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Electrocatalytic Synthesis of Essential Amino Acids from Nitric Oxide Using Atomically Dispersed Fe on N-doped Carbon |
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| Authors: | Jiahui Xian Suisheng Li Hui Su Peisen Liao Shihan Wang Yawei Zhang Wenqian Yang Jun Yang Yamei Sun Yaling Jia Qinglin Liu Prof. Qinghua Liu Prof. Guangqin Li |
| Affiliation: | 1. MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510006 China These authors contributed equally to this work.;2. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029 China Key Laboratory of Light Energy Conversion Materials of Hunan Province College, College of Chemistry and Chemical Engineering, Hunan Normal University, Changsha, 410081 China These authors contributed equally to this work.;3. MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510006 China School of Chemistry and Environment, Jiaying University, Meizhou, 514015 China These authors contributed equally to this work.;4. MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510006 China;5. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029 China |
| Abstract: | 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 α-amino acids from nitric oxide (NO) by reacting with α-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 μmol mgcat−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 α-keto acid to form oxime and subsequent reductive hydrogenation occurred on the way to amino acid. Over 6 kinds of α-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. |
| Keywords: | Amino Acid Synthesis Electrocatalysis Hydroxylamine Metal–Organic Frameworks Nitrogen Oxide |