通过反应诱导的强金属支相互作用推翻高活性化选择性
Hui Xin1, Le Lin1, Rongtan Li1,2
1State Key Laboratory of Catalysis, iChEM, Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, P. R. China.
在二氧化碳化过程中,在低温下实现了强烈的金属支相互作用 (SMSI). 这种由氧化覆盖层对纳米颗粒的动态封装选择性地产生了具有高活性和稳定的CO.
科学领域:
- 催化剂
- 材料科学
- 表面化学
背景情况:
- 强金属支相互作用 (SMSI) 通常需要高温 (≥500°C) 进行金属纳米粒子由支材料封装.
- 这种经典的SMSI状态往往会导致由于活性部位的阻塞而导致催化性能降低.
研究的目的:
- 在二氧化碳化过程中研究Ru-MoO3催化剂中低温SMSI的形成.
- 了解动态封装的机制及其对催化选择性和活性的影响.
主要方法:
- 在250°C使用Ru-MoO3催化剂化CO2.
- 使用现场反应条件分析了Ru@MoO3封装结构的形成.
- 通过O2处理研究了SMSI状态的可逆性.
主要成果:
- 使用二氧化碳化气在250°C的低温下达到SMSI状态.
- 已证明选择性二氧化碳转化为二氧化碳的选择性>99.0%,取代了新鲜Ru催化剂100%的CH4选择性.
- 观察到优良的催化活性和长期稳定性.
- 显示封装氧化物层可以通过O2处理去除,恢复到甲化.
结论:
- 金属纳米催化剂的动态封装可以在反应过程中在现场生成.
- 低温SMSI形成提高了催化性能和产品选择性.
- 这种方法提供了一种控制向产品合成的催化剂行为的途径.
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