Industrial‐current Ammonia Synthesis by Polarized Cuprous Cyanamide Coupled to Valorization of Glycerol at 4,000 mA cm<sup>−2</sup>

J Jiacheng (Jayden) Wang (State Key Laboratory of High‐Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai 200050 China) H Huong T. D. Bui (Department of Chemistry) H Huashuai Hu (School of Environmental Science and Technology) S Shuyi Kong (State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering) X Xunlu Wang (School of Environmental Science and Technology) H Hongbo Zhu (Institute of Genetics and Crop Breeding, Fujian Agriculture and Forestry University) J Junqing Ma (Shanghai Institute of Ceramics, Chinese Academy of Sciences) J Jintao Xu (School of Physics, Central South University 1 , Changsha 410083,) Y Yihong Liu L Lijia Liu (Department of Chemistry, Western University, 1151 Richmond Street, London, ON N6A5B7, Canada) W Wei Chen H Hui Bi (Shanghai Institute of Ceramics, Chinese Academy of Sciences) M Minghui Yang (School of Environmental Science and Technology) F Fuqiang Huang (Key Laboratory of Intelligent Creation for Extreme Energy Materials of Ministry of Education, School of Materials Science and Engineering and Zhang Jiang Institute for Advanced Study) T Tore Brinck (Department of Chemistry, CBH) J Jiacheng Wang (Zhejiang Key Laboratory for Island Green Energy and New Materials, Institute of Electrochemistry, School of Materials Science and Engineering)

Abstract

AbstractThe electrocatalytic nitrate reduction (NO3RR) holds significance in both NH3 synthesis and nitrate contamination remediation. However, achieving industrial‐scale current and high stability in membrane electrode assembly (MEA) electrolyzer remains challenging due to inherent high full‐cell voltage for sluggish NO3RR and water oxidation. Here, Cu2NCN with positive surface electrostatic potential VS(r) is applied as highly efficient NO3RR electrocatalysts to achieve industrial‐current and low‐voltage stable NH3 production in MEA electrolyzer with coupled anodic glycerol oxidation. This paired electro‐refinery (PER) system reaches 4000 mA cm−2 at 2.52 V and remains stable at industrial‐level 1000 mA cm−2 for 100 h with the NH3 production rate of 97000 µgNH3 h−1 cm−2 and a Faradaic efficiency of 83%. Theoretical calculations elucidate that the asymmetric and electron‐withdrawing [N−C≡N] units enhance polarization and VS(r), promoting robust and asymmetric adsorption of NO3* on Cu2NCN to facilitate O−N bond dissociation. A comprehensive techno‐economic analysis demonstrates the profitability and commercial viability of this coupled system. Our work opens a new avenue and marks a significant advancement in MEA systems for industrial NH3 synthesis.

Article Details

Volume / Issue Vol. 37, Issue 14
Published April 01, 2025
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (16)

J

Jiacheng (Jayden) Wang

State Key Laboratory of High‐Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai 200050 China

H

Huong T. D. Bui

Department of Chemistry

H

Huashuai Hu

School of Environmental Science and Technology

S

Shuyi Kong

State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering

X

Xunlu Wang

School of Environmental Science and Technology

H

Hongbo Zhu

Institute of Genetics and Crop Breeding, Fujian Agriculture and Forestry University

J

Junqing Ma

Shanghai Institute of Ceramics, Chinese Academy of Sciences

J

Jintao Xu

School of Physics, Central South University 1 , Changsha 410083,

Y

Yihong Liu

L

Lijia Liu

Department of Chemistry, Western University, 1151 Richmond Street, London, ON N6A5B7, Canada

W

Wei Chen

H

Hui Bi

Shanghai Institute of Ceramics, Chinese Academy of Sciences

M

Minghui Yang

School of Environmental Science and Technology

F

Fuqiang Huang

Key Laboratory of Intelligent Creation for Extreme Energy Materials of Ministry of Education, School of Materials Science and Engineering and Zhang Jiang Institute for Advanced Study

T

Tore Brinck

Department of Chemistry, CBH

J

Jiacheng Wang

Zhejiang Key Laboratory for Island Green Energy and New Materials, Institute of Electrochemistry, School of Materials Science and Engineering