Issue 35, 2021

Rigid two-dimensional indium metal–organic frameworks boosting nitrogen electroreduction at all pH values

Abstract

Based on an ion exchange and dissolution–recrystallization mechanism, rigid indium metal–organic framework (In-MOF) nanosheets have been synthesized under mild conditions. The collective advantages of the rigid structure and two-dimensional architecture (thickness: 1.3 nm) enable In-MOF to show great activity during nitrogen electroreduction and excellent stability over a wide pH range. At pH values <7, In-MOF nanosheets demonstrate an ammonia yield rate ≥ 24.70 μg h−1 mg−1 (or 4.94 μg h−1 cm−2) and faradic efficiency ≥6.72%. At pH values ≥7, 2D In-MOF can operate efficiently with a record NH3 yield of 79.20 μg h−1 mg−1 (or 15.94 μg h−1 cm−2) and faradic efficiency of 14.98%, making it one of the most active MOF-based electrocatalysts for nitrogen electroreduction. Furthermore, the reaction mechanism of nitrogen electroreduction has been revealed using density function theory (DFT) simulations, and it follows enzymatic pathways at all pH values, with the potential determining step being *H2NNH2* → *NH2 + NH3. It is expected that the present study will offer valuable clues for the design and fabrication of low-cost and efficient all-pH nitrogen reduction electrocatalysts for industrial applications.

Graphical abstract: Rigid two-dimensional indium metal–organic frameworks boosting nitrogen electroreduction at all pH values

Supplementary files

Article information

Article type
Paper
Submitted
31 mar 2021
Accepted
23 avq 2021
First published
23 avq 2021

J. Mater. Chem. A, 2021,9, 20040-20047

Rigid two-dimensional indium metal–organic frameworks boosting nitrogen electroreduction at all pH values

Y. Sun, B. Xia, S. Ding, L. Yu, S. Chen and J. Duan, J. Mater. Chem. A, 2021, 9, 20040 DOI: 10.1039/D1TA02684D

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