Garg Abhishek, Saha Arunava, Dutta Supriti, Pati Swapan K, Eswaramoorthy Muthusamy, Rao Cnr
Chemistry and Physics of Materials Unit, School of Advanced Materials (SAMat), Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR), Jakkur P.O., Bangalore 560064, India.
Theoretical Sciences Unit, School of Advanced Materials, Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR), Bangalore 560064, India.
ACS Appl Mater Interfaces. 2024 Jul 17;16(28):36392-36400. doi: 10.1021/acsami.4c05818. Epub 2024 Jul 4.
The electrochemical reduction of nitrate (NO) ions to ammonia (NH) provides an alternative method to eliminate harmful NO pollutants in water as well as to produce highly valuable NH chemicals. The NH yield rate however is still limited to the μmol h cm range when dealing with dilute NO concentrations found in waste streams. Copper (Cu) has attracted much attention because of its unique ability to effectively convert NO to NH. We have reported a simple and scalable electrochemical method to produce a Cu foil having its surface covered with a porous Cu nanostructure enriched with (100) facets, which efficiently catalyzes NO to NH. The Cu(100)-rich electrocatalyst showed a very high NH production rate of 1.1 mmol h cm in NO concentration as low as 14 mM NO, which is 4-5 times higher than the best-reported values. Increasing the NO concentration (140 mM) resulted in an NH production yield rate of 3.34 mmol h cm. The durability test conducted for this catalyst foil in a flow cell system showed greater than 100 h stability with a Faradaic efficiency greater than 98%, demonstrating its potential to be used on an industrially relevant scale. Further, density functional theory (DFT) calculations have been performed to understand the better catalytic activity of Cu(100) compared to Cu(111) facets toward NORR.
将硝酸根(NO₃⁻)离子电化学还原为氨(NH₃),为消除水中有害的NO₃⁻污染物以及生产高价值的NH₃化学品提供了一种替代方法。然而,在处理废水中稀有的NO₃⁻浓度时,NH₃的产率仍限制在μmol h⁻¹ cm⁻²范围内。铜(Cu)因其能有效将NO₃⁻转化为NH₃的独特能力而备受关注。我们报道了一种简单且可扩展的电化学方法来制备表面覆盖有富含(100)晶面的多孔铜纳米结构的铜箔,该铜箔能有效催化NO₃⁻转化为NH₃。富含Cu(100)的电催化剂在低至14 mM NO₃⁻浓度下显示出1.1 mmol h⁻¹ cm⁻²的极高NH₃产率,这比报道的最佳值高4 - 5倍。将NO₃⁻浓度提高到140 mM时,NH₃产率达到3.34 mmol h⁻¹ cm⁻²。在流动池系统中对该催化剂箔进行的耐久性测试表明,其稳定性超过100小时,法拉第效率大于98%,证明了其在工业相关规模上应用的潜力。此外,还进行了密度泛函理论(DFT)计算,以了解与Cu(111)晶面相比,Cu(1%)对NO₃⁻还原反应(NORR)具有更好催化活性的原因。