Sn catalyst reconstruction and microenvironment modulation for efficient amino acid electrosynthesis via C–N coupling
Abstract
Abstract The electrosynthesis of amino acids represents a fascinating and promising frontier in green chemistry, offering a sustainable alternative to conventional industrial processes such as the energy-intensive Strecker synthesis through the adoption of efficient, electricity-driven methods. Herein, Sn is identified as an effective catalyst for glycine electrosynthesis using concentrated nitric acid and oxalic acid as feedstocks, and we investigate the reaction mechanism at industrial-level current rate (1 A cm -2 ). In-situ characterization reveals that the Sn undergoes dynamic valence cycle and reconstructs into amorphous-Sn under acidic conditions. At high current, the change in local pH promotes the anionic states of oxalic acid and C-intermediates, which enhances the adsorption of key intermediates such as glyoxalic acid and acid oxime. This switches the mechanism from a chain reaction to an interfacial hydrogenation, thereby increasing the rate of glycine formation. By increasing the dominance of interfacial reaction versus the chain reaction, we achieve a glycine Faradaic efficiency of 93%, and industrial-level partial current density of 0.9 A cm −2 in a flow cell.
Article Details
Authors (14)
Shuhe Han
Institute of Molecular Plus, Department of Chemistry
Huimin Liu
Janis Timoshenko
Department of Interface Science, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, Berlin 14195, Germany
Joonbaek Jang
Department of Interface Science, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, Berlin 14195, Germany
Mengyao Su
Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543, Singapore
Chenghua Sun
Department of Chemistry and Biotechnology, Swinburne University of Technology, Hawthorn, VIC 3122, Australia
Chengying Guo
Institute of Molecular Plus, Department of Chemistry
Yanmei Huang
Arno Bergmann
Beatriz Roldan Cuenya
Department of Interface Science
Yifu Yu
Institute of Molecular Plus, Department of Chemistry
Bin Zhang
Kai Leng
Department of Applied Physics
Kian Ping Loh
Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543, Singapore