促进稀土氧碳酸盐表面的分子交换,以催化水气转移反应
Lu-Lu Zhou1, Shan-Qing Li2, Chao Ma3
1Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan250100, China.
Journal of the American Chemical Society
|January 19, 2023
概括
稀土氧碳酸盐具有独特的"自我清洁"表面,可进行高效的异质催化. 这一发现通过防止催化剂失活和促进C1化学应用来增强水气转移反应.
科学领域:
- 材料科学与催化
- 纳米材料
- 稀土化学
背景情况:
- 不同质的催化需要可访问的催化剂表面,以有效地激活反应物和产品脱落.
- 保持催化剂活性和防止活性部位的阻塞是催化过程中的关键挑战.
研究的目的:
- 研究稀土氧碳酸盐 (Ln2O2CO3) 作为新型催化剂的支持.
- 为水气转移反应 (WGS) 开发高活性和稳定的催化剂.
- 了解稀土氧碳酸盐在催化反应中的表面化学作用.
主要方法:
- 在稀土氧碳酸盐 (La2O2CO3和Sm2O2CO3) 上通过沉积沉合成Cu催化剂.
- 催化剂性能和性能的实验性描述.
- 密度函数理论 (DFT) 的计算以阐明反应机制.
主要成果:
- 稀土氧碳酸盐具有分子可交换的表面结构,具有有序的Ln2O2^2+和CO3^2-离子.
- 支持Ln2O2CO3的Cu催化剂显示出WGS反应的良好活性和稳定性.
- DFT的计算和实验证实了Ln2O2CO3的自发H2O离合,释放了CO2并形成了基.
- 这种表面机制防止碳酸盐的积累,保持活跃点并促进WGS反应平衡.
结论:
- 稀土氧化碳提供了独特的
- 自动清洁
- 不同质催化剂的活性表面.
- 发现的机制提高了水气转移反应的效率和稳定性.
- 稀土氧碳酸纳米材料在C1化学中具有显著的应用潜力.
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