材料科学
氨
纳米颗粒
硝酸
一氧化氮
无机化学
相(物质)
氧化物
相变
过渡金属
催化作用
纳米技术
冶金
有机化学
化学
凝聚态物理
物理
作者
Sheng Wang,Guilan Fan,Deyan Luan,Yan Guo,Xiaojun Gu,Xiong Wen Lou
标识
DOI:10.1002/adma.202408580
摘要
Abstract Electrocatalytic reduction of nitric oxide (NO) to ammonia (NH 3 ) represents a potential solution for improving the disrupted nitrogen cycle balance. Unfortunately, designing efficient electrocatalysts for NO reduction reaction (NORR) remains a notable challenge, especially at low concentrations. Herein, a displacement‐alloying strategy is reported to successfully induce the phase transition of Co nanoparticles supported on carbon nanosheets from face‐centered cubic (fcc) to hexagonal close‐packed (hcp) structure through Ru incorporation. The obtained RuCo alloy with hcp phase structure (hcp‐RuCo) exhibits apparent NORR activity with a record‐high Faraday efficiency of 99.2% and an NH 3 yield of 77.76 µg h −1 mg cat −1 at −0.1 V versus reversible hydrogen electrode at a NO concentration of 1 vol %, surpassing Co nanoparticles with fcc phase structure and most reported catalysts. Density functional theory calculations reveal that the excellent NORR activity of hcp‐RuCo can be attributed to the optimized electronic structure of Co site and lowered energy barrier of the potential rate‐determining step through phase transition. Furthermore, the assembled Zn‐NO battery using hcp‐RuCo as the cathode achieves a power density of 2.33 mW cm −2 and an NH 3 yield of 45.94 µg h −1 mg cat −1 . This work provides a promising research perspective for low‐concentration NO conversion.
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