Talin Avanesian , Zubin Darbari , Marija Iloska , J. Anibal Boscoboinik , Qin Wu
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引用次数: 0
摘要
一氧化碳键的拉伸频率是表面结合的一氧化碳分子局部环境的敏感探测器,包括吸附位点和密度,即表面覆盖率。在这项工作中,我们将分析范围扩展到了因吸附构型不同而产生的频率偏移之外。利用密度泛函理论(DFT)计算,我们直接探索了表面覆盖率与钯表面吸附的 CO 拉伸频率之间的相关性。我们还对钯(111)上的 CO 进行了恒压红外反射吸收测量,并利用压力和覆盖率之间的现有关系得出了覆盖率依赖性。这两个结果都与之前报告的实验数据进行了比较。我们推导出的峰值频率和面积与表面覆盖率的相关性有助于实时解释实验红外光谱,并从瞬态动力学实验中提取随时间变化的浓度数据。
Investigation of coverage dependence of the stretching frequency of CO adsorbed on Pd surfaces at low coverage limits
The stretching frequency of the CO bond is a sensitive probe of the local environment of a surface-bound CO molecule, including the adorption site and density, i.e. surface coverage. In this work, we extend our analysis beyond the frequency shift due to differences in adsorption configurations. Using density functional theory (DFT) calculations, we directly explore the correlations between surface coverage and the stretching frequency of adsorbed CO on Pd surfaces. We also perform constant pressure infrared reflection absorption measurements of CO on Pd(111) and use existing relations between pressure and coverage to derive coverage dependency. Both results are compared to previously reported experimental data. Our derived correlations of peak frequency and area with surface coverage can help interpret experimental IR spectra in real time and extract time-dependent concentration data from transient kinetic experiments.
期刊介绍:
Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to:
• model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions
• nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena
• reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization
• phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization
• surface reactivity for environmental protection and pollution remediation
• interactions at surfaces of soft matter, including polymers and biomaterials.
Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.