用于高电流密度和耐用的一氧化氮到氨电还原的钯铜单原子合金
PdCu Single-Atom Alloys for High-Current-Density and Durable NO-to-NH Electroreduction.
作者信息
Chen Kai, Xiang Jiaqi, Guo Yali, Liu Xijun, Li Xingang, Chu Ke
机构信息
School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou 730070, China.
State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials, School of Resources, School of Resources, Environment and Materials, Guangxi University, Nanning 530004, China.
出版信息
Nano Lett. 2024 Jan 17;24(2):541-548. doi: 10.1021/acs.nanolett.3c02259. Epub 2024 Jan 7.
Electrochemical reduction of NO to NH (NORR) offers a prospective method for efficient NH electrosynthesis. Herein, we first design single-atom Pd-alloyed Cu (PdCu) as an efficient and robust NORR catalyst at industrial-level current densities (>0.2 A cm). Operando spectroscopic characterizations and theoretical computations unveil that Pd strongly electronically couples its adjacent two Cu atoms (PdCu) to enhance the NO activation while promoting the NO-to-NH protonation energetics and suppressing the competitive hydrogen evolution. Consequently, the flow cell assembled with PdCu exhibits an unprecedented NH yield rate of 1341.3 μmol h cm and NH-Faradaic efficiency of 85.5% at an industrial-level current density of 210.3 mA cm, together with an excellent long-term durability for 200 h of electrolysis, representing one of the highest NORR performances on record.
将NO电化学还原为NH₃（NORR）为高效NH₃电合成提供了一种有前景的方法。在此，我们首次设计了单原子钯合金化铜（PdCu）作为一种在工业级电流密度（>0.2 A cm⁻²）下高效且稳定的NORR催化剂。原位光谱表征和理论计算表明，Pd与其相邻的两个Cu原子（PdCu）形成强电子耦合，增强了NO的活化，同时促进了NO到NH₃的质子化能量学，并抑制了竞争性析氢反应。因此，组装有PdCu的流动电池在210.3 mA cm⁻²的工业级电流密度下表现出前所未有的1341.3 μmol h⁻¹ cm⁻²的NH₃产率和85.5%的NH₃法拉第效率，以及长达200 h电解的优异长期耐久性，代表了有记录以来最高的NORR性能之一。
Zotero 插件