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Model car-exhaust catalyst studied by TPD and TP-RAIRS: Surface reactions of NO on clean and O-covered Ir{100}

机译:TPD和TP-RAIRS研究的模型汽车尾气催化剂:NO在纯净和O覆盖的Ir {100}上的表面反应

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The adsorption of NO on Ir{100} has been studied as a function of NO coverage and temperature using temperature programmed reflection absorption infrared spectroscopy (TP-RAIRS), low energy electron diffraction (LEED) and temperature programmed desorption (TPD). After saturating the clean (1 x 5)-reconstructed surface with NO at 95 K, two N_2 desorption peaks are observed upon heating. The first N_2 peak at 346 K results from the decomposition of bridge-bonded NO, and the second at 475 K from the decomposition of atop-bonded NO molecules. NO decomposition is proposed to be the rate limiting step for both N_2 desorption states. For high NO coverages on the (1 x 5) surface, the narrow width of the first N_2 desorption peak is indicative of an autocatalytic process for which the parallel formation of N_2O appears to be the crucial step. When NO is adsorbed on the metastable unreconstructed (1 x 1) phase of clean Ir{100} N_2 desorption starts at lower temperatures, indicating that this surface modification is more reactive. When a high coverage of oxygen, near 0.5 ML, is pre-adsorbed on the surface, the decomposition of NO is inhibited and mainly desorption of intact NO is observed.
机译:使用程序升温反射吸收红外光谱(TP-RAIRS),低能电子衍射(LEED)和程序升温脱附(TPD),研究了NO在Ir {100}上的吸附随NO覆盖率和温度的变化。在95 K下用NO饱和干净的(1 x 5)重建表面后,加热后观察到两个N_2解吸峰。在346 K处的第一个N_2峰是由桥键合的NO分解产生的,而在475 K处的第二个N_2峰是由键合上的NO分子的分解产生的。对于两个N_2解吸态,NO分解被提议为限速步骤。对于(1 x 5)表面上较高的NO覆盖率,第一个N_2解吸峰的较窄宽度表示自动催化过程,对于该过程,平行形成N_2O似乎是关键步骤。当NO吸附在纯Ir {100} N_2的亚稳态未重构(1 x 1)相上时,解吸在较低温度下开始,表明该表面改性更具反应性。当在表面上预吸附接近0.5 ML的高氧气含量时,NO的分解受到抑制,主要观察到完整NO的解吸。

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