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.
引用
收藏
页数:9
相关论文
共 50 条
  • [31] Synthesis of N-doped and Undoped Carbon Nanotubes on Fe/MgO Catalysts
    Cao Yong
    Jiao Qing-Ze
    Zhao Yun
    ACTA PHYSICO-CHIMICA SINICA, 2009, 25 (11) : 2380 - 2384
  • [32] Peroxydisulfate activation by atomically-dispersed Fe-Nx on N-doped carbon: Mechanism of singlet oxygen evolution for nonradical degradation of aqueous contaminants
    Du, Ningjie
    Liu, Ying
    Li, Qiuju
    Miao, Wei
    Wang, Dandan
    Mao, Shun
    CHEMICAL ENGINEERING JOURNAL, 2021, 413
  • [33] Synthesis and Electrocatalytic Performance of N-Doped Ordered Mesoporous Carbon-Ni Nanocomposite
    Pan Xu-Chen
    Tang Jing
    Xue Hai-Rong
    Guo Hu
    Fan Xiao-Li
    Zhu Ze-Tao
    He Jian-Ping
    CHINESE JOURNAL OF INORGANIC CHEMISTRY, 2015, 31 (02) : 282 - 290
  • [34] Isolated diatomic Zn-Fe in N-doped carbon for electrocatalytic nitrogen reduction to ammonia
    Zhang, Le
    Fan, Guilan
    Xu, Wence
    Yu, Meng
    Wang, Lei
    Yan, Zhenhua
    Cheng, Fangyi
    CHEMICAL COMMUNICATIONS, 2020, 56 (80) : 11957 - 11960
  • [35] Atomically dispersed Ni anchored on polymer-derived mesh-like N-doped carbon nanofibers as an efficient CO2 electrocatalytic reduction catalyst
    Tai Cao
    Rui Lin
    Shoujie Liu
    Weng-Chon Max Cheong
    Zhi Li
    Konglin Wu
    Youqi Zhu
    Xiaolu Wang
    Jian Zhang
    Qiheng Li
    Xiao Liang
    Ninghua Fu
    Chen Chen
    Dingsheng Wang
    Qing Peng
    Yadong Li
    Nano Research, 2022, 15 : 3959 - 3963
  • [36] Atomically dispersed Ni anchored on polymer-derived mesh-like N-doped carbon nanofibers as an efficient CO2 electrocatalytic reduction catalyst
    Cao, Tai
    Lin, Rui
    Liu, Shoujie
    Cheong, Weng-Chon
    Li, Zhi
    Wu, Konglin
    Zhu, Youqi
    Wang, Xiaolu
    Zhang, Jian
    Li, Qiheng
    Liang, Xiao
    Fu, Ninghua
    Chen, Chen
    Wang, Dingsheng
    Peng, Qing
    Li, Yadong
    NANO RESEARCH, 2022, 15 (05) : 3959 - 3963
  • [37] Atomically dispersed Zn-NxCy sites on N-doped carbon for catalytic transfer hydrogenation of ethyl levulinate into γ-valerolactone
    Ban, Lijun
    Zhao, Jianghong
    Zhang, Yin
    Huang, Xin
    Chen, Yanyan
    Li, Haitao
    Zhao, Yongxiang
    Liu, Haichao
    CHEMICAL ENGINEERING JOURNAL, 2024, 494
  • [38] Catalytic Hydrogenolysis by Atomically Dispersed Iron Sites Embedded in Chemically and Redox Non-innocent N-Doped Carbon
    Luo, Zhicheng
    Li, Li
    Nguyen, Vy T.
    Kanbur, Uddhav
    Li, Yuting
    Zhang, Jie
    Nie, Renfeng
    Biswas, Abhranil
    Bud'ko, Sergey L.
    Oh, Jinsu
    Zhou, Lin
    Huang, Wenyu
    Sadow, Aaron D.
    Wang, Bin
    Scott, Susannah L.
    Qi, Long
    JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2024, 146 (12) : 8618 - 8629
  • [39] General Synthesis of Hierarchically Macro/Mesoporous Fe,Ni-Doped CoSe/N-Doped Carbon Nanoshells for Enhanced Electrocatalytic Oxygen Evolution
    Wang, Binhang
    Wu, Tianyu
    Chen, Guangrui
    Liu, Xinyao
    Li, Wen
    He, Qingxia
    Li, Dong-Sheng
    Guan, Bu Yuan
    Liu, Yunling
    INORGANIC CHEMISTRY, 2021, 60 (09) : 6782 - 6789
  • [40] Atomically dispersed Mn atoms coordinated with N and O within an N-doped porous carbon framework for boosted oxygen reduction catalysis
    Huo, Juanjuan
    Cao, Xianjun
    Tian, Yaping
    Li, Lu
    Qu, Junpeng
    Xie, Yuhan
    Nie, Xinming
    Zhao, Yufei
    Zhang, Jinqiang
    Liu, Hao
    NANOSCALE, 2023, 15 (11) : 5448 - 5457