High-performance electrocatalytic nitrate reduction into ammonia by chitosan regulated Co nanocatalyst

IF 5.3 2区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Applied Nano Materials Pub Date : 2024-10-09 DOI:10.1039/d4qi02058h

Yaqian Xin, Shengbo Zhang, Jiafang Liu, Yong Jiang, Yunxia Zhang, Guozhong Wang, Haimin Zhang

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Abstract

Electrocatalytic nitrate reduction reaction (NtrRR) offers an attractive alternative to the Haber-Bosh process for ambient ammonia (NH3) production. Herein, chitosan regulated Co nanoparticles (Co-NPs/CC) is designed as an electrocatalyst for achieving highly efficient NtrRR catalysis, which exhibits a high NH3 yield rate of 9181.7 ± 60.9 μg h−1 cm−2 at −1.2 V (vs. RHE) and a high Faradaic efficiency (FE) of 88.7 ± 4.0% at −1.0 V (vs. RHE) in 0.1 M K2SO4 + 0.1 M KNO3 electrolyte under ambient conditions. The Co-NPs/CC also exhibited an outstanding performance with selectivity of 99.5 ± 0.2% for NH3 synthesis. The obtained NH4+ was also qualitatively determined by colorimetric and 1H NMR methods. 15N isotopic labelling identifies that the N atom of formed NH3 originates from nitrate. Taking advantage of in situ attenuated total reflection surface-enhanced infrared adsorption spectroscopy (ATR-SEIRAS) and different electrochemical mass spectrometry (DEMS) measurements, the electrocatalytic NtrRR mechanism was verified. This work presents a novel strategy in designing nano-precious NtrRR electrocatalyst with exposed favorable active sites.

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壳聚糖调控 Co 纳米催化剂的高性能电催化硝酸盐还原成氨

电催化硝酸盐还原反应（NtrRR）为环境氨气（NH3）生产提供了一种极具吸引力的哈伯-波什工艺替代方案。在这里，壳聚糖调节钴纳米粒子（Co-NPs/CC）被设计为一种实现高效硝酸还原反应催化的电催化剂，在环境条件下，在 0.1 M K2SO4 + 0.1 M KNO3 电解质中，其 NH3 产率在 -1.2 V 时达到 9181.7 ± 60.9 μg h-1 cm-2 （相对于 RHE），法拉第效率（FE）在 -1.0 V 时达到 88.7 ± 4.0%（相对于 RHE）。Co-NPs/CC 在合成 NH3 方面的选择性为 99.5 ± 0.2%，同样表现出色。获得的 NH4+ 也通过比色法和 1H NMR 法进行了定性测定。15N 同位素标记确定了所形成的 NH3 的 N 原子来自硝酸盐。利用原位衰减全反射表面增强红外吸附光谱法（ATR-SEIRAS）和不同的电化学质谱法（DEMS）测量，验证了电催化 NtrRR 机制。这项工作提出了一种设计具有暴露有利活性位点的纳米贵金属 NtrRR 电催化剂的新策略。

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来源期刊

ACS Applied Nano Materials Multiple-

CiteScore

8.30

自引率

3.40%

发文量

1601

期刊介绍： ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.