Bifunctional CuNi-x nano-alloys for electrocatalytic nitrate reduction and HPAM oxidation coupling reactions†

IF 6 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Lijie Qi, Yu Fu, Borui Ji, Bauyrzhan Sarsenbekuly, Wanli Kang, Hongbin Yang and Shujun Liu
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引用次数: 0

Abstract

Electrochemical synthesis of ammonia (NH3) through cathodic nitrate reduction presents an effective alternative to the Haber–Bosch process, enabling efficient ammonia production without significant environmental pollution. The electrocatalytic degradation strategy is an efficient and environmentally friendly tool for the treatment of oily wastewater containing partially hydrolized polyacrylamide (HPAM). Thus, coupling cathodic nitrate reduction with anodic HPAM oxidation can further enhance ammonia synthesis efficiency and HPAM degradation efficiency. Here, we reported an N-doped carbon nanotube loaded with CuNi-x (x = 0.5, 1, 2) as an electrocatalyst for cathodic nitrate reduction coupled with anodic HPAM oxidative degradation. Notably, the CuNi-1 variant achieved the highest ammonia yield of 4962.76 ± 40.22 μg h−1 mgcat−1 and a faradaic efficiency of 85.91 ± 0.42%. Furthermore, the oxidative degradation rate of HPAM reached a maximum of 81.91 ± 0.36% within 2 h. Anodic HPAM oxidation not only promotes cathodic nitrate reduction but also enables the acquisition of valuable anodic products. Using in situ ATR-SEIRAS, in situ DEMS, and DFT calculations, we thoroughly analyzed reaction intermediates and the critical role of the CuNi bimetallic system in electrocatalytic nitrate reduction. The coupled reaction system was established to achieve both efficient ammonia synthesis and HPAM degradation.

Abstract Image

用于电催化硝酸还原和HPAM氧化偶联反应的双功能cu -x纳米合金
通过阴极硝酸盐还原电化学合成氨(NH3)是Haber-Bosch工艺的有效替代方法,可以在不造成严重环境污染的情况下高效生产氨。电催化降解是处理含部分水解聚丙烯酰胺(HPAM)含油废水的一种高效、环保的方法。因此,将阴极硝酸还原与阳极HPAM氧化耦合可以进一步提高氨合成效率和HPAM降解效率。在这里,我们报道了一种负载cu -x (x = 0.5, 1,2)的n掺杂碳纳米管作为阴极硝酸盐还原和阳极HPAM氧化降解的电催化剂。值得注意的是,cu -1突变体的氨收率最高,为4962.76±40.22 μg h−1 mgcat−1,法拉第效率为85.91±0.42%。在2 h内,HPAM的氧化降解率达到最大值81.91±0.36%。HPAM的阳极氧化不仅促进了硝酸盐的阴极还原,而且可以获得有价值的阳极产物。利用原位ATR-SEIRAS、原位DEMS和DFT计算,我们深入分析了反应中间体和CuNi双金属体系在电催化硝酸还原中的关键作用。建立了高效合成氨和降解HPAM的耦合反应体系。
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来源期刊
Materials Chemistry Frontiers
Materials Chemistry Frontiers Materials Science-Materials Chemistry
CiteScore
12.00
自引率
2.90%
发文量
313
期刊介绍: Materials Chemistry Frontiers focuses on the synthesis and chemistry of exciting new materials, and the development of improved fabrication techniques. Characterisation and fundamental studies that are of broad appeal are also welcome. This is the ideal home for studies of a significant nature that further the development of organic, inorganic, composite and nano-materials.
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