Efficient Glycine Electrosynthesis via CO<sub>2</sub>‐Recyclable Hydrogen Donation on Pb/Pb<sub>7</sub>Bi<sub>3</sub> Heterointerfaces
Abstract
AbstractElectrochemical synthesis has emerged as a sustainable platform in constructing C─N bonds for amino acid production. Glycine, a particularly valuable target compound, continues to experience escalating global demand, yet achieving simultaneous high efficiency and operational stability remains a persistent challenge. Herein, we demonstrate a CO2‐mediated strategy for glycine electrosynthesis using oxalic acid and N2/nitrate as feedstocks. By using Pb/Pb7Bi3‐CO2 catalytic system, a very high glycine Faradaic efficiency (FE) of 91.8% with durable stability over 120 h could be achieved. Moreover, when using nonthermal plasma‐activated N2 as the nitrogen source, the glycine production rate could maintain at 94.4 µmol h−1 cm−2 with N‐selectivity as high as 93.2%. Mechanistic investigations combining experiments and theoretical calculations reveal that CO2 undergoes facile protonation on the Pb/Pb7Bi3 heterointerfaces to form *OCOH intermediate, which donates hydrogen for the reduction of oxalic acid and nitrate into glyoxylic acid and NH2OH, respectively, while CO2 is simultaneously regenerated. Notably, hydrogenation via the *OCOH intermediate significantly lowers the energy barriers compared to direct protonation, thereby promoting the subsequent spontaneous C─N bond formation and enabling highly efficient electrosynthesis of glycine.
Article Details
Authors (13)
Pengsong Li
Institute of Chemistry, Chinese Academy of Sciences , , ,
Yong Wang
Xiangda Zhang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Re‐search/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry Chinese Academy of Sciences Beijing 100190 P.R. China
Congyang Wang
University of Chinese Academy of Sciences , , ,
Yuqing Hou
Institute of Chemistry, Chinese Academy of Sciences , , ,
Ganwen Zhang
Institute of Chemistry, Chinese Academy of Sciences , , ,
Xihua Wang
Lihong Jing
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Qingli Qian
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Xinchen Kang
Institute of Chemistry, Chinese Academy of Sciences , , ,
Xiaofu Sun
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Qinggong Zhu
Institute of Chemistry, Chinese Academy of Sciences , , ,
Buxing Han
Institute of Chemistry, Chinese Academy of Sciences , , ,