Department of Chemistry, Institute of Molecular Plus, School of Science, Tianjin University, Tianjin, 300072, China.
Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Frontiers Science Center for Synthetic Biology, (Ministry of Education), Tianjin University, Tianjin, 300072, China.
Angew Chem Int Ed Engl. 2021 Feb 23;60(9):4474-4478. doi: 10.1002/anie.202014017. Epub 2021 Jan 7.
Nitrate is one of the essential raw ingredients in agriculture and industry. The electrochemical nitrogen oxidation reaction (NOR) is promising to replace the conventional nitrate synthesis industry with high energy consumption and greenhouse gas emission. Here, tensile-strained palladium porous nanosheets (Pd-s PNSs) were prepared. They exhibited enhanced activity for electrochemical NOR at ambient conditions, greatly outperforming Pd nanosheets. N isotope labeling experiments proved that nitrate originated from nitrogen oxidation. Combining electrochemical in situ Raman and FTIR spectroscopy with density functional calculations, it was revealed that the tensile strain could facilitate the formation of NOR active species of PdO , leading to high activity.
硝酸盐是农业和工业中必不可少的原材料之一。电化学氮氧化反应（NOR）有望取代传统的高能耗和温室气体排放的硝酸盐合成工业。在此，制备了拉伸应变钯多孔纳米片（Pd-s PNSs）。它们在环境条件下表现出增强的电化学 NOR 活性，大大优于钯纳米片。N 同位素标记实验证明硝酸盐来源于氮氧化。结合电化学原位拉曼和傅里叶变换红外光谱以及密度泛函计算，表明拉伸应变可以促进 NOR 活性物种 PdO 的形成，从而导致高活性。
