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A mechanistic study of molecular CO2 interaction and adsorption on carbon implanted SnS2 thin film for photocatalytic CO2 reduction activity
Nano Energy ( IF 16.8 ) Pub Date : 2020-03-19 , DOI: 10.1016/j.nanoen.2020.104717
Tadesse Billo , Indrajit Shown , Aswin kumar Anbalagan , Tirta Amerta Effendi , Amr Sabbah , Fang-Yu Fu , Che-Men Chu , Wei-Yen Woon , Ruei-San Chen , Chih-Hao Lee , Kuei-Hsien Chen , Li-Chyong Chen

Gas-phase photocatalytic reactions to convert carbon dioxide and water into oxygen and hydrocarbons are the foundation of life on earth. However, the efficiency of photosynthesis is relatively low (∼1%), which leaves much room for artificial photosynthesis to reach the benchmark of the solar cells (>15%). In this work, carbon implanted SnS2 thin films (C-SnS2) were prepared to study photocatalytic activity and adsorbate-catalyst surface interactions during CO2 photoreduction. The electron density distribution in C-SnS2 and its contribution toward the photogenerated charge transfer process has been analyzed by the angle-dependent X-ray absorption near-edge structure (XANES) study. The C-SnS2 surface affinity toward the CO2 molecule was monitored by in-situ dark current and Raman spectroscopy measurements. By optimizing the dose during ion implantation, SnS2 thin film with 1 wt% carbon incorporation shows 108 times enhancement in the CO2 conversion efficiency and more than 89% product selectivity toward CH4 formation compared with the as-grown SnS2 without carbon incorporation. The improved photocatalytic activity can be ascribed to enhanced light harvesting, pronounced charge-transfer between SnS2 and carbon with improved carrier separation and the availability of highly active carbon sites that serve as favorable CO2 adsorption sites.



中文翻译:

分子CO的机理研究2相互作用和吸附在碳上的SnS植入2薄膜为光催化CO 2还原活性

将二氧化碳和水转化为氧气和碳氢化合物的气相光催化反应是地球生命的基础。但是,光合作用的效率相对较低(约1%),这为人工光合作用达到太阳能电池的基准(> 15%)留下了很大的空间。在这项工作中,准备了碳注入的SnS 2薄膜(C-SnS 2),以研究CO 2光还原过程中的光催化活性和吸附物-催化剂表面的相互作用。通过角度相关的X射线吸收近边缘结构(XANES)研究,分析了C-SnS 2中的电子密度分布及其对光生电荷转移过程的贡献。C-SnS 2通过原位暗电流和拉曼光谱测量监测对CO 2分子的表面亲和力。通过优化离子注入过程中的剂量,与未掺碳的SnS 2相比,掺碳1 wt%的SnS 2薄膜的CO 2转化效率提高了108倍,产品对CH 4形成的选择性超过89%。。改善的光催化活性可以归因于增强的光收集,SnS 2和碳之间的显着电荷转移,改善的载流子分离以及用作有利CO 2的高活性碳位的可用性 吸附位。

更新日期:2020-03-20
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