Synthesis of amino acids by electrocatalytic reduction of CO2 on chiral Cu surfaces

被引:65
作者
Fang, Yuxi [1 ]
Liu, Xi [2 ,4 ]
Liu, Zhipan [3 ]
Han, Lu [1 ]
Ai, Jing [1 ]
Zhao, Gui [4 ]
Terasaki, Osamu [5 ,6 ]
Cui, Cunhao [7 ]
Yang, Jiuzhong [8 ]
Liu, Chengyuan [8 ]
Zhou, Zhongyue [7 ]
Chen, Liwei [2 ,4 ]
Che, Shunai [1 ,2 ]
机构
[1] Tongji Univ, Sch Chem Sci & Engn, 1239 Siping Rd, Shanghai 200092, Peoples R China
[2] Shanghai Jiao Tong Univ, Frontiers Sci Ctr Transformat Mol, Sch Chem & Chem Engn, State Key Lab Met Matrix Composites,Shanghai Key L, 800 Dongchuan Rd, Shanghai 200240, Peoples R China
[3] Fudan Univ, Collaborat Innovat Ctr Chem Energy Mat, Shanghai Key Lab Mol Catalysis & Innovat Mat, Dept Chem,Key Lab Computat Phys Sci, 2005 Songhu Rd, Shanghai 200438, Peoples R China
[4] Shanghai Jiao Tong Univ, Insitu Ctr Phys Sci, Sch Chem Sci & Engn, 800 Dongchuan Rd, Shanghai 200240, Peoples R China
[5] ShanghaiTech Univ, Ctr High Resolut Electron Microscopy, Shanghai 201210, Peoples R China
[6] ShanghaiTech Univ, Shanghai Key Lab High Resolut Microscopy, Shanghai 201210, Peoples R China
[7] Shanghai Jiao Tong Univ, Sch Mech Engn, 800 Dongchuan Rd, Shanghai 200240, Peoples R China
[8] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, 42 Hezuohua South Rd, Hefei 230029, Anhui, Peoples R China
来源
CHEM | 2023年 / 9卷 / 02期
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
CARBON-DIOXIDE; SELECTIVITY; ADSORPTION; CONVERSION; CATALYSTS;
D O I
10.1016/j.chempr.2022.10.017
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
CO2 reduction and fixation products, ranging from small molecules to biomolecules, are highly diverse in natural systems. Although various multicarbon products of CO2 reduction were artificially obtained, the C3+ products with various functional groups (e.g., C-N and C-O bonds), especially biomolecules, have never been reported. Herein, we synthesized C3+ amino acids via electrocatalytic synthesis from CO2 and NH3, using chiral Cu films (CCFs) as electrodes. Electron mi-croscopy and theoretical calculations suggested that chiral kink sites can possibly be formed on the surface of CCFs fabricated through electrodeposition in the presence of histidine (His). Serine (Ser), with an enantiomeric excess (ee) greater than 90%, is the main component of various amino acids. Experimental and computational data showed that the 3-hydropyruvic acid formation from H2CO- CO* is the stereo-determining step in the Ser formation pathway. The chiral kink sites were speculated to be restricting the configura-tion changes of C3+ intermediates to involve a thermodynamically and kinetically favorable formation of enantiomeric Ser.
引用
收藏
页码:460 / 471
页数:13
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