journal article·2026-02-17

Boosting Electrocatalytic Ammonia Synthesis via Main-Group Metal Doping and Ionic Liquid Encapsulation in Copper Metal–Organic Frameworks

Bo Han, Jie Ding, Man-Fai Ng, Chengyi Liu, Chu Zhang, Cailing Chen, Nan Zhang, Yue Hu, Jing Yan, Beier Jia, Erhai Hu, Mengxin Chen, Zhangliu Tian, Yu Han, Shibo Xi, Chade Lv, Qiang Zhu, Madhavi Srinivasan, Bin Liu, Qingyu Yan

ACS Nano· Volume 20· Issue 6
Publisher page

Abstract

The electrochemical nitrogen reduction reaction (EN 2 RR) provides a sustainable method for synthesizing ammonia at room temperature, but it is hindered by the low ammonia faradic efficiency (FE) and production yield. Herein, we report an effective EN 2 RR electrocatalyst: the ionic liquid-encapsulated aluminum copper bimetallic metal–organic framework (IL-AlCu-MOF). Comparisons across pristine Cu-MOF, AlCu-MOF, IL-Cu-MOF, and IL-AlCu-MOF reveal that the combination of Al doping and IL encapsulation can simultaneously promote dinitrogen activation and accelerate proton generation via water dissociation in a neutral electrolyte, which synergistically enhances the yield and selectivity of ammonia in EN 2 RR. The IL-AlCu-MOF achieves an NH 3 yield of 124.7 μg·h –1 ·mg cat –1 with an FE NH 3 of 20.3% at −0.3 V (vs reversible hydrogen electrode, RHE) in 0.1 M K 2 SO 4 . In situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) measurements indicate improved water dissociation kinetics over that of IL-AlCu-MOF, and differential electrochemical mass spectrometry (DEMS) captures the EN 2 RR intermediates. Density functional theory (DFT) calculations show that Al doping modulates the Cu electronic structure for enhanced N 2 activation, while IL encapsulation strengthens water adsorption at the MOF surface and thus accelerates water dissociation, both of which contribute to boosting the EN 2 RR performance.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · CO2 Reduction Techniques and Catalysts · Advanced Photocatalysis Techniques

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Energy Research Institute@NTU (ERI@N)

Nanyang Technological University

Department of Materials Science and Engineering, Department of Chemistry, Hong Kong Institute for Clean Energy (HKICE) & Center for Super-Diamond and Advanced Films (COSDAF)

City University of Hong Kong

Institute of High-Performance Computing (IHPC)

Agency for Science, Technology and Research (A*STAR)

Institute of Sustainability for Chemicals, Energy and Environment (ISCE)

MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering

Harbin Institute of Technology

Physical Sciences and Engineering Division, Advanced Membranes and Porous Materials (AMPM) Center

King Abdullah University of Science and Technology (KAUST)

State Key Laboratory of Applied Organic Chemistry, Frontiers Science Center for Rare Isotopes, College of Chemistry and Chemical Engineering

Lanzhou University

School of Materials Science and Engineering

International Collaboration Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics

Shenzhen University

IMRE (Institute of Materials Research and Engineering)

Funding

Ministry of Education - Singapore · Innovation and Technology Fund · City University of Hong Kong · JC STEM lab of Advanced CO2 Upcycling

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