Chilukoti Srilakshmi, Gao Feng, Anderson Bruce G, Niemantsverdriet J W Hans, Garland Marc
Institute of Chemical and Engineering Sciences, 1 Pesek Road, Jurong Island, Singapore, 627833.
Phys Chem Chem Phys. 2008 Sep 28;10(36):5510-20. doi: 10.1039/b806890a. Epub 2008 Jul 18.
The adsorption of NO and CO was studied on an alumina-supported palladium catalyst by in situ diffuse reflectance infrared spectroscopy (DRIFTS). The temperature range was 50-160 degrees C and a wide variety of partial pressures was used. The band-target entropy minimization (BTEM) algorithm was applied to the DRIFTS data sets resulting in the pure component spectra of numerous species adsorbed on both the Pd (primarily a variety of Pd-CO and Pd-NO species, in various oxidation states and coordinations) and alumina surface species (i.e. nitrates, nitrites, carbonates, bicarbonates, formates, and isocyanates) as well as gas phase species. Twenty seven previously known species were identified as well as three new and previously unreported or previously unassigned spectra. The present study indicates that BTEM can be meaningfully applied to Pd/Al2O3 DRIFTS in order to provide enhanced spectroscopic analysis. Moreover, the present results are compared in detail with the recent BTEM analysis of CO and NO adsorption on Pt/Al2O3 using DRIFTS (Phys. Chem. Chem. Phys. 2008, 10, 3535).
采用原位漫反射红外光谱(DRIFTS)研究了一氧化氮(NO)和一氧化碳(CO)在氧化铝负载钯催化剂上的吸附情况。温度范围为50 - 160摄氏度,并使用了多种分压。将带目标熵最小化(BTEM)算法应用于DRIFTS数据集,得到了吸附在钯(主要是各种处于不同氧化态和配位状态的钯 - 一氧化碳和钯 - 一氧化氮物种)和氧化铝表面物种(即硝酸盐、亚硝酸盐、碳酸盐、碳酸氢盐、甲酸盐和异氰酸酯)以及气相物种上的众多物种的纯组分光谱。鉴定出了27种先前已知的物种以及三种新的、以前未报道或未归属的光谱。本研究表明,BTEM可有效地应用于钯/氧化铝DRIFTS,以提供增强的光谱分析。此外,将本研究结果与最近使用DRIFTS对一氧化碳和一氧化氮在铂/氧化铝上吸附的BTEM分析(《物理化学化学物理》,2008年,第10卷,第3535页)进行了详细比较。