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Blocking the non-selective sites through surface plasmon-induced deposition of metal oxide on Au/TiO2 for CO-PROX reaction
Chem Catalysis Pub Date : 2021-05-17 , DOI: 10.1016/j.checat.2021.04.003
Feng Hong , Shengyang Wang , Junying Zhang , Bingsen Zhang , Keju Sun , Jiahui Huang , Botao Qiao , Na Ta , Mingrun Li , Dan Li , Weixin Huang , Masatake Haruta , Can Li

CO preferential oxidation (PROX) in excess hydrogen is a promising strategy for CO removal in hydrogen-rich reformate. However, the CO conversion and CO2 selectivity in the PROX reaction dramatically decrease with rising temperature, resulting in a major challenge to complete CO removal across a wide temperature window. Here, we developed a photoexcited deposition of metal oxide (PDMO) method based on surface plasmonic resonance of Au nanoparticles, which can tune the interfacial properties by depositing lead oxide at the Au-TiO2 interface. The interface modified Pb3O4/Au/TiO2 catalyst can successfully eliminate CO in a wide temperature range (70°C–140°C) and exhibit superior stability in the PROX reaction. Further experiments demonstrated that the improved PROX performance is due to the severely depressed hydrogen oxidation through simultaneously inhibiting the activation of hydrogen and oxygen. The results further reveal that the interface of Au/TiO2 is the superactive but non-selective site for H2 and CO oxidation.



中文翻译:

通过表面等离子体诱导的金属氧化物沉积在 Au/TiO 2 上用于 CO-PROX 反应来阻断非选择性位点

过量氢气中的 CO 优先氧化 (PROX) 是去除富氢重整油中 CO 的一种很有前景的策略。然而,PROX 反应中的 CO 转化率和 CO 2选择性随着温度的升高而显着降低,这导致在很宽的温度范围内完成 CO 去除是一项重大挑战。在这里,我们开发了一种基于 Au 纳米粒子表面等离子体共振的金属氧化物光激发沉积 (PDMO) 方法,该方法可以通过在 Au-TiO 2界面沉积氧化铅来调整界面特性。界面改性Pb 3 O 4 /Au/TiO 2催化剂可以在很宽的温度范围内(70°C-140°C)成功消除 CO,并在 PROX 反应中表现出优异的稳定性。进一步的实验表明,PROX 性能的提高是由于通过同时抑制氢和氧的活化而严重抑制了氢氧化。结果进一步表明,Au/TiO 2的界面是H 2和CO 氧化的超活性但非选择性位点。

更新日期:2021-07-15
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