Extending Ring‐Chain Coupling Empirical Law to Lithium‐Mediated Electrochemical Ammonia Synthesis

Author:

Li Ya1,Wang Zhenkang2,Ji Haoqing2,Wang Mengfan2,Qian Tao3,Yan Chenglin42ORCID,Lu Jianmei1

Affiliation:

1. Collaborative Innovation Center of Suzhou Nano Science and Technology College of Chemistry Chemical Engineering and Materials Science Soochow University 199 Ren'ai Road Suzhou 215123 P. R. China

2. Key Laboratory of Core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of Energy Soochow University Suzhou Jiangsu 215006 P. R. China

3. College of Chemistry and Chemical Engineering Nantong University Nantong Jiangsu 226019 P. R. China

4. School of Petrochemical Engineering Changzhou University Changzhou 213164 P. R. China

Abstract

AbstractWith its efficient nitrogen fixation kinetics, electrochemical lithium‐mediated nitrogen reduction reaction (LMNRR) holds promise for replacing Haber–Bosch process and realizing sustainable and green ammonia production. However, the general interface problem in lithium electrochemistry seriously impedes the further enhancement of LMNRR performance. Inspired by the development history of lithium battery electrolytes, here, we extend the ring‐chain solvents coupling law to LMNRR system to rationally optimize the interface during the reaction process, achieving nearly a two‐fold Faradaic efficiency up to 54.78±1.60 %. Systematic theoretical simulations and experimental analysis jointly decipher that the anion‐rich Li+ solvation structure derived from ring tetrahydrofuran coupling with chain ether successfully suppresses the excessive passivation of electrolyte decomposition at the reaction interface, thus promoting the mass transfer of active species and enhancing the nitrogen fixation kinetics. This work offers a progressive insight into the electrolyte design of LMNRR system.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Jiangsu Province

Jiangsu Provincial Key Research and Development Program

Natural Science Research of Jiangsu Higher Education Institutions of China

Priority Academic Program Development of Jiangsu Higher Education Institutions

Publisher

Wiley

Subject

General Chemistry,Catalysis

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