硫兴奋剂梯度调节了单原子催化剂中的自旋轨道工程:优化了d-p轨道杂交,以实现高效的过氧单硫酸盐激活
Pengyu Zhang1, Hao Huang2, Weikai Kong3
1Environmental Materials and Pollution Control Laboratory, Institute of Solid State Physics (ISSP), HFIPS, Chinese Academy of Sciences (CAS), Hefei 230031, China; University of Science and Technology of China (USTC), Hefei 230026, China.
Water research
|November 8, 2025
概括
在单原子催化剂 (SAC) 中的硫注射优化了电子配置,以增强过氧硫酸盐 (PMS) 激活. Co-S1N3催化剂在通过电子转移降解硫法迪亚方面表现出卓越的性能.
科学领域:
- 环境化学环境化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 单原子催化剂 (SAC) 的合理设计对于基于过氧化硫酸盐的先进氧化过程 (PMS-AOP) 是至关重要的.
- 在SAC中,了解协调环境,电子配置和催化功能之间的关系是有限的.
研究的目的:
- 使用硫梯度兴奋剂策略,设计具有调节电子配置的SAC.
- 调查协调几何学和电子状态对PMS激活对硫法酸降解的影响.
主要方法:
- 通过硫梯度兴奋剂开发了一系列Co-SxN4-x (x = 0,1,2,3) 单原子催化剂.
- 采用多尺度表征技术和理论分析来研究催化剂结构和电子特性.
- 评估过氧单硫酸盐激活的硫法酸盐降解中的催化活性和阐明反应机制.
主要成果:
- 硫兴奋剂诱导了结构性从平面到扭曲的四面体协调的过渡,改变了的自旋状态.
- 中间旋转的Co-S1N3配置表现出火山类型的活动趋势,实现了卓越的催化性能.
- 优化的Co 3d-O 2p轨道杂交和s-键吸附强度促进了电子转移动力学.
结论:
- 建立了一个"旋转轨道"活动框架,用于设计高效的SAC.
- 硫梯度工程协同调节旋转状态和轨道杂交,以实现高性能催化.
- 为开发可持续水资源整治的SAC提供了通用范式.
相关概念视频
Oxidation of Alkenes: Syn Dihydroxylation with Potassium Permanganate
16.3K
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.
16.3K
Oxidation of Alkenes: Syn Dihydroxylation with Osmium Tetraoxide
12.5K
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.
12.5K
Colors and Magnetism
13.9K
Color in Coordination Complexes
When atoms or molecules absorb light at the proper frequency, their electrons are excited to higher-energy orbitals. For many main group atoms and molecules, the absorbed photons are in the ultraviolet range of the electromagnetic spectrum, which cannot be detected by the human eye. For coordination compounds, the energy difference between the d orbitals often allows photons in the visible range to be absorbed and emitted, which is seen as colors by the human...
When atoms or molecules absorb light at the proper frequency, their electrons are excited to higher-energy orbitals. For many main group atoms and molecules, the absorbed photons are in the ultraviolet range of the electromagnetic spectrum, which cannot be detected by the human eye. For coordination compounds, the energy difference between the d orbitals often allows photons in the visible range to be absorbed and emitted, which is seen as colors by the human...
13.9K
Spin–Spin Coupling: One-Bond Coupling
1.4K
Coupling interactions are strongest between NMR-active nuclei bonded to each other, where spin information can be transmitted directly through the pair of bonding electrons. While nuclei polarize their electrons to the opposite spins, the bonding electron pair has opposite spins. Configurations with antiparallel nuclear spins are expected to be lower in energy. When coupling makes antiparallel states more favorable, J is considered to have a positive value. The one-bond coupling constant, 1J,...
1.4K
Valence Bond Theory
11.1K
Coordination compounds and complexes exhibit different colors, geometries, and magnetic behavior, depending on the metal atom/ion and ligands from which they are composed. In an attempt to explain the bonding and structure of coordination complexes, Linus Pauling proposed the valence bond theory, or VBT, using the concepts of hybridization and the overlapping of the atomic orbitals. According to VBT, the central metal atom or ion (Lewis acid) hybridizes to provide empty orbitals of suitable...
11.1K
Structural Isomerism
21.4K
Isomerism in Complexes
Isomers are different chemical species that have the same chemical formula. Structural isomerism of coordination compounds can be divided into two subcategories, the linkage isomers and coordination-sphere isomers.
Linkage isomers occur when the coordination compound contains a ligand that can bind to the transition metal center through two different atoms. For example, the CN− ligand can bind through the carbon atom or through the nitrogen atom. Similarly, SCN− can...
Isomers are different chemical species that have the same chemical formula. Structural isomerism of coordination compounds can be divided into two subcategories, the linkage isomers and coordination-sphere isomers.
Linkage isomers occur when the coordination compound contains a ligand that can bind to the transition metal center through two different atoms. For example, the CN− ligand can bind through the carbon atom or through the nitrogen atom. Similarly, SCN− can...
21.4K


