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具有大比表面积和高效可见光驱动二氧化碳转化的单层空心 NiO-NiS 催化剂。

Single layered hollow NiO-NiS catalyst with large specific surface area and highly efficient visible-light-driven carbon dioxide conversion.

机构信息

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.

出版信息

Chemosphere. 2021 Oct;280:130759. doi: 10.1016/j.chemosphere.2021.130759. Epub 2021 May 3.

Abstract

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.

摘要

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。

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