Maimaiti Halidan, Awati Abuduheiremu, Zhang Dedong, Yisilamu Gunisakezi, Xu Bo
Institute of Chemistry and Chemical Industry, Xinjiang University Urumqi 830046 Xinjiang China
RSC Adv. 2018 Oct 23;8(63):35989-35997. doi: 10.1039/c8ra06062b. eCollection 2018 Oct 22.
To obtain high-efficiency, low-cost, environmentally friendly carbon-based photocatalytic material, we synthesized coal-based carbon dots with sp carbon structure and multilayer graphene lattice structure by the hydrogen peroxide (HO) oxidation method to strip nano-scale crystalline carbon in the coal structure and link with oxygen-containing groups such as the hydroxyl group. N, S co-doped aminated coal-based carbon nanoparticles (NH-CNPs) were then obtained by thionyl chloride chlorination and ethylenediamine passivation. The physical properties and chemical structure of the synthesized NH-CNPs were studied and the photocatalytic CO reduction performance was tested. The results show that NH-CNPs are vesicle-type spherical particles with particle size of 42.16 ± 7.5 nm and have a mesoporous structure that is capable of adsorbing CO. A defect structure was formed on the surface of the NH-CNPs due to the doping of N and S elements, thereby significantly improving the ability to photogenerate electrons under visible light along with the ability to efficiently separate the photo-generated carriers. The photocatalytic reduction products of CO over NH-CNPs were CHOH, CO, CHOH, H and CH. After 10 hours of reaction, the total amount of products was 807.56 μmol g cat, the amount of CHOH was 618.7 μmol g cat, and the calculated selectivity for conversion of CO to CHOH was up to 76.6%.
为了获得高效、低成本、环境友好的碳基光催化材料,我们通过过氧化氢(HO)氧化法合成了具有sp碳结构和多层石墨烯晶格结构的煤基碳点,以剥离煤结构中的纳米级结晶碳并与羟基等含氧基团相连。然后通过亚硫酰氯氯化和乙二胺钝化获得N、S共掺杂的胺化煤基碳纳米颗粒(NH-CNPs)。研究了合成的NH-CNPs的物理性质和化学结构,并测试了其光催化CO还原性能。结果表明,NH-CNPs为囊泡型球形颗粒,粒径为42.16±7.5nm,具有能够吸附CO的介孔结构。由于N和S元素的掺杂,在NH-CNPs表面形成了缺陷结构,从而显著提高了可见光下光生电子的能力以及光生载流子的有效分离能力。NH-CNPs上CO的光催化还原产物为CHOH、CO、CHOH、H和CH。反应10小时后,产物总量为807.56μmol g cat,CHOH的量为618.7μmol g cat,计算得到的CO转化为CHOH的选择性高达76.6%。