†Chemistry Department and ‡Center for Functional Nanomaterials (CFN), Brookhaven National Laboratory, Upton, New York 11973, United States.
§Dalian University of Technology, Dalian 116024, Liaoning Province, China.
J Am Chem Soc. 2015 Aug 19;137(32):10104-7. doi: 10.1021/jacs.5b06150. Epub 2015 Aug 6.
Capture and recycling of CO2 into valuable chemicals such as alcohols could help mitigate its emissions into the atmosphere. Due to its inert nature, the activation of CO2 is a critical step in improving the overall reaction kinetics during its chemical conversion. Although pure gold is an inert noble metal and cannot catalyze hydrogenation reactions, it can be activated when deposited as nanoparticles on the appropriate oxide support. In this combined experimental and theoretical study, it is shown that an electronic polarization at the metal-oxide interface of Au nanoparticles anchored and stabilized on a CeO(x)/TiO2 substrate generates active centers for CO2 adsorption and its low pressure hydrogenation, leading to a higher selectivity toward methanol. This study illustrates the importance of localized electronic properties and structure in catalysis for achieving higher alcohol selectivity from CO2 hydrogenation.
将二氧化碳捕获和再循环为有价值的化学物质，如醇类，可以帮助减少其排放到大气中。由于其惰性性质，二氧化碳的活化是改善其化学转化过程中整体反应动力学的关键步骤。虽然纯金是一种惰性贵金属，不能催化加氢反应，但当它沉积在适当的氧化物载体上形成纳米颗粒时，就可以被激活。在这项结合实验和理论的研究中，研究表明，锚定并稳定在 CeO(x)/TiO2 衬底上的 Au 纳米颗粒的金属-氧化物界面处的电子极化产生了用于 CO2 吸附及其低压加氢的活性中心，从而导致甲醇的选择性更高。这项研究说明了局部电子特性和结构在催化中的重要性，这对于实现从 CO2 加氢中获得更高醇选择性具有重要意义。
