使用-N-4-Schiff基复合物的电化学减少CO2到CO的理论研究
Wilasinee Santiwarodom1, Pavee Apilardmongkol1, Thanawit Kuamit1
1Center of Excellence in Computational Chemistry (CECC), Department of Chemistry, Faculty of Science, Chulalongkorn University, Pathumwan, Bangkok 10330, Thailand. Vudhichai.P@chula.ac.th.
Physical chemistry chemical physics : PCCP
|September 9, 2024
概括
这项研究探讨了-N4-Schiff基复合物用于电化学减少二氧化碳 (CO2) 到一氧化碳 (CO). 复合物1-Ni显示了最高的催化活性,催化剂电荷影响性能.
科学领域:
- 催化剂是一种催化剂.
- 计算化学计算化学
- 电化学 电化学 电化学
背景情况:
- 通过电化学方法减少二氧化碳 (CO2) 是可持续化工生产的一个有前途的途径.
- -N4-Schiff基复合物是二氧化碳转换的潜在催化剂.
- 了解反应机制对于催化剂设计至关重要.
研究的目的:
- 通过使用DFT来研究二氧化碳的电化学降解.
- 为了比较三种-N4-Schiff基复合物的催化活性:1-Ni,2-Ni和[2-Ni]Me.
- 阐明反应途径并确定影响催化性能的关键因素.
主要方法:
- 使用密度函数理论 (DFT) 的计算.
- 提出了两种减少二氧化碳的途径:外部和内部的质子转移.
- 计算了反应能量概况,包括过渡状态和激活能量.
主要成果:
- 没有过渡状态的外部质子转移途径显示了所有复合体的外热步骤.
- 复合物1-Ni的总反应能量最低 (-5.72 eV),表明具有较高的催化活性.
- 内部质子转移途径涉及过渡状态;复杂的1-Ni具有较低的激活能量 (0.83 eV),与实验数据保持一致.
结论:
- 复合物的催化活性与预吸附中心的电荷有关;较少的阳性电荷与较高的活性相关.
- 复杂的1-Ni显示出了二氧化碳电还原的巨大潜力.
- DFT计算为有效的二氧化碳减排催化剂的机制和设计提供了宝贵的见解.
相关概念视频
Electrodeposition
612
Electrodeposition is a technique used to separate an analyte from interferents by electrochemical processes. Here, the analyte is a metal ion that can be deposited on an electrode immersed in the sample solution. The electrochemical setup consists of an anode and a cathode. When an electric current is applied to the setup, oxidation occurs at the anode. At the cathode, which consists of a large metal surface, metal ions undergo reduction and deposit onto the surface.
Electrodeposition can...
Electrodeposition can...
612
Redox Equilibria: Overview
544
A reduction-oxidation reaction is commonly called a redox reaction. In a redox reaction, electrons are transferred from one species to another rather than being shared between or among atoms. The reducing agent or reductant is the species that loses electrons and gets oxidized in the process. The species that gains electrons and gets reduced in the process is the oxidizing agent or oxidant. Redox reactions are represented as two separate equations called half-reactions, where one equation...
544
Electrolysis
26.2K
In a galvanic cell, the electrical work is done by a redox system on its surroundings as electrons produced by the spontaneous redox reactions are transferred through an external circuit. Alternatively, an external circuit does work on a redox system by imposing a voltage sufficient to drive an otherwise nonspontaneous reaction in a process known as electrolysis. For instance, recharging a battery involves the use of an external power source to drive the spontaneous (discharge) cell reaction in...
26.2K
Oxidation and Reduction of Organic Molecules
6.3K
Energy production within a cell involves many coordinated chemical pathways. Most of these pathways are combinations of oxidation and reduction reactions, which occur at the same time. An oxidation reaction strips an electron from an atom in a compound, and the addition of this electron to another compound is a reduction reaction. Because oxidation and reduction usually occur together, these pairs of reactions are called redox reactions.
The removal of an electron from a molecule, results in a...
The removal of an electron from a molecule, results in a...
6.3K
Aldehydes and Ketones to Alkanes: Wolff–Kishner Reduction
4.4K
Wolff–Kishner reduction involves converting aldehydes and ketones to alkanes using hydrazine and a base. The reaction converts a carbonyl group to a methylene group. The method was independently discovered by N. Kishner in 1911 and L. Wolff in 1912. The reduction is carried out in high-boiling solvents such as ethylene glycol and diethylene glycol because heat is required to deprotonate the N–H proton in one of the reaction steps. ...
4.4K
Role of Reduced Coenzymes NADH and FADH₂
11.2K
The energy released from the breakdown of the chemical bonds within nutrients can be stored either through the reduction of electron carriers or in the bonds of adenosine triphosphate (ATP). In living systems, a small class of compounds functions as mobile electron carriers, molecules that bind to and shuttle high-energy electrons between compounds in pathways. The principal electron carriers that will be considered originate from the B vitamin group and are derivatives of nucleotides; they are...
11.2K


