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氨电化学合成的动力学和氘同位素分析

Kinetic and deuterium isotope analyses of ammonia electrochemical synthesis.

作者信息

Li Chien-I, Matsuo Hiroki, Otomo Junichiro

机构信息

Department of Environment Systems, Graduate School of Frontier Sciences, The University of Tokyo 5-1-5 Kashiwanoha, Kashiwa-shi Chiba 277-8563 Japan.

Department of Transdisciplinary Science and Engineering, School of Environment and Society, Tokyo Institute of Technology 2-12-1 Ookayama, Meguro-ku Tokyo 152-8550 Japan

出版信息

RSC Adv. 2021 May 19;11(29):17891-17900. doi: 10.1039/d1ra00190f. eCollection 2021 May 13.

DOI:10.1039/d1ra00190f
PMID:35480192
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9033204/
Abstract

The mechanism of electrochemical promotion of ammonia formation was investigated by kinetic and deuterium isotope analyses using a cell with a Pt (anode)|BaCeYO (BCY)|Fe (cathode) configuration on the introduction of a gaseous mixture of H(D)-N to the cathode at 550 °C. To clarify the mechanism of electrochemical ammonia synthesis, the reaction orders for hydrogen, , and nitrogen, , were investigated. The values of and did not change after applying a negative voltage, which indicates that the reaction mechanism at rest potential is the same as that with cathodic polarization. Furthermore, deuterium isotope analysis was conducted to investigate the mechanism of electrochemical promotion. The isotopic composition of ammonia (, NH D ) formed in the cathode was determined using Fourier-transform infrared spectroscopy (FTIR). The results show that the ammonia products with cathodic polarization correspond to the species of H (or D) in the cathode, that is, NH (or ND) was mainly formed when H (or D) was introduced to the cathode. Isotopic analysis revealed that the ammonia formation rate the electrochemical promotion of catalysis (EPOC) is faster than that the charge-transfer reaction, suggesting that a significant increase in the ammonia formation rate will be caused by the EPOC.

摘要

在550℃下，将H(D)-N气态混合物引入阴极，使用具有Pt(阳极)|BaCeYO(BCY)|Fe(阴极)结构的电池，通过动力学和氘同位素分析研究了电化学促进氨生成的机制。为了阐明电化学合成氨的机制，研究了氢气、 和氮气、 的反应级数。施加负电压后， 和 的值没有变化，这表明静止电位下的反应机制与阴极极化时相同。此外，进行了氘同位素分析以研究电化学促进的机制。使用傅里叶变换红外光谱(FTIR)测定阴极中形成的氨( 、NH D )的同位素组成。结果表明，具有阴极极化的氨产物与阴极中的H(或D)种类相对应，即当H(或D)引入阴极时，主要形成NH(或ND)。同位素分析表明，催化电化学促进(EPOC)的氨生成速率比电荷转移反应的氨生成速率快，这表明EPOC将导致氨生成速率显著增加。

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