Selective Mass Accumulation at the Metal–Polymer Bridging Interface for Efficient Nitrate Electroreduction to Ammonia and Zn-Nitrate Batteries

作者：Guojie Chao, Wei Zong, Jiexin Zhu, Haifeng Wang, Kaibin Chu, Hele Guo, Jian Wang, Yuhang Dai, Xuan Gao, Longxiang Liu, Fei Yun Guo, Ivan Paul Parkin, Wei Dong Luo, Paul Robert Shearing, Longsheng Zhang, Guanjie He, Tianxi Liu · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c00400 · 被引用次数：83 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques、Caching and Content Delivery

High Resolution Image Download MS PowerPoint Slide The electrochemical conversion of nitrate (NO 3 – ), a common nitrogen source in industrial wastewater and contaminated groundwater, into ammonia (NH 3 ), signifies an approach to wastewater treatment and NH 3 production. Nevertheless, its selectivity and activity at low NO 3 – 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/Cu 2 O 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 NO 3 – and H 2 O, creating a Janus NO 3 – -rich and H 2 O-poor domain near the catalyst surface. Operando characterizations and theoretical simulations indicate that the metal–polymer bridging interface selectively accumulates NO 3 – and reduces the energy barrier toward the reduction of *NH 2 OH to *NH 2, overcoming the mass transfer limitations at a low NO 3 – concentration. E-CuBDC exhibits a high Faradaic efficiency (FE) of over 90% across wide NO 3 – concentrations (7.1–100 mM NO 3 – ) and high applied voltages. Additionally, it achieved stable NH 3 production over 100 h at ampere-level current densities. When applied in a Zn–NO 3 – system, this newly developed E-CuBDC catalyst demonstrates an outstanding power...