在催化中利用相过渡:CO2和H2在杂的VO2-多态体上反应
Berenike Stahl1, Thomas Bredow1
1Mulliken Center for Theoretical Chemistry, Clausius-Institute for Physical and Theoretical Chemistry, University of Bonn, Beringstr. 4, D-53115 Bonn, Germany.
Journal of physics. Condensed matter : an Institute of Physics journal
|December 29, 2023
概括
二氧化瓦纳 (VO2) 阶段过渡影响二氧化碳化. 不同的多态提供不同的吸附能量,改变反应热力学和催化作用的动力学.
科学领域:
- 材料科学 材料科学 材料科学
- 表面化学 表面化学
- 催化剂是一种催化剂.
背景情况:
- 二氧化瓦纳 (VO2) 呈现了四边形路和单结构之间的可逆相过渡.
- 之前的研究表明,在Mo稳定的VO2多态体上,二氧化碳吸附能量不同.
- 这种差异可以通过管理CO表面覆盖率来提高催化反应.
研究的目的:
- 研究VO2相转换对影响CO2化热力学和动力学的潜力.
- 证明使用VO2多态来调整催化反应路径的原理证明.
- 探索基于VO2相过渡的催化循环的可行性.
主要方法:
- 密度函数理论 (DFT) 对二氧化碳,中间体和产品的吸附能量的计算.
- 无弹性带 (NEB) 方法用于计算二氧化碳化反应障碍物.
- 区分反应坐标 (DRC) 方法用于确定 VO2 大量相位过渡的最小能量路径.
主要成果:
- 在VO2多态体之间观察到二氧化碳化到酸和甲的反应能量的显著差异.
- 发现VO2与气相相比,降低了CO2化反应障碍.
- 阐明了无兴奋剂的VO2批量相转换的最小能量路径.
结论:
- VO2相转换可以改变CO2化热力学和动力学.
- 通过稳定特定的VO2多态,可以优化催化反应条件.
- 基于理论发现,提出了一个利用VO2相变的新型催化循环.
更多相关视频
相关概念视频
Catalysis
26.9K
The presence of a catalyst affects the rate of a chemical reaction. A catalyst is a substance that can increase the reaction rate without being consumed during the process. A basic comprehension of a catalysts’ role during chemical reactions can be understood from the concept of reaction mechanisms and energy diagrams.
26.9K
Phase I Reactions: Oxidation of Carbon-Heteroatom and Miscellaneous Systems
99
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...
99
Oxidation of Alkenes: Syn Dihydroxylation with Osmium Tetraoxide
10.2K
Alkenes are converted to 1,2-diols or glycols through a process called dihydroxylation. It involves the addition of two hydroxyl groups across the double bond with two different stereochemical approaches, namely anti and syn. Dihydroxylation using osmium tetroxide progresses with syn stereochemistry.
10.2K
Oxidation of Alkenes: Syn Dihydroxylation with Potassium Permanganate
11.5K
Alkenes can be dihydroxylated using potassium permanganate. The method encompasses the reaction of an alkene with a cold, dilute solution of potassium permanganate under basic conditions to form a cis-diol along with a brown precipitate of manganese dioxide.
11.5K
Reduction of Alkenes: Catalytic Hydrogenation
12.0K
Alkenes undergo reduction by the addition of molecular hydrogen to give alkanes. Because the process generally occurs in the presence of a transition-metal catalyst, the reaction is called catalytic hydrogenation.
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
12.0K
Reduction of Alkenes: Asymmetric Catalytic Hydrogenation
3.3K
Catalytic hydrogenation of alkenes is a transition-metal catalyzed reduction of the double bond using molecular hydrogen to give alkanes. The mode of hydrogen addition follows syn stereochemistry.
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
3.3K


