Li Zong-Xu, Tian Sheng, Hu Qing, Huang Xin-Yi, Tan Hong-Yi, Guo Jun-Kang, Yin Shuang-Feng
Advanced Catalytic Engineering Research Center of the Ministry of Education, State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, PR China.
Advanced Catalytic Engineering Research Center of the Ministry of Education, State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, PR China.
J Colloid Interface Sci. 2025 Feb 15;680(Pt A):578-586. doi: 10.1016/j.jcis.2024.10.192. Epub 2024 Nov 1.
Electrocatalytic CH amination of hydrocarbons is a promising avenue for the synthesis of high-value CN compounds. However, efficient activation of CH bonds remains a significant challenge in electrocatalytic CN coupling. Herein, we present a novel strategy to enhance the electrocatalytic conversion of toluene to N-benzylacetamide through a Ritter-type reaction by engineering a hydrophobic electrode-electrolyte interface using polytetrafluoroethylene (PTFE)-coated carbon paper (CP). The hydrophobic CP-based electrode exhibited a superior N-benzylacetamide productivity of 1860.9 mmol mh and a substantially higher Faradaic efficiency (FE) of 70.1 % compared to pure CP (41.5 %). Experimental results and density functional theory (DFT) calculations reveal that the PTFE coating promotes toluene adsorption and efficiently lowers the energy barrier for toluene dehydrogenation. Additionally, the hydrophobic interface effectively hinders water adsorption on the electrode, suppressing the competitive water oxidation reaction. This study underscores the crucial role of interfacial engineering in optimizing electrocatalytic CN coupling reactions for the sustainable synthesis of high-value amide compounds.
碳氢化合物的电催化CH胺化是合成高价值含氰化合物的一条有前景的途径。然而，在电催化碳氮偶联反应中，CH键的有效活化仍然是一个重大挑战。在此，我们提出了一种新策略，通过使用聚四氟乙烯（PTFE）涂层碳纸（CP）构建疏水电极-电解质界面，通过 Ritter 型反应提高甲苯电催化转化为N-苄基乙酰胺的效率。与纯CP（41.5%）相比，基于疏水CP的电极表现出优异的N-苄基乙酰胺产率，为1860.9 mmol m h，法拉第效率（FE）显著更高，为70.1%。实验结果和密度泛函理论（DFT）计算表明，PTFE涂层促进了甲苯吸附，并有效降低了甲苯脱氢的能垒。此外，疏水界面有效阻碍了电极上的水吸附，抑制了竞争性的水氧化反应。这项研究强调了界面工程在优化电催化碳氮偶联反应以可持续合成高价值酰胺化合物中的关键作用。
