近日，研究院硕士研究生姚美晶在美国化学期刊The Journal of Physical Chemistry C上发表题为《The Adsorption Mechanisms of Typical Carbonyl-Containing Volatile Organic Compounds on Anatase TiO2(001) Surface: A DFTInvestigation》的学术论文。该论文采用理论化学计算为研究手段，首次对室内大气中典型的含羰基类化合物乙醛、丙酮与乙酸甲酯在锐钛矿型二氧化钛催化剂(001)表面的吸附机制进行了系统的模拟研究。吸附机理表明：锐钛矿型二氧化钛催化剂(001)表面可以与羰基化合物通过五配位Ti原子发生化学吸附反应，且乙醛、丙酮与乙酸甲酯在锐钛矿(001)表面的吸附均具有热力学稳定性，其吸附顺序为乙醛＞丙酮≈乙酸甲酯。这研究结果说明尽管大气羰基污染物的取代基效应会让含羰基类化合物的吸附能下降，但是取代基的大小并不会明显影响其吸附机理，因此含有裸露羰基的大气羰基化合物更容易稳定地吸附在该催化剂表面。该论文提供的数据可以为正确理解含羰基类挥发性有机化合物在锐钛矿催化剂表面的吸附机理提供详细的理论依据，也可以进一步为光催化技术净化羰基挥发性有机物的实际应用研究提供良好的技术支撑。
Abstract:The carbonyl-containing compounds (CCs) are typical volatile organic compounds (VOCs) and ubiquitously present in the environment. Hence, the adsorption mechanisms of typical CCs on anatase TiO2(001) surface were investigated systematically usingdensity functional theory (DFT). The adsorption mechanisms show that three typical CCs, acetaldehyde, acetone and methylacetate, areeasily trapped on the anatase TiO2(001) surface via the interaction between carbonyl group with Ti5csites of catalyst surface. Especially for acetaldehyde,because the bare carbonyl group interacts with both Ti5catom and O2catom of the surface, it hasthe strongest adsorption energy, leading to be trapped stably by catalytic surface. The substituent effect of different CCs has less impact on its adsorption models in thesestudied systems, and the bare carbonyl group is the key functional group. Our theoretical results are expected to provide insight into the adsorption mechanisms of CCs on TiO2catalyst and to help understand the further catalytic degradation mechanisms of air pollutants at the molecular level.
论文下载地址：
http://pubs.acs.org/doi/abs/10.1021/acs.jpcc.7b02964
