Developing single-site Pt catalysts for the preferential oxidation of CO: A surface science and first principles-guided approach
Developing single-site Pt catalysts for the preferential oxidation of CO: A surface science and first principles-guided approach
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DOI：
10.1016/j.apcatb.2020.119716
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发表时间：
2021-05
期刊：
影响因子：
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通讯作者：
Jilei Liu;Alyssa J. R. Hensley;G. Giannakakis;A. Therrien;A. Sukkar;A. Schilling;Kyle Groden;Nisa Ulumuddin;Ryan T. Hannagan;M. Ouyang;M. Flytzani-Stephanopoulos;Jean-Sabin McEwen;E. Sykes
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文献类型：
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作者：
Jilei Liu;Alyssa J. R. Hensley;G. Giannakakis;A. Therrien;A. Sukkar;A. Schilling;Kyle Groden;Nisa Ulumuddin;Ryan T. Hannagan;M. Ouyang;M. Flytzani-Stephanopoulos;Jean-Sabin McEwen;E. Sykes
我们报告了一项综合研究，结合了表面科学、密度泛函理论 (DFT) 计算以及催化剂合成、表征和测试，以研究在 H2 存在下 CO 相对于单中心 Pt1/CuxO 催化剂的优先氧化。表面科学研究表明，虽然 Pt1/CuxO 模型表面能够通过 Mars-van Krevelen 机制实现低温 CO 氧化，但没有证据表明 H2 活化或氧化。基于 DFT 的计算解释了这些结果，并证明与 Pt1/CuxO 的 H2 解吸相比，H2 氧化势垒较高。受这些模型催化剂研究的启发，合成了纳米多孔 Pt1/CuxO 催化剂，并被证明对 CO 优先氧化具有活性和高选择性。这项工作突出了表面科学、理论和催化剂研究相结合在识别新催化材料方面的潜力，在这种情况下，开发了一种有前途的用于 CO 优先氧化的单中心 Pt1/CuxO 催化剂。
We report a comprehensive study combining surface science, Density Functional Theory (DFT) calculations, and catalyst synthesis, characterization, and testing to investigate the preferential oxidation of CO in the presence of H2over single-site Pt1/CuxO catalysts. Surface science studies show that while Pt1/CuxO model surfaces enable low-temperature CO oxidation via a Mars-van Krevelen mechanism, there was no evidence for H2activation or oxidation. DFT-based calculations explain these results and demonstrate that the H2oxidation barrier is high as compared to H2desorption from Pt1/CuxO. Inspired by these model catalyst studies, nanoporous Pt1/CuxO catalysts were synthesized and demonstrated to be active and highly selective for the preferential oxidation of CO. This work highlights the potential of combined surface science, theory, and catalyst studies for identifying new catalytic materials, which in this case led to the development of a promising single-site Pt1/CuxO catalyst for the preferential oxidation of CO.