Department of Chemistry, College of Natural Sciences, Yeungnam University, Gyeongsan, Gyeongbuk, 38541, Republic of Korea.
School of Chemical Engineering, Yeungnam University, Gyeongsan, Gyeongbuk, 38541, Republic of Korea.
Chemosphere. 2021 Oct;280:130759. doi: 10.1016/j.chemosphere.2021.130759. Epub 2021 May 3.
A sea urchin-shaped, single-layer, and hollow NiO-NiS photocatalyst with a large surface area was designed for carbon dioxide (CO) conversion in this study. A d-glucose polymeric hollow frame was fabricated using a d-glucose monomer, and NiO particles were stably grown on it using the hydrothermal method to form a hollow NiO surface. The d-glucose frame was removed by heat treatment to create hollowed NiO; hollowed NiO-NiS (h-NiO-NiS) was subsequently obtained through ion exchange between the O ions in NiO and S ions in the sulfur powder. Additionally, we attempted to determine the correlation among the surface area of the h-NiO-NiS catalyst, CO gas adsorption capacity, and catalyst performance. The surface area of the h-NiO-NiS catalyst was ten times larger than that of the nanometer-sized NiO-NiS (n-NiO-NiS, 21.2 m g) catalyst. The CO photocatalytic conversion performance of the hollowed catalyst was approximately seven times larger than that of the nanosized catalyst. As the amount of ion-exchanged S increased, methane selectivity increased, and optimal methane production was obtained when the weight ratio of NiO and sulfur powder was 1 : 4. Using temperature-programmed desorption (TPD) analyses of CO and HO, the adsorption of water molecules on the Ni-S surface and that of CO gas on the Ni-O surface during CO conversion reaction were confirmed. The h-NiO-NiS catalyst facilitated an effective charge separation through a well-developed interfacial transition between the linked NiS and NiO, and resulted in increased CO photoreduction performance under sunlight.
本研究设计了一种具有大比表面积的海胆状单层中空 NiO-NiS 光催化剂,用于二氧化碳(CO)转化。使用 d-葡萄糖单体制备了 d-葡萄糖聚合空心框架,然后通过水热法在其上稳定生长 NiO 颗粒,形成空心 NiO 表面。通过热处理去除 d-葡萄糖框架,从而产生空心化的 NiO;随后通过 NiO 中的 O 离子与硫磺粉末中的 S 离子之间的离子交换得到空心 NiO-NiS(h-NiO-NiS)。此外,我们尝试确定 h-NiO-NiS 催化剂的表面积、CO 气体吸附能力和催化剂性能之间的相关性。h-NiO-NiS 催化剂的表面积是纳米级 NiO-NiS(n-NiO-NiS,21.2 m g)催化剂的十倍。空心催化剂的 CO 光催化转化率约为纳米催化剂的七倍。随着离子交换 S 的增加,甲烷选择性增加,当 NiO 和硫磺粉末的重量比为 1:4 时,可获得最佳的甲烷产量。通过 CO 和 HO 的程序升温脱附(TPD)分析,确认了在 CO 转化反应过程中 Ni-S 表面上水分子的吸附以及 Ni-O 表面上 CO 气体的吸附。h-NiO-NiS 催化剂通过链接的 NiS 和 NiO 之间良好发展的界面过渡促进了有效的电荷分离,从而在阳光照射下提高了 CO 光还原性能。