在Fe-N-C催化剂中通过高能p轨道进行双极效应,以增强酸氧减氧反应
Chen Yang1, Bo Liu1, Yunlong Zhang1
1State Key Laboratory of Space Power-Sources, MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, MOE Engineering, Research Center for Electrochemical Energy Storage and Carbon Neutrality in Cold Regions, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, Heilongjiang, 150001, China.
Angewandte Chemie (International ed. in English)
|December 22, 2025
概括
具有N-XVA双极的工程铁单原子催化剂显示了氧降解反应的增强稳定性和活性. 这一突破在与催化剂相比,在质子交换膜燃料电池 (PEMFC) 中提供了卓越的性能.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
背景情况:
- 调节金属单原子催化剂是性能的关键.
- 第一个协调的修改降低了稳定性;第二个的修改效果有限.
- 设计单个Fe原子的电子结构对于高效的催化是至关重要的.
研究的目的:
- 为了引入N-XVA二极管来设计Fe单原子催化剂.
- 研究N-XVA双极对Fe3d轨道调制和OH*结合能量的影响.
- 评估工程催化剂在氧气还原反应和质子交换膜燃料电池 (PEMFC) 中的催化活性和稳定性.
主要方法:
- 合成FeN4-Sb/C催化剂,其中包括N-XVA双极体.
- 氧降解反应 (ORR) 活性的电化学表征.
- 加速耐久性测试 (3万个周期).
- 使用开发的催化剂制造和测试PEMFCs.
主要成果:
- N-XVA二极管增强Fe原子两极化,并优化OH*结合能,接近火山情节峰值.
- 在耐用性测试后,FeN4-Sb/C催化剂实现了高半波潜力 (0.833 V) 和最小降解 (18 mV).
- 含有FeN4-Sb/C的PEMFC显示出高功率密度 (H2-O2: 1.1 W cm-2; H2-空气: 0.6 W cm-2),性能优于商业Pt/C和其他单原子/双原子催化剂.
结论:
- 该研究揭示了Fe单原子催化剂的双极调节ORR活动的周期性趋势.
- N-XVA二极管有效地提高了催化剂性能和稳定性.
- FeN4-Sb/C催化剂显示出在PEMFC中实际应用的巨大潜力.
相关概念视频
Catalysis
30.0K
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.
30.0K
Reactivity of Enolate Ions
3.2K
Enolate ions are formed by the acid–base reaction of a carbonyl compound with a base. This leads to deprotonation of the α hydrogen atom, leading to a resonance-stabilized enolate ion where one of the contributing structures is an oxyanion, which imparts additional stability. Therefore, the proton on the α carbon is more acidic in nature than that of other sp3-hybridized C–H bonds but less acidic than those in O–H bonds where the negative charge in the conjugate...
3.2K
Nuclear Overhauser Enhancement (NOE)
1.3K
Irradiation of a spin-active nucleus causes an increase or decrease in the signal intensity of neighboring nuclei that are not necessarily chemically bonded or involved in J-coupling. This phenomenon, called the nuclear Overhauser enhancement (NOE), results from through-space interactions between the nuclear spins. The NOE effect decreases with increasing internuclear distance and is generally not observed beyond 4 angstroms. In NOE, dipole-dipole interactions between neighboring spin-active...
1.3K
Reduction of Alkenes: Asymmetric Catalytic Hydrogenation
3.8K
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...
3.8K
Crystal Field Theory - Octahedral Complexes
30.4K
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...
30.4K
π Electron Effects on Chemical Shift: Overview
1.6K
An applied magnetic field causes loosely bound π-electrons in organic molecules to circulate, producing a local or induced diamagnetic field over a large spatial volume. As the molecules tumble in solution, the field generated by π-electrons in spherical substituents results in a zero net field. However, the net field generated by π-electrons in non-spherical substituents is not zero. The effect of this induced field depends on the orientation of the molecule with respect to B0,...
1.6K


