CO2 电还原反应通过一个二维TM@TAP单原子催化剂.
Xiaolin Wang1, Qing Zhang2, Shenghai Zhang1
1School of Chemistry and Chemical Engineering, Ankang Research Centre of New Nano-materials Science and Technology, Qinba Chinese Medicine Resources R&D Center, Ankang University Ankang 725000 China wangxlchem@foxmail.com.
RSC advances
|December 6, 2023
概括
过渡金属原子固的单层过渡金属二甲基化物 (TM@TAP) 作为二氧化碳还原反应 (CO2RR) 的电催化剂具有前景. 像Cr@TAP和Rh@TAP这样的特定催化剂表现出高活性和对所需产品的选择性.
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
- 计算化学计算化学
背景情况:
- 电催化二氧化碳的减少对于可持续能源至关重要.
- 开发高效和选择性的电催化剂是一个关键的挑战.
- 单层过渡金属二甲基化物为催化提供可调节的电子特性.
研究的目的:
- 系统地研究TM@TAP作为CO2RR的电催化剂.
- 探索反应机制和产品选择性.
- 为特定的减少产品确定高度活性和选择性的催化剂.
主要方法:
- 在理论选中使用了第一原则计算.
- 考虑通过H和OH中间体阻断活性部位.
- 对反应途径和限制潜力的详细分析.
主要成果:
- Cr@TAP,Zn@TAP,Mo@TAP和Cd@TAP可以选择性地产生HCOOH.
- Mn@TAP和Rh@TAP有利于二氧化碳的产生.
- 铁@TAP可以产生CH3OH,Co@TAP可以产生HCHO,而TC@TAP/Ru@TAP可以产生CH4.
- Cr@TAP (-0.33 V) 和Rh@TAP (-0.28 V) 显示出高活性.
- Fe@TAP 显示了 CH3OH 生产 (-0.51 V) 的潜力.
结论:
- TM@TAP电催化剂对CO2RR具有不同的选择性.
- Cr@TAP,Rh@TAP和Fe@TAP是具体的二氧化碳减排产品的有希望的候选产品.
- 该研究为CO2RR电催化剂的合理设计提供了见解.
相关概念视频
Thermal and Photochemical Electrocyclic Reactions: Overview
2.3K
Electrocyclic reactions are reversible reactions. They involve an intramolecular cyclization or ring-opening of a conjugated polyene. Shown below are two examples of electrocyclic reactions. In the first reaction, the formation of the cyclic product is favored. In contrast, in the second reaction, ring-opening is favored due to the high ring strain associated with cyclobutene formation.
2.3K
Thermal Electrocyclic Reactions: Stereochemistry
2.0K
The stereochemistry of electrocyclic reactions is strongly influenced by the orbital symmetry of the polyene HOMO. Under thermal conditions, the reaction proceeds via the ground-state HOMO.
Selection Rules: Thermal Activation
Conjugated systems containing an even number of π-electron pairs undergo a conrotatory ring closure. For example, thermal electrocyclization of (2E,4E)-2,4-hexadiene, a conjugated diene containing two π-electron pairs, gives trans-3,4-dimethylcyclobutene.
Selection Rules: Thermal Activation
Conjugated systems containing an even number of π-electron pairs undergo a conrotatory ring closure. For example, thermal electrocyclization of (2E,4E)-2,4-hexadiene, a conjugated diene containing two π-electron pairs, gives trans-3,4-dimethylcyclobutene.
2.0K
Interfacial Electrochemical Methods: Overview
251
Interfacial electrochemical methods focus on the phenomena occurring at the boundary between an electrode and a solution, as opposed to bulk methods that concentrate on the solution's overall properties. These interfacial methods are classified as either static or dynamic based on the presence of a nonzero current in the electrochemical cell and the consistency of analyte concentrations. Static methods, such as potentiometry, measure the cell's potential without any significant current...
251
Chemiosmosis
98.8K
Oxidative phosphorylation is a highly efficient process that generates large amounts of adenosine triphosphate (ATP), the basic unit of energy that drives many cellular processes. Oxidative phosphorylation involves two processes— the electron transport chain and chemiosmosis.
Electron Transport Chain
The electron transport chain involves a series of protein complexes on the inner mitochondrial membrane that undergo a series of redox reactions. At the end of this chain, the electrons...
Electron Transport Chain
The electron transport chain involves a series of protein complexes on the inner mitochondrial membrane that undergo a series of redox reactions. At the end of this chain, the electrons...
98.8K
E2 Reaction: Kinetics and Mechanism
10.3K
SN2 substitutions and E2 eliminations of alkyl halides proceed via a concerted pathway. While the nucleophile attacks the alpha carbon in SN2 reactions, it functions as a strong base and abstracts a beta hydrogen in the E2 mechanism. The rate-limiting transition state in E2 elimination reactions is characterized by partially broken carbon–hydrogen and carbon–halogen bonds and a partially formed pi bond between the alpha and beta carbons. The beta hydrogen and halide are eliminated...
10.3K
Double Resonance Techniques: Overview
214
Double resonance techniques in Nuclear Magnetic Resonance (NMR) spectroscopy involve the simultaneous application of two different frequencies or radiofrequency pulses to manipulate and observe two distinct nuclear spins. One important application of double resonance is spin decoupling, which selectively suppresses coupling with one type of nucleus while observing the NMR signal from another nucleus, simplifying the spectrum and enhancing resolution.
Spin decoupling is usually achieved by...
Spin decoupling is usually achieved by...
214


