Zhurenok Angelina V, Vasichenko Danila B, Berdyugin Semen N, Gerasimov Evgeny Yu, Saraev Andrey A, Cherepanova Svetlana V, Kozlova Ekaterina A
Federal Research Center, Boreskov Institute of Catalysis SB RAS, Lavrentieva Ave. 5, Novosibirsk 630090, Russia.
Nikolaev Institute of Inorganic Chemistry, Siberian Branch of the Russian Academy of Science, Novosibirsk 630090, Russia.
Nanomaterials (Basel). 2023 Jul 26;13(15):2176. doi: 10.3390/nano13152176.
In this study, we proposed photocatalysts based on graphite-like carbon nitride with a low content (0.01-0.5 wt.%) of noble metals (Pd, Rh) for hydrogen evolution under visible light irradiation. As precursors of rhodium and palladium, labile aqua and nitrato complexes Rh(HO)(μ-OH)∙4HO and (EtN)[Pd(NO)], respectively, were proposed. To obtain metallic particles, reduction was carried out in H at 400 °C. The synthesized photocatalysts were studied using X-ray diffraction, X-ray photoelectron spectroscopy, UV-Vis diffuse reflectance spectroscopy and high-resolution transmission electron microscopy. The activity of the photocatalysts was tested in the hydrogen evolution from aqueous and aqueous alkaline solutions of TEOA under visible light with a wavelength of 428 nm. It was shown that the activity for the 0.01-0.5% Rh/g-CN series is higher than in the case of the 0.01-0.5% Pd/g-CN photocatalysts. The 0.5% Rh/g-CN sample showed the highest activity per gram of catalyst, equal to 3.9 mmol g h, whereas the most efficient use of the metal particles was found over the 0.1% Rh/g-CN photocatalyst, with the activity of 2.4 mol per gram of Rh per hour. The data obtained are of interest and can serve for further research in the field of photocatalytic hydrogen evolution using noble metals as cocatalysts.
在本研究中，我们提出了基于类石墨氮化碳且贵金属（钯、铑）含量较低（0.01 - 0.5 wt.%）的光催化剂，用于在可见光照射下析氢。分别提出了不稳定的水合和硝酸根配合物Rh(HO)(μ - OH)∙4HO和(EtN)[Pd(NO)]作为铑和钯的前驱体。为了获得金属颗粒，在400℃的氢气中进行还原。使用X射线衍射、X射线光电子能谱、紫外 - 可见漫反射光谱和高分辨率透射电子显微镜对合成的光催化剂进行了研究。在波长为428 nm的可见光下，测试了光催化剂在三乙醇胺水溶液和碱性水溶液中析氢的活性。结果表明，0.01 - 0.5% Rh/g - CN系列的活性高于0.01 - 0.5% Pd/g - CN光催化剂。0.5% Rh/g - CN样品每克催化剂显示出最高活性，等于3.9 mmol g h，而在0.1% Rh/g - CN光催化剂上发现金属颗粒的利用效率最高，每克铑每小时的活性为2.4 mol。所获得的数据很有意义，可用于以贵金属作为助催化剂的光催化析氢领域的进一步研究。
