从单个原子到集群:解开Pt/CeO2的结构演变,以增强CO氧化
1Center for Theoretical and Computational Chemistry, State Key Laboratory of Advanced Chemical Power Sources, Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Department of Chemistry, Nankai University, Tianjin 300071, China.
The journal of physical chemistry letters
|March 10, 2025
概括
在Ceria催化剂上的单个原子在CO氧化过程中演变为集群. 更高的吸附与替代原子的比率增强了催化活性,指导了有效的催化剂设计.
科学领域:
- 不同质的催化剂.
- 材料科学是一种材料科学.
- 表面化学 表面化学
背景情况:
- 了解催化剂结构演变和活性位点识别对于异质反应至关重要.
- 在 (Pt/CeO2) 上的是一种广泛研究的催化系统.
研究的目的:
- 研究CO氧化过程中Pt/CeO2催化剂的结构演变.
- 为了确定初始催化剂状态对活性点和反应性的影响.
- 为设计高效催化剂提供理论见解.
主要方法:
- 用理论计算来研究结构动态.
- 专注于单个原子转化为集群的过程.
- 分析替代 (Pt_in) 和吸附 (Pt_ad) 原子的作用.
主要成果:
- 在反应条件下,单个Pt原子聚合成集群.
- 从Pt_in形成的集群完全基于被替换的原子.
- Pt_in和Pt_ad的共存导致额外的吸附集群 (Pt_ad).
- 增加的Pt_ad/Pt_in比率导致更多的聚合物和增强的CO氧化活性.
结论:
- 在反应条件下,催化剂的结构演变和活性位点动态是至关重要的.
- 吸附到替代的原子的比例显著影响了催化性能.
- 理论见解可以指导先进的Pt/CeO2催化剂的合理设计.
相关概念视频
Turnover Number and Catalytic Efficiency
9.9K
The turnover number of an enzyme is the maximum number of substrate molecules it can transform per unit time. Turnover numbers for most enzymes range from 1 to 1000 molecules per second. Catalase has the known highest turnover number, capable of converting up to 2.8×106 molecules of hydrogen peroxide into water and oxygen per second. Lysozyme has the lowest known turnover number of half a molecule per second.
Chymotrypsin is a pancreatic enzyme that breaks down proteins during digestion....
Chymotrypsin is a pancreatic enzyme that breaks down proteins during digestion....
9.9K
Phase I Oxidative Reactions: Overview
221
Phase I biotransformation, or functionalization, is a crucial chemical process that converts drugs and other xenobiotics into more water-soluble forms, facilitating expulsion from the body. It involves oxidative, reductive, and hydrolytic reactions that add or unveil polar functional groups on lipophilic substrates. Key players in phase I reactions are the mixed-function oxidases. Situated in liver cell microsomes, these enzymes predominantly carry out drug metabolism. They require molecular...
221
Redox Equilibria: Overview
500
A reduction-oxidation reaction is commonly called a redox reaction. In a redox reaction, electrons are transferred from one species to another rather than being shared between or among atoms. The reducing agent or reductant is the species that loses electrons and gets oxidized in the process. The species that gains electrons and gets reduced in the process is the oxidizing agent or oxidant. Redox reactions are represented as two separate equations called half-reactions, where one equation...
500
Oxygen Transport in the Blood
2.4K
Hemoglobin (Hb) is a crucial molecule in the human body, consisting of four polypeptide chains, each bound to an iron-containing heme group. This unique structure enables hemoglobin to bind to oxygen, with each molecule capable of combining with four molecules of oxygen, leading to rapid and reversible oxygen loading. When fully loaded with oxygen, it is called oxyhemoglobin, while hemoglobin that has released oxygen is called reduced hemoglobin or deoxyhemoglobin. As hemoglobin binds oxygen,...
2.4K
Oxidation-Reduction Reactions
64.0K
Oxidation–Reduction Reactions
64.0K
Phase I Reactions: Oxidation of Carbon-Heteroatom and Miscellaneous Systems
55
Oxidative reactions are pivotal in metabolizing numerous compounds, including pharmaceutical drugs. These reactions often occur in carbon-heteroatom systems, such as carbon-nitrogen, carbon-sulfur, and carbon-oxygen.
In carbon-nitrogen systems, aliphatic and aromatic amines can undergo oxidative reactions. Secondary and tertiary amines, like those found in tricyclic antidepressants, can undergo N-dealkylation, a process that involves the oxidation of the alkyl group. In addition, oxidative...
In carbon-nitrogen systems, aliphatic and aromatic amines can undergo oxidative reactions. Secondary and tertiary amines, like those found in tricyclic antidepressants, can undergo N-dealkylation, a process that involves the oxidation of the alkyl group. In addition, oxidative...
55


