Gold Catalysis Research Center, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Nanoscale. 2017 Nov 9;9(43):16879-16886. doi: 10.1039/c7nr06566c.
Size-dependence is an important factor in gold nanocatalysis. In this study, we explored the catalytic performance of atomically precise Au(PET) nanocluster catalysts (where, PET = phenylethanethiolate) of different gold atoms and sizes, including Au(PET) (∼1.2 nm), Au(PET) (∼1.5 nm), and Au(PET) (∼1.9 nm) nanoclusters. These Au(PET) gold clusters, immobilized on activated carbon (AC) and used as heterogeneous catalysts, were characterized by transmission electron microscope (TEM), BET as well as X-ray photoelectron spectroscopy (XPS). They showed good catalytic activity in the aerobic oxidation of d-glucose into gluconic acid (or gluconates) with ∼98% selectivity. We observed a distinct size dependence of the gold nanocluster in the oxidation reactions, which follows as Au(PET)/AC > Au(PET)/AC > Au(PET)/AC. It was primarily determined by the surface area of the nanoscopic Au nanocluster. Further, the turnover frequency (TOF) for the Au(PET)/AC catalyst was found to be 2.3 s, which is comparable with that for Au/EC300 and much higher than those for the commercial Pd/AC and Pd-Bi/AC catalysts under the identical reaction conditions. On the whole, the core size of the gold nanoclusters played an important role in the catalytic process.
尺寸依赖性是金纳米催化中的一个重要因素。在这项研究中,我们探索了不同金原子和尺寸的原子精确 Au(PET)纳米团簇催化剂(其中,PET = 苯乙硫醇)的催化性能,包括 Au(PET)(1.2nm)、Au(PET)(1.5nm)和 Au(PET)(~1.9nm)纳米团簇。这些 Au(PET)金团簇被固定在活性炭(AC)上并用作多相催化剂,通过透射电子显微镜(TEM)、BET 和 X 射线光电子能谱(XPS)进行了表征。它们在有氧氧化 d-葡萄糖成葡萄糖酸(或葡萄糖酸盐)中表现出良好的催化活性,选择性约为 98%。我们观察到金纳米团簇在氧化反应中存在明显的尺寸依赖性,其顺序为 Au(PET)/AC > Au(PET)/AC > Au(PET)/AC。这主要取决于纳米级 Au 纳米团簇的表面积。此外,发现 Au(PET)/AC 催化剂的周转频率(TOF)为 2.3s,与 Au/EC300 的 TOF 相当,远高于相同反应条件下商业 Pd/AC 和 Pd-Bi/AC 催化剂的 TOF。总的来说,金纳米团簇的核心尺寸在催化过程中起着重要作用。