通过S/N双协调调节Fe单原子位的电子结构,以实现高效的芬顿式催化
Huiwang Dai1, Zhendong Zhao2, Kun Wang2
1Department of Environmental Science, Zhejiang University, Hangzhou, Zhejiang 310058, China; Zhejiang Ecological Civilization Academy, Anji, Zhejiang 310058, China.
Journal of hazardous materials
|January 1, 2024
概括
引入一种新型的硫和协调铁单原子催化剂 (Fe-SN-C) 增强过氧硫酸盐激活. 这种催化剂显著提高了双A降解效率,为环境修复技术提供了有前途的进步.
科学领域:
- 材料科学 材料科学 材料科学
- 环境化学环境化学
- 催化剂是一种催化剂.
背景情况:
- 单原子催化剂 (SAC) 对于过氧硫酸盐 (PMS) 激活至关重要,但它们的效率受到金属中心电子状态的限制.
- 在传统的金属-N4位点中的高电子阴性限制了电子传输,阻碍了PMS激活.
研究的目的:
- 开发一种新型的单原子催化剂,具有改进的电子特性,用于增强PMS激活.
- 调查硫和协调铁催化剂 (Fe-SN-C) 对于芬顿类反应的催化性能和机制.
主要方法:
- 合成Fe-SN-C催化剂,将硫纳入Fe单原子位的协调球体 (Fe-S1N3).
- 使用Fe-SN-C/PMS系统对双A降解的催化活性的评估.
- 在广泛的pH范围和在背景基质的存在下分析催化稳定性.
- 使用实验结果和理论计算 (例如,DFT) 来阐明催化机制.
主要成果:
- Fe-SN-C催化剂显著增强了双A降解的活性,速度常数为0.405分钟-1,比原始Fe-N-C高11.9倍.
- 该Fe-SN-C/PMS系统在不同的pH值和基质条件下表现出极好的催化稳定性,这是由于快速生成高价值Fe物种.
- 理论计算表明,双S和N协调优化了Fe的电子结构,增加了局部电子密度,并通过Fe3d-O2p轨道相互作用促进了PMS激活.
结论:
- 将硫纳入Fe单原子位的协调球中,有效调节电子结构,从而在PMS激活中获得优越的催化性能.
- Fe-SN-C催化剂是一个有希望的战略,通过芬顿式反应有效降解有机污染物.
- 这项研究强调了精确调节单原子催化剂的协调环境的重要性,以优化它们的催化活性和稳定性.
更多相关视频
10:52Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics
Published on: April 12, 2019
12.8K
10:59Author Spotlight: Tracking Electrochemistry on Single Nanoparticles with Surface-Enhanced Raman Scattering Spectroscopy and Microscopy
Published on: May 12, 2023
2.6K
相关概念视频
02:42Valence Bond Theory
8.6K
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...
8.6K
02:58Crystal Field Theory - Octahedral Complexes
26.6K
Crystal Field Theory
To explain the observed behavior of transition metal complexes (such as colors), a model involving electrostatic interactions between the electrons from the ligands and the electrons in the unhybridized d orbitals of the central metal atom has been developed. This electrostatic model is crystal field theory (CFT). It helps to understand, interpret, and predict the colors, magnetic behavior, and some structures of coordination compounds of transition metals.
CFT focuses on...
To explain the observed behavior of transition metal complexes (such as colors), a model involving electrostatic interactions between the electrons from the ligands and the electrons in the unhybridized d orbitals of the central metal atom has been developed. This electrostatic model is crystal field theory (CFT). It helps to understand, interpret, and predict the colors, magnetic behavior, and some structures of coordination compounds of transition metals.
CFT focuses on...
26.6K
02:51Metal-Ligand Bonds
20.8K
The hemoglobin in the blood, the chlorophyll in green plants, vitamin B-12, and the catalyst used in the manufacture of polyethylene all contain coordination compounds. Ions of the metals, especially the transition metals, are likely to form complexes.
In these complexes, transition metals form coordinate covalent bonds, a kind of Lewis acid-base interaction in which both of the electrons in the bond are contributed by a donor (Lewis base) to an electron acceptor (Lewis acid). The Lewis acid in...
In these complexes, transition metals form coordinate covalent bonds, a kind of Lewis acid-base interaction in which both of the electrons in the bond are contributed by a donor (Lewis base) to an electron acceptor (Lewis acid). The Lewis acid in...
20.8K
03:02Colors and Magnetism
11.7K
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...
11.7K
02:46Crystal Field Theory - Tetrahedral and Square Planar Complexes
42.6K
Tetrahedral Complexes
Crystal field theory (CFT) is applicable to molecules in geometries other than octahedral. In octahedral complexes, the lobes of the dx2−y2 and dz2 orbitals point directly at the ligands. For tetrahedral complexes, the d orbitals remain in place, but with only four ligands located between the axes. None of the orbitals points directly at the tetrahedral ligands. However, the dx2−y2 and dz2 orbitals (along the Cartesian axes) overlap with the ligands less than the dxy,...
Crystal field theory (CFT) is applicable to molecules in geometries other than octahedral. In octahedral complexes, the lobes of the dx2−y2 and dz2 orbitals point directly at the ligands. For tetrahedral complexes, the d orbitals remain in place, but with only four ligands located between the axes. None of the orbitals points directly at the tetrahedral ligands. However, the dx2−y2 and dz2 orbitals (along the Cartesian axes) overlap with the ligands less than the dxy,...
42.6K