双金属片
选择性
钯
催化作用
纳米线
化学
纳米材料
无机化学
化学工程
材料科学
纳米技术
有机化学
工程类
作者
Changhui Fu,Shaoxian Song,Lin Hu,Zixun Liu,Zhouyang Yin,Xiaoshu Lv,Sen Zhang,Guangming Jiang
标识
DOI:10.1016/j.cej.2022.134969
摘要
Selective electrocatalytic nitrate reduction reaction (NO3RR) to dinitrogen (N2) is essential to nitrogen-cycle management and environmental sustainability. Palladium-based nanomaterials were extensively studied as NO3RR catalysts, but only delivered limited N2 selectivity (<50%, NH3 dominated the product). Here we report that, by tuning bimetallic composition of CuPd alloy nanowires, the Cu28Pd72 nanowires deliver a near-unit conversion of NO3–-N and an unprecedented N2 product selectivity of 75.9 ± 5.2% in treating 22.5 mg L−1 NO3–-N solution at −0.80 V vs. Ag/AgCl. Combining in-situ spectrometric measurements and theoretical calculations, we demonstrate that the contiguous Pd ensemble with a specific size at catalyst surface is essential to the N2 formation via a kinetically-favored pathway of NO2* → NO* → N* → N2*. Alloying Pd with Cu is indispensable as Cu contributes to the N*-N* pairing by initiating the NO3––NO2* conversion and lowering the Hads coverage on catalyst. This work discloses the key surface atomic structure for N2 formation, and provides a guideline for the design of efficient NO3RR catalyst that enables selective NO3––N2 conversion.
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