Ye Minghao, Jiang Xiaoli, Zhang Yagang, Liu Yang, Liu Yanxia, Zhao Lin
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, China.
State Key Laboratory of Electronic Thin Films and Integrated Devices, University of Electronic Science and Technology of China, Chengdu 611731, China.
Nanomaterials (Basel). 2024 Jan 1;14(1):102. doi: 10.3390/nano14010102.
Ammonia (NH) is vital in modern agriculture and industry as a potential energy carrier. The electrocatalytic reduction of nitrate (NO) to ammonia under ambient conditions offers a sustainable alternative to the energy-intensive Haber-Bosch process. However, achieving high selectivity in this conversion poses significant challenges due to the multi-step electron and proton transfer processes and the low proton adsorption capacity of transition metal electrocatalysts. Herein, we introduce a novel approach by employing functionalized multi-walled carbon nanotubes (MWCNTs) as carriers for active cobalt catalysts. The exceptional conductivity of MWCNTs significantly reduces charge transfer resistance. Their unique hollow structure increases the electrochemical active surface area of the electrocatalyst. Additionally, the one-dimensional hollow tube structure and graphite-like layers within MWCNTs enhance adsorption properties, thus mitigating the diffusion of intermediate and stabilizing active cobalt species during nitrate reduction reaction (NitRR). Using the MWCNT-supported cobalt catalyst, we achieved a notable NH yield rate of 4.03 mg h cm and a high Faradaic efficiency of 84.72% in 0.1 M KOH with 0.1 M NO. This study demonstrates the potential of MWCNTs as advanced carriers in constructing electrocatalysts for efficient nitrate reduction.
氨（NH₃）作为一种潜在的能量载体，在现代农业和工业中至关重要。在环境条件下将硝酸盐（NO₃⁻）电催化还原为氨，为能源密集型的哈伯-博施法提供了一种可持续的替代方法。然而，由于多步电子和质子转移过程以及过渡金属电催化剂的低质子吸附能力，在这种转化中实现高选择性面临重大挑战。在此，我们引入了一种新方法，即使用功能化多壁碳纳米管（MWCNTs）作为活性钴催化剂的载体。MWCNTs的优异导电性显著降低了电荷转移电阻。其独特的中空结构增加了电催化剂的电化学活性表面积。此外，MWCNTs内的一维中空管结构和类石墨层增强了吸附性能，从而减轻了硝酸盐还原反应（NitRR）过程中中间体的扩散并稳定了活性钴物种。使用MWCNT负载的钴催化剂，我们在含有0.1 M NO₃⁻的0.1 M KOH溶液中实现了4.03 mg h⁻¹ cm⁻²的显著NH₃产率和84.72%的高法拉第效率。这项研究证明了MWCNTs作为构建高效硝酸盐还原电催化剂的先进载体的潜力。
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