg 作为光催化剂的 1e -还原位点,其负载量与初始反应速率呈线性相关。而 SAAg 的量仅为 6.0 × 10 –8 mol g-1,SAAg的TOF达到1.4×10 4 h -1。SAAg 的氧化态在静止和工作状态均保持为 0。这项研究表明,SAAg 可能是一种有效的助催化剂,通常用于有机卤化物的还原脱卤。