Analytical Chemistry-Center for Electrochemical Sciences (CES), Faculty of Chemistry and Biochemistry, Ruhr University Bochum, Universitätsstr. 150, 44780, Bochum, Germany.
Inorganic Chemistry, Faculty of Chemistry and Center for Nanointegration Duisburg-Essen (Cenide), University of Duisburg-Essen, Universitätsstr. 7, 45141, Essen, Germany.
Angew Chem Int Ed Engl. 2023 Feb 13;62(8):e202214830. doi: 10.1002/anie.202214830. Epub 2023 Jan 18.
Electrochemically converting nitrate to ammonia is an essential and sustainable approach to restoring the globally perturbed nitrogen cycle. The rational design of catalysts for the nitrate reduction reaction (NO RR) based on a detailed understanding of the reaction mechanism is of high significance. We report a Cu O+Co O tandem catalyst which enhances the NH production rate by ≈2.7-fold compared to Co O and ≈7.5-fold compared with Cu O, respectively, however, most importantly, we precisely place single Cu O and Co O cube-shaped nanoparticles individually and together on carbon nanoelectrodes provide insight into the mechanism of the tandem catalysis. The structural and phase evolution of the individual Cu O+Co O nanocubes during NO RR is unveiled using identical location transmission electron microscopy. Combining single-entity electrochemistry with precise nano-placement sheds light on the dynamic transformation of single catalyst particles during tandem catalysis in a direct way.
电化学将硝酸盐转化为氨是恢复全球受干扰氮循环的一种重要且可持续的方法。基于对反应机制的深入了解，合理设计硝酸盐还原反应（NO RR）的催化剂具有重要意义。我们报告了一种 CuO+CoO 串联催化剂，与 CoO 相比，它将 NH3 的生成速率提高了约 2.7 倍，与 CuO 相比，提高了约 7.5 倍，但最重要的是，我们精确地将单个 CuO 和 CoO 立方纳米颗粒单独和一起放置在碳纳米电极上，深入了解串联催化的机制。使用相同位置的透射电子显微镜揭示了单个 CuO+CoO 纳米立方体在 NO RR 过程中的结构和相演化。将单实体电化学与精确的纳米定位相结合，直接揭示了串联催化过程中单个催化剂颗粒的动态转化。
