Selective mass accumulation at the metal-polymer bridging interface for efficient nitrate electroreduction to ammonia and Zn-nitrate batteries

Chao, G; Zong, W; Zhu, J; Wang, H; Chu, K; Guo, H; Wang, J; Dai, Y; Gao, X; Liu, L; Guo, F; Parkin, IP; Luo, W; Shearing, PR; Zhang, L; He, G; Liu, T

Journal article

Selective mass accumulation at the metal-polymer bridging interface for efficient nitrate electroreduction to ammonia and Zn-nitrate batteries

Abstract:: The electrochemical conversion of nitrate (NO₃^–), a common nitrogen source in industrial wastewater and contaminated groundwater, into ammonia (NH₃), signifies an approach to wastewater treatment and NH₃ production. Nevertheless, its selectivity and activity at low NO₃^– concentrations and industrial current densities are constrained by limited mass transfer around the electrode. Here, we report a metal–polymer bridging interface constructed by anchoring Cu/Cu₂O nanoparticles onto a two-dimensional (2D) Cu-based benzene dicarboxylate (CuBDC) coordination polymer via in situ electroreduction (denoted as E-CuBDC). This interface weakens the electrostatic repulsion and regulates the distribution/migration of NO₃^– and H₂O, creating a Janus NO₃^–-rich and H₂O-poor domain near the catalyst surface. Operando characterizations and theoretical simulations indicate that the metal–polymer bridging interface selectively accumulates NO₃^– and reduces the energy barrier toward the reduction of *NH₂OH to *NH₂, overcoming the mass transfer limitations at a low NO₃^– concentration. E-CuBDC exhibits a high Faradaic efficiency (FE) of over 90% across wide NO₃^– concentrations (7.1–100 mM NO₃^–) and high applied voltages. Additionally, it achieved stable NH₃ production over 100 h at ampere-level current densities. When applied in a Zn–NO₃^– system, this newly developed E-CuBDC catalyst demonstrates an outstanding power density and FE for NH₃ production, showcasing its great potential for large-scale electrochemical conversion and storage systems. This study presents a generalizable strategy for constructing metal–polymer interfaces to regulate interfacial mass transport.

Publication status:: Published

Peer review status:: Peer reviewed

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APA Style

Chao, G., Zong, W., Zhu, J., Wang, H., Chu, K., Guo, H., Wang, J., Dai, Y., Gao, X., Liu, L., Guo, F., Parkin, I. P., Luo, W., Shearing, P. R., Zhang, L., He, G., & Liu, T. (2025). Selective mass accumulation at the metal-polymer bridging interface for efficient nitrate electroreduction to ammonia and Zn-nitrate batteries. Journal of the American Chemical Society, 147(25), 21432–21442.

MLA Style

Chao, G, et al. “Selective Mass Accumulation at the Metal-Polymer Bridging Interface for Efficient Nitrate Electroreduction to Ammonia and Zn-Nitrate Batteries.” Journal of the American Chemical Society, vol. 147, no. 25, 2025, pp. 21432–42.

Chicago Style

Chao, G, W Zong, J Zhu, et al. 2025. “Selective Mass Accumulation at the Metal-Polymer Bridging Interface for Efficient Nitrate Electroreduction to Ammonia and Zn-Nitrate Batteries.” Journal of the American Chemical Society 147 (25): 21432–42.
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