Highly Efficient Electrosynthesis of Glycine over an Atomically Dispersed Iron Catalyst

被引:31
|
作者
Cheng, Yingying [1 ]
Liu, Shiqiang [1 ]
Jiao, Jiapeng [2 ]
Zhou, Meng [1 ]
Wang, Yiyong [1 ,3 ]
Xing, Xueqing [4 ]
Chen, Zhongjun [4 ]
Sun, Xiaofu [1 ,3 ]
Zhu, Qinggong [1 ,3 ]
Qian, Qingli [1 ,3 ]
Wang, Congyang [1 ,3 ]
Liu, Huizhen [1 ,3 ]
Liu, Zhimin [1 ,3 ]
Kang, Xinchen [1 ,3 ]
Han, Buxing [1 ,2 ,3 ]
机构
[1] Chinese Acad Sci, CAS Res Educ Ctr Excellence Mol Sci, Beijing Natl Lab Mol Sci, CAS Lab Colloid & Interface & Thermodynam,Ctr Carb, Beijing 100190, Peoples R China
[2] East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, State Key Lab Petr Mol & Proc Engn, Shanghai 200062, Peoples R China
[3] Univ Chinese Acad Sci, Sch Chem, Beijing 100049, Peoples R China
[4] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China
基金
中国国家自然科学基金; 中国博士后科学基金; 北京市自然科学基金;
关键词
ELECTROCHEMICAL REDUCTION REACTION; OXALIC-ACID; NITRATE REDUCTION; CRYSTAL-STRUCTURE; NITROGEN;
D O I
10.1021/jacs.4c01093
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Glycine is a nonessential amino acid that plays a vital role in various biological activities. However, the conventional synthesis of glycine requires sophisticated procedures or toxic feedstocks. Herein, we report an electrochemical pathway for glycine synthesis via the reductive coupling of oxalic acid and nitrate or nitrogen oxides over atomically dispersed Fe-N-C catalysts. A glycine selectivity of 70.7% is achieved over Fe-N-C-700 at -1.0 V versus RHE. Synergy between the FeN3C structure and pyrrolic nitrogen in Fe-N-C-700 facilitates the reduction of oxalic acid to glyoxylic acid, which is crucial for producing glyoxylic acid oxime and glycine, and the FeN3C structure could reduce the energy barrier of *HOOCCH2NH2 intermediate formation thus accelerating the glyoxylic acid oxime conversion to glycine. This new synthesis approach for value-added chemicals using simple carbon and nitrogen sources could provide sustainable routes for organonitrogen compound production.
引用
收藏
页码:10084 / 10092
页数:9
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