双金属氮化物NiMoN析氢催化剂制备及其电解海水析氢性能的研究
收稿日期: 2022-07-15
网络出版日期: 2022-09-19
基金资助
国家自然科学基金(22008134)
Preparation of Highly Active Transition Bimetallic Nitride NiMoN Hydrogen Evolution Reaction (HER) Catalyst and Its Performance Study in Seawater Electrolysis
Received date: 2022-07-15
Online published: 2022-09-19
Supported by
National Natural Science Foundation of China(22008134)
电解水制氢是最具潜力的绿氢制备技术, 而高效析氢反应(HER)催化剂的开发对其大规模推广意义重大. 选用氯化镍和钼酸铵为镍源和钼源, 通过原位生长法获得NiMo双金属催化剂前驱体, 再以二腈二胺为氮源, 高温氮化-程序升温法制备了一系列NiMoxN@NC催化剂(x代表钼酸铵和氯化镍的物质的量比), 并对催化剂进行了结构、形貌以及金属价态表征. 分别在1 mol/L KOH碱液以及模拟海水中分析了析氢(HER)性能. 结果表明, 碱液中NiMoxN@NC催化剂均具有良好的电荷转移速率(Rct<1 Ω), 具有较好的内在催化活性(Tafel斜率103~168 mV/dec). 其中, NiMo0.75N@NC催化剂具有最高的极限电流(–178 mA/cm2), 最小的过电势η10=0.164 V, η100=0.448 V), 最高的内在催化活性, Tafel斜率只有103 mV/dec, 且具有较好的稳定性. 在海水中, 在10 mA/cm2和40 mA/cm2的负载电流下, NiMo0.75N@NC催化剂依旧表现出了较好的稳定性.
关键词： 氢能源; 过渡双金属氮化物催化剂; NiMoN@NC催化剂; 海水制氢; 析氢反应(HER)过程
蒋博龙 , 崔艳艳 , 史顺杰 , 姜楠 , 谭伟强 . 双金属氮化物NiMoN析氢催化剂制备及其电解海水析氢性能的研究[J]. 化学学报, 2022 , 80(10) : 1394 -1400 . DOI: 10.6023/A22070309
Hydrogen production by water electrolysis was supposed to be the most potential green hydrogen production technology. The development of high-efficiency hydrogen evolution reaction (HER) catalyst is of great significance for its large-scale promotion. In this study, nickel chloride and ammonium molybdate were used as nickel and molybdenum sources respectively to obtain the precursor of NiMo bimetallic catalyst by in-situ growth method. The dinitrile diamine was used as nitrogen source and a series of NiMoxN@NC (x represents the molar ratio of ammonium molybdate and nickel chloride) catalysts were prepared by high temperature nitridation temperature programmed method and characterized by X-ray diffraction (XRD), scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS). The HER performance of as prepared catalysts was tested in 1 mol/L KOH solution and simulated seawater respectively. Results showed that all NiMoxN@NC catalysts have presented a relatively high conductivity (Rct<1 Ω) and intrinsic catalytic activity (Tafel slope of 103~168 mV/dec). Among them, the NiMo0.75N@NC catalyst posessed the highest limiting current density (–178 mA/cm2) and the lowest overpotential η at certain current densities of 10 mA/cm2 and 100 mA/cm2 (η10=0.164 V, η100=0.448 V). Furthermore, the NiMo0.75N@NC catalyst has also presented a relatively high stability in KOH solution and seawater.
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