Unveiling the Activity Origin of Copper-based Electrocatalyst for Selective Nitrate Reduction to Ammonia.

By Yuting Wang, Wei Zhou, Ranran Jia, Yifu Yu, Bin Zhang. Angewandte Chemie, 2020

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Unveiling the active phase of catalytic materials under reaction conditions is important for the designed construction of efficient electrocatalysts for selective nitrate reduction to ammonia. Here, we probed the origin of the prominent activity enhancement for CuO (Faradaic efficiency: 95.8%, Selectivity: 81.2%) toward selective nitrate electroreduction to ammonia. 15 N isotope labeling experiments proved that ammonia originated from nitrate reduction. Both the 1 H nuclear magnetic resonance (NMR) spectra and colorimetric methods were performed to quantify ammonia. In situ Raman and ex situ experiments revealed that CuO was electrochemically converted into Cu/Cu 2 O, which serves as an active phase. The combined results of online differential electrochemical mass spectrometry (DEMS) and density functional theory (DFT) calculations demonstrated that the electron transfer from Cu 2 O to Cu at the interface could facilitate the formation of * NOH intermediate and suppress the hydrogen evolution reaction, leading to high selectivity and Faradaic efficiency.

Subfields: Catalysis, Computer Networks and Communications, Renewable Energy, Sustainability and the Environment

View Paper: https://www.semanticscholar.org/paper/fcb5bca425dc05dc494c1f3a5691841f0cbdcff5

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