Gao Shuang, Li Guo-Dong, Liu Yipu, Chen Hui, Feng Liang-Liang, Wang Yun, Yang Min, Wang Dejun, Wang Shan, Zou Xiaoxin
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, International Joint Research Laboratory of Nano-Micro Architecture Chemistry, College of Chemistry, Jilin University, 2699 Qianjin Street, Changchun 130012, China.
Nanoscale. 2015 Feb 14;7(6):2306-16. doi: 10.1039/c4nr04924a.
One of the main barriers blocking sustainable hydrogen production is the use of expensive platinum-based catalysts to produce hydrogen from water. Herein we report the cost-effective synthesis of catalytically active, nitrogen-doped, cobalt-encased carbon nanotubes using inexpensive starting materials-urea and cobalt chloride hexahydrate (CoCl2·6H2O). Moreover, we show that the as-obtained nanocarbon material exhibits a remarkable electrocatalytic activity toward the hydrogen evolution reaction (HER); and thus it can be deemed as a potential alternative to noble metal HER catalysts. In particular, the urea-derived carbon nanotubes synthesized at 900 °C (denoted as U-CNT-900) show a superior catalytic activity for HER with low overpotential and high current density in our study. Notably also, U-CNT-900 has the ability to operate stably at all pH values (pH 0-14), and even in buffered seawater (pH 7). The possible synergistic effects between carbon-coated cobalt nanoparticles and the nitrogen dopants can be proposed to account for the HER catalytic activity of U-CNT-900. Given the high natural abundance, ease of synthesis, and high catalytic activity and durability in seawater, this U-CNT-900 material is promising for hydrogen production from water in industrial applications.
阻碍可持续制氢的主要障碍之一是使用昂贵的铂基催化剂从水中制氢。在此,我们报告了使用廉价的起始原料——尿素和六水合氯化钴(CoCl₂·6H₂O),以具有成本效益的方式合成具有催化活性的氮掺杂钴包覆碳纳米管。此外,我们表明所获得的纳米碳材料对析氢反应(HER)表现出显著的电催化活性;因此,它可被视为贵金属HER催化剂的潜在替代品。特别是,在我们的研究中,900℃合成的尿素衍生碳纳米管(表示为U-CNT-900)对HER表现出优异的催化活性,具有低过电位和高电流密度。同样值得注意的是,U-CNT-900能够在所有pH值(pH 0 - 14)下稳定运行,甚至在缓冲海水中(pH 7)也是如此。可以提出碳包覆钴纳米颗粒与氮掺杂剂之间可能的协同效应来解释U-CNT-900的HER催化活性。鉴于其高天然丰度、易于合成以及在海水中的高催化活性和耐久性,这种U-CNT-900材料在工业应用中从水中制氢方面具有广阔前景。