题目: | Abiotic Formation of an Amide Bond via Surface-Supported Direct Carboxyl-Amine Coupling |
作者: | Biao Yang, 1,2,#,* Kaifeng Niu,1,3,# Felix Haag,2 Nan Cao,1,2 Junjie Zhang,1 Haiming Zhang,1 Qing Li,1 Francesco Allegretti,2 Jonas Björk,3 Johannes V. Barth,2,* Lifeng Chi 1,4,* |
单位: | 1 Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials &devices, Soochow University, 215123 Suzhou, P. R. China 2 Physics Department E20, Technical University of Munich, D-85748 Garching, Germany 3 Department of Physics, Chemistry and Biology, IFM, Linköping University, 58183 Linköping, Sweden 4 Institute for Advanced Study (TUM-IAS), Technical University of Munich, D-85748 Garching, Germany |
摘要: | Amide bond formation is one of the most important reactions in biochemistry, notably being of crucial importance for the origin of life. Herein, we combine scanning tunneling microscopy and X-ray photoelectron spectroscopy studies to provide evidence for thermally activated abiotic formation of amide bonds between adsorbed precursors through direct carboxyl-amine coupling under ultrahigh vacuum conditions by means of on-surface synthesis. Complementary insights from temperature- programmed desorption measurements and density functional theory calculations reveal the competition between cross-coupling amide formation and decarboxylation reactions on the Au(111) surface. Furthermore, we demonstrate the critical influence of the employed metal support: whereas on Au(111) the coupling readily occurs, different reaction scenarios prevail on Ag(111) and Cu(111). The systematic experiments signal that archetypical bio-related molecules can be abiotically synthesized in clean environments without water or oxygen. |
影响因子: | 12.959 |
分区情况: | 一区 |
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