二原子活性点嵌入了石墨烯作为氨基合成的电催化剂
Xiaoting Chen1,2, Man-Rong Zhao2, Bingyi Song2
1Key Laboratory of Theoretical Chemistry of Environment, Ministry of Education; School of Chemistry, South China Normal University, Guangzhou 510006, China.
ACS applied materials & interfaces
|October 23, 2024
概括
在石墨烯上使用的双过渡金属二原子催化剂 (DAC) 显示出通过电化学降解有效合成氨的前景. 最好的催化剂,Mn2@GY,显示没有发病潜力,突出了催化剂设计的新范式.
科学领域:
- 计算材料科学 计算材料科学
- 催化剂是一种催化剂.
- 电化学 电化学 电化学
背景情况:
- 氨 (NH3) 对工业和农业至关重要.
- 电化学降解反应 (eNRR) 提供了一种可持续的NH3合成途径.
- 目前的ENRR方法存在高超电位和低法拉第效率的问题.
研究的目的:
- 研究在石墨烯 (GY) 上固定的双过渡金属二原子催化剂 (DAC) 作为 eNRR 的电催化剂.
- 用理论计算来确定氨合成的高活性和选择性催化剂.
主要方法:
- 使用密度函数理论 (DFT) 的计算.
- 使用了四个阶段的分层高通量选过程.
- 稳定性,初始潜力和选择性被评估为催化剂选择.
主要成果:
- 由于更好的活性部位暴露,Graphyne-anchored DACs表现出增强的活性.
- 从最初的325名候选人中确定了13种符合条件的催化剂.
- Mn2@GY没有出现发病潜力,而Ir2@GY和RhOs@GY的发病潜力分别为-0.07V和-0.12V.
结论:
- 石墨烯上的DAC对于高效的氨基合成具有重要意义.
- 该研究为设计ENRR和其他反应的催化剂提供了一个新的范式.
- 催化剂和N2之间的有效电荷转移和轨道相互作用是高催化活性的关键.
相关概念视频
Catalysis
26.7K
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.
26.7K
Structure of Amines
2.5K
The hybridized nitrogen atom in amines possesses a lone pair of electrons and is bound to three substituents with a bond angle of around 108°, which is less than the tetrahedral angle of 109.5°. However, the C–N–H bond angle is slightly larger at 112°, with a carbon–nitrogen bond length of 147 pm. This carbon–nitrogen bond length of of amines is longer than the carbon–oxygen bond of alcohols (143 pm) but shorter than alkanes’...
2.5K
Preparation of 1° Amines: Gabriel Synthesis
3.5K
Direct alkylation is not a suitable method for synthesizing amines because it produces polyalkylated products. Gabriel synthesis is the most preferred method to exclusively make primary amines. The method uses phthalimide, which contains a protected form of nitrogen that participates in alkylation only once to predominantly give primary amines.
Strong bases like NaOH or KOH deprotonate the phthalimide to form the corresponding anion, which acts as a nucleophile. Further, the anion attacks an...
Strong bases like NaOH or KOH deprotonate the phthalimide to form the corresponding anion, which acts as a nucleophile. Further, the anion attacks an...
3.5K
Acidity of 1-Alkynes
9.6K
The acidic strength of hydrocarbons follows the order: Alkynes > Alkenes > Alkanes. The strength of an acid is commonly expressed in units of pKa — the lower the pKa, the stronger the acid. Among the hydrocarbons, terminal alkynes have lower pKa values and are, therefore, more acidic. For example, the pKa values for ethane, ethene, and acetylene are 51, 44, and 25, respectively, as shown here.
9.6K
Reduction of Alkynes to trans-Alkenes: Sodium in Liquid Ammonia
9.1K
Alkynes can be reduced to trans-alkenes using sodium or lithium in liquid ammonia. The reaction, known as dissolving metal reduction, proceeds with an anti addition of hydrogen across the carbon–carbon triple bond to form the trans product. Since ammonia exists as a gas (bp = −33°C) at room temperature, the reaction is carried out at low temperatures using a mixture of dry ice (sublimes at −78°C) and acetone.
When dissolved in liquid ammonia, an alkali metal,...
When dissolved in liquid ammonia, an alkali metal,...
9.1K
Preparation of Amines: Reductive Amination of Aldehydes and Ketones
2.7K
Carbonyl compounds and primary amines undergo reductive amination first to produce imines, followed by secondary amines in the same reaction mixture, using selective reducing agents like sodium cyanoborohydride or sodium triacetoxyborohydride. Reductive amination produces different degrees of substitution of amines depending on the starting amine substrate.
2.7K


