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
  • [1] Atomically dispersed Fe atoms anchored on N-doped carbon hollow nanospheres boost the electrocatalytic performance for oxygen reduction reaction
    Liu, Danye
    Chen, Dong
    Yang, Jun
    GREEN ENERGY & ENVIRONMENT, 2019, 4 (03) : 208 - 209
  • [2] Atomically dispersed Fe atoms anchored on N-doped carbon hollow nanospheres boost the electrocatalytic performance for oxygen reduction reaction
    Danye Liu
    Dong Chen
    Jun Yang
    GreenEnergy&Environment, 2019, 4 (03) : 208 - 209
  • [3] Atomically Dispersed Copper on N-Doped Carbon Nanosheets for Electrocatalytic Synthesis of Carbamates from CO2 as a C1 Source
    Li, Shi-Ming
    Shi, Yi
    Zhang, Jing-Jie
    Wang, Ying
    Wang, Huan
    Lu, Jia-Xing
    CHEMSUSCHEM, 2021, 14 (09) : 2050 - 2055
  • [4] Electrochemical Nitrate Production via Nitrogen Oxidation with Atomically Dispersed Fe on N-Doped Carbon Nanosheets
    Guo, Ying
    Zhang, Shaoce
    Zhang, Rong
    Wang, Donghong
    Zhu, Daming
    Wang, Xuewan
    Xiao, Diwen
    Li, Na
    Zhao, Yuwei
    Huang, Zhaodong
    Xu, Wenjie
    Chen, Shuangming
    Song, Li
    Fan, Jun
    Chen, Qing
    Zhi, Chunyi
    ACS NANO, 2022, 16 (01) : 655 - 663
  • [5] Atomically dispersed antimony on N-doped carbon for highly efficient oxygen reduction reaction
    Zhang, Dan
    Xie, Xing
    Sun, Panpan
    Wei, Yongan
    Gong, Tao
    Huang, Niu
    Lv, Xiaowei
    Fang, Liang
    Sun, Xiaohua
    CHEMICAL ENGINEERING JOURNAL, 2022, 439
  • [6] Atomically Dispersed Co on N-Doped Porous Carbon for the Highly Efficient Catalytic Oxidation of Aromatic Alcohols to Acids and Nitriles
    Li, Boyang
    Kou, Jinfang
    Zeng, Gong
    Ma, Jiantai
    Dong, Zhengping
    ACS CATALYSIS, 2023, 13 (24) : 16286 - 16299
  • [7] Atomic Fe Dispersed on N-Doped Carbon Hollow Nanospheres for High-Efficiency Electrocatalytic Oxygen Reduction
    Chen, Yifan
    Li, Zhijuan
    Zhu, Yanbo
    Sun, Dongmei
    Liu, Xien
    Xu, Lin
    Tang, Yawen
    ADVANCED MATERIALS, 2019, 31 (08)
  • [8] MOF-derived N-doped porous carbon anchoring atomically-dispersed Fe for electrochemical sensing of paracetamol
    Zhang, Xue
    Kang, Shihan
    Cheng, Wangxing
    Wang, Lei
    Lu, Nannan
    Chen, Lin-Wei
    MICROCHEMICAL JOURNAL, 2025, 212
  • [9] Coupling Atomically Dispersed Fe-N5 Sites with Defective N-Doped Carbon Boosts CO2 Electroreduction
    Li, Zhao
    Jiang, Jinxia
    Liu, Ximeng
    Zhu, Zhaozhao
    Wang, Junjie
    He, Qian
    Kong, Qingquan
    Niu, Xiaobin
    Chen, Jun Song
    Wang, John
    Wu, Rui
    SMALL, 2022, 18 (38)
  • [10] Atomically Dispersed Fe-N5 Sites Anchored in Porous N-Doped Carbon Nanofibers for Effective Hydrogen Evolution Reaction
    Li, Mengnan
    Yu, Jing
    Liu, Qi
    Liu, Jingyuan
    Chen, Rongrong
    Zhu, Jiahui
    Li, Rumin
    Wang, Jun
    ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2022, 10 (40) : 13505 - 13513