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调整单个原子和Ceria之间的相互作用,通过对的化剂进行有效的催化氨氧化

Wei Tan^1,2, Yandi Cai¹, Haowei Yu¹

¹State Key Laboratory of Pollution Control and Resource Reuse, School of Environment, Jiangsu Key Laboratory of Vehicle Emissions Control, Center of Modern Analysis, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China.

Environmental science & technology

|October 3, 2023

概括

这项研究开发了高效的单原子催化剂,用于氨 (NH3) 氧化,在化的化上. 优化的Pt1/Ce0.9Zr0.1O2催化剂在消除有害的NH3滑落方面表现出卓越的性能.

科学领域:

材料科学材料科学材料科学
催化剂是一种催化剂.
环境化学环境化学

背景情况:

氨 (NH3) 滑落是固定脱和柴油排气系统中的重要污染物.
开发高效的低温NH3氧化催化剂对于环境保护至关重要.
基于的催化剂,特别是单原子催化剂,显示出希望,但需要优化支持相互作用.

研究的目的:

开发一种用于构建高效NH3氧化催化剂的简单策略.
研究ZrO2兴奋剂对Pt/CeO2催化剂结构和活性的影响.
阐明NH3氧化性能增强背后的机制.

主要方法:

使用ZrO2兴奋剂策略合成Pt1/Ce(x) Zr(1-x) O2催化剂.
系统性表征包括 (但不限于) X射线衍射,传输电子显微镜和X射线光电子谱学.
使用in-situ/operando技术评估NH3氧化活性和机制研究.

主要成果:

当x >= 0.7.7时,Pt物种存在于Ce(x) Zr(1-x) O2上作为单个原子.
观察到Pt-CeO2相互作用强度和Pt-O-Ce协调数 (CN(Pt-O-Ce)) 的火山趋势,其中ZrO2含量各不相同.
由于增强的Pt-CeO2相互作用和最佳的氧缺陷度,Pt1/Ce0.9Zr0.1O2表现出明显更高的NH3氧化活性.

结论:

在单原子Pt催化剂中,ZrO2兴奋剂有效调整了Pt-CeO2相互作用和协调环境.
该Pt1/Ce0.9Zr0.1O2催化剂显示出优越的低温NH3氧化活性.
这项工作为设计高效Pt/CeO2基催化剂的NH3减排提供了一种新的方法.

关键词:

氧化 NH3 的过程中.Pt 单个原子催化剂在 Pt-CeO2 相互作用中.Pt−O−Ce的协调号码是这是一个ZrO2兴奋剂策略.

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