Kapkowski Maciej, Niemczyk-Wojdyla Anna, Bartczak Piotr, Pyrkosz Bulska Monika, Gajcy Kamila, Sitko Rafal, Zubko Maciej, Szade Jacek, Klimontko Joanna, Balin Katarzyna, Polanski Jaroslaw
Institute of Chemistry, University of Silesia, Szkolna 9, 40-006 Katowice, Poland.
Institute of Materials Science, University of Silesia, 75 Pułku Piechoty 1A, 41-500 Chorzów, Poland.
Nanomaterials (Basel). 2019 Mar 15;9(3):442. doi: 10.3390/nano9030442.
The classical stoichiometric oxidation of alcohols is an important tool in contemporary organic chemistry. However, it still requires huge modifications in order to comply with the principles of green chemistry. The use of toxic chemicals, hazardous organic solvents, and the large amounts of toxic wastes that result from the reactions are a few examples of the problems that must be solved. Nanogold alone or conjugated with palladium were supported on different carriers (SiO₂, C) and investigated in order to evaluate their catalytic potential for environmentally friendly alcohol oxidation under solvent-free and base-free conditions in the presence H₂O₂ as a clean oxidant. We tested different levels of Au loading (0.1⁻1.2% wt.) and different active catalytic site forms (monometallic Au or bimetallic Au⁻Pd sites). This provided new insights on how the structure of the Au-dispersions affected their catalytic performance. Importantly, the examination of the catalytic performance of the resulting catalysts was oriented toward a broad scope of alcohols, including those that are the most resistant to oxidation-the primary aliphatic alcohols. Surprisingly, the studies proved that Au/SiO₂ at a level of Au loading as low as 0.1% wt. appeared to be efficient and prospective catalytic system for the green oxidation of alcohol. Most importantly, the results revealed that 0.1% Au/SiO₂ might be the catalyst of choice with a wide scope of utility in the green oxidation of various structurally different alcohols as well as the non-activated aliphatic ones.
醇类的经典化学计量氧化是当代有机化学中的一项重要工具。然而,为了符合绿色化学的原则,它仍需要进行大量改进。使用有毒化学品、有害有机溶剂以及反应产生的大量有毒废物就是一些必须解决的问题实例。将纳米金单独或与钯结合负载在不同载体(SiO₂、C)上,并进行研究,以评估它们在无溶剂、无碱条件下,以H₂O₂作为清洁氧化剂时对环境友好型醇氧化的催化潜力。我们测试了不同水平的金负载量(0.1⁻1.2%重量)和不同的活性催化位点形式(单金属金或双金属金⁻钯位点)。这为金分散体的结构如何影响其催化性能提供了新的见解。重要的是,对所得催化剂催化性能的考察针对的是广泛的醇类,包括那些最难氧化的伯脂肪醇。令人惊讶的是,研究证明,金负载量低至0.1%重量的Au/SiO₂似乎是醇绿色氧化的高效且有前景的催化体系。最重要的是,结果表明0.1% Au/SiO₂可能是在各种结构不同的醇以及未活化脂肪醇的绿色氧化中具有广泛用途的首选催化剂。