Molecular Engineering of a Metal-Organic Polymer for Enhanced Electrochemical Nitrate-to-Ammonia Conversion and Zinc Nitrate Batteries

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

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Detail(s)

Original languageEnglish
Article numbere202309930
Journal / PublicationAngewandte Chemie - International Edition
Volume62
Issue number48
Online published12 Oct 2023
Publication statusPublished - 2023

Abstract

Metal–organic framework-based materials are promising single-site catalysts for electrocatalytic nitrate (NO3) reduction to value-added ammonia (NH3) on account of well-defined structures and functional tunability but still lack a molecular-level understanding for designing the high-efficient catalysts. Here, we proposed a molecular engineering strategy to enhance electrochemical NO3-to-NH3 conversion by introducing the carbonyl groups into 1,2,4,5-tetraaminobenzene (BTA) based metal-organic polymer to precisely modulate the electronic state of metal centers. Due to the electron-withdrawing properties of the carbonyl group, metal centers can be converted to an electron-deficient state, fascinating the NO3 adsorption and promoting continuous hydrogenation reactions to produce NH3. Compared to CuBTA with a low NO3-to-NH3 conversion efficiency of 85.1 %, quinone group functionalization endows the resulting copper tetraminobenzoquinone (CuTABQ) distinguished performance with a much higher NH3 FE of 97.7 %. This molecular engineering strategy is also universal, as verified by the improved NO3-to-NH3 conversion performance on different metal centers, including Co and Ni. Furthermore, the assembled rechargeable Zn−NO3 battery based on CuTABQ cathode can deliver a high power density of 12.3 mW cm−2. This work provides advanced insights into the rational design of metal complex catalysts through the molecular-level regulation for NO3 electroreduction to value-added NH3. © 2023 Wiley-VCH GmbH.

Research Area(s)

  • Metal–Organic Framework, NH3 Synthesis, NO3− Reduction, Zinc Batteries

Citation Format(s)

Molecular Engineering of a Metal-Organic Polymer for Enhanced Electrochemical Nitrate-to-Ammonia Conversion and Zinc Nitrate Batteries. / Zhang, Rong; Hong, Hu; Liu, Xinghui et al.
In: Angewandte Chemie - International Edition, Vol. 62, No. 48, e202309930, 2023.

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review