期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 11, 期 30, 页码 16068-16073出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d3ta03467d
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In this study, pyridine-functionalized silver nanosheets were successfully synthesized as an electrocatalyst for nitrate electroreduction reaction (NO3RR), showing higher activity compared to pure silver catalysts. The modulation of electronic structures using a chemical functionalization strategy provides valuable insights for the rational design of noble metal-based electrocatalysts.
The nitrate electroreduction reaction (NO3RR) serves as an environmentally friendly method for ammonia (NH3) synthesis and effectively mitigates nitrate pollution in natural water bodies. The chemical functionalization of noble metal nanostructures can effectively enhance their activity and selectivity in electrocatalytic reactions. In this study, we successfully synthesized pyridine (Py) functionalized silver (Ag) nanosheets (Py-Ag NSs) as an electrocatalyst for NO3RR. Density functional theory calculation results revealed that the adsorbed pyridine modulated the electronic structure of Ag atoms, thereby facilitating the adsorption of nitrate ions and the following reduction steps. Consequently, Py-Ag NSs revealed significantly improved activity for NO3RR compared to pure Ag catalysts. Notably, at a potential of -0.53 V, Py-Ag NSs exhibited a faradaic efficiency and production rate of NH3 reaching 96.6% and 72.664 mg h(-1) mg(cat)(-1), respectively. This work provides valuable insights into the modulation of electronic structures using a chemical functionalization strategy, thus guiding the rational design of noble metal-based electrocatalysts.
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