Electrocatalytic Synthesis of Essential Amino Acids from Nitric Oxide Using Atomically Dispersed Fe on N-doped Carbon

被引:84
|
作者
Xian, Jiahui [1 ]
Li, Suisheng [1 ]
Su, Hui [2 ,3 ]
Liao, Peisen [1 ,4 ]
Wang, Shihan [1 ]
Zhang, Yawei [1 ]
Yang, Wenqian [1 ]
Yang, Jun [1 ]
Sun, Yamei [1 ]
Jia, Yaling [1 ]
Liu, Qinglin
Liu, Qinghua [2 ]
Li, Guangqin [1 ]
机构
[1] Sun Yat Sen Univ, Lehn Inst Funct Mat, Sch Chem, MOE Lab Bioinorgan & Synthet Chem, Guangzhou 510006, Peoples R China
[2] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
[3] Hunan Normal Univ, Key Lab Light Energy Convers Mat Hunan Prov Coll, Coll Chem & Chem Engn, Changsha 410081, Peoples R China
[4] Jiaying Univ, Sch Chem & Environm, Meizhou 514015, Peoples R China
关键词
Amino Acid Synthesis; Electrocatalysis; Hydroxylamine; Metal-Organic Frameworks; Nitrogen Oxide; METAL-ORGANIC FRAMEWORKS; EFFICIENT OXYGEN REDUCTION; CONVERSION; CO2;
D O I
10.1002/anie.202304007
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
How to transfer industrial exhaust gases of nitrogen oxides into high-values product is significantly important and challenging. Herein, we demonstrate an innovative method for artificial synthesis of essential alpha-amino acids from nitric oxide (NO) by reacting with alpha-keto acids through electrocatalytic process with atomically dispersed Fe supported on N-doped carbon matrix (AD-Fe/NC) as the catalyst. A yield of valine with 32.1 mu mol mg(cat)(-1) is delivered at -0.6 V vs. reversible hydrogen electrode, corresponding a selectivity of 11.3 %. In situ X-ray absorption fine structure and synchrotron radiation infrared spectroscopy analyses show that NO as nitrogen source converted to hydroxylamine that promptly nucleophilic attacked on the electrophilic carbon center of alpha-keto acid to form oxime and subsequent reductive hydrogenation occurred on the way to amino acid. Over 6 kinds of alpha-amino acids have been successfully synthesized and gaseous nitrogen source can be also replaced by liquid nitrogen source (NO3-). Our findings not only provide a creative method for converting nitrogen oxides into high-valued products, which is of epoch-making significance towards artificial synthesis of amino acids, but also benefit in deploying near-zero-emission technologies for global environmental and economic development.
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页数:9
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