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DOI10.1002/adma.202312616
CO2 Enrichment Boosts Highly Selective Infrared-Light-Driven CO2 Conversion to CH4 by UiO-66/Co9S8 Photocatalyst
发表日期2024
ISSN0935-9648
EISSN1521-4095
英文摘要Photocatalytic CO2 reduction to high-value chemicals is an attractive approach to mitigate climate change, but it remains a great challenge to produce a specific product selectively by IR light. Hence, UiO-66/Co9S8 composite is designed to couple the advantages of metallic photocatalysts and porous CO2 adsorbers for IR-light-driven CO2-to-CH4 conversion. The metallic nature of Co9S8 endows UiO-66/Co9S8 with exceptional IR light absorption, while UiO-66 dramatically enhances its local CO2 concentration, revealed by finite-element method simulations. As a result, Co9S8 or UiO-66 alone does not show observable IR-light photocatalytic activity, whereas UiO-66/Co9S8 exhibits exceptional activity. The CH4 evolution rate over UiO-66/Co9S8 reaches 25.7 mu mol g(-1) h(-1) with ca.100% selectivity under IR light irradiation, outperforming most reported catalysts under similar reaction conditions. The X-ray absorption fine structure spectroscopy spectra verify the presence of two distinct Co sites and confirm the existence of metallic Co & horbar;Co bond in Co9S8. Energy diagrams analysis and transient absorption spectra manifest that CO2 reduction mainly occurs on Co9S8 for UiO-66/Co9S8, while density functional theory calculations demonstrate that high-electron-density Co1 sites are the key active sites, possessing lower energy barriers for further protonation of *CO, leading to the ultra-high selectivity toward CH4.
英文关键词CO2 enrichment; CO2 photoreduction; infrared light photocatalysis; metallic photocatalysts
语种英语
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS类目Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS记录号WOS:001143291400001
来源期刊ADVANCED MATERIALS
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/296603
作者单位Sichuan University; Ulsan National Institute of Science & Technology (UNIST); Chinese Academy of Sciences; University of Science & Technology of China, CAS; Sichuan University; Sichuan University; Chinese Academy of Sciences; Shenzhen Institute of Advanced Technology, CAS
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GB/T 7714
. CO2 Enrichment Boosts Highly Selective Infrared-Light-Driven CO2 Conversion to CH4 by UiO-66/Co9S8 Photocatalyst[J],2024.
APA (2024).CO2 Enrichment Boosts Highly Selective Infrared-Light-Driven CO2 Conversion to CH4 by UiO-66/Co9S8 Photocatalyst.ADVANCED MATERIALS.
MLA "CO2 Enrichment Boosts Highly Selective Infrared-Light-Driven CO2 Conversion to CH4 by UiO-66/Co9S8 Photocatalyst".ADVANCED MATERIALS (2024).
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