材料科学
光催化
吸收(声学)
光化学
纳米技术
催化作用
分析化学(期刊)
化学
有机化学
复合材料
作者
Siheng Yang,Woo‐Jin Byun,Fei Zhao,Dingwen Chen,Jiang‐Gao Mao,Wei Zhang,Jing Peng,Chengyuan Liu,Yang Pan,Jun Huang,Junfa Zhu,Xueli Zheng,Haixia Fu,Maolin Yuan,Hua Chen,Ruixiang Li,Meng Zhang,Wei Che,Jong‐Beom Baek,Jin Ho Lee,Jiaqi Xu
标识
DOI:10.1002/adma.202312616
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/Co9 S8 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 Co9 S8 endows UiO-66/Co9 S8 with exceptional IR light absorption, while UiO-66 dramatically enhances its local CO2 concentration, revealed by finite-element method simulations. As a result, Co9 S8 or UiO-66 alone does not show observable IR-light photocatalytic activity, whereas UiO-66/Co9 S8 exhibits exceptional activity. The CH4 evolution rate over UiO-66/Co9 S8 reaches 25.7 µmol 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─Co bond in Co9 S8 . Energy diagrams analysis and transient absorption spectra manifest that CO2 reduction mainly occurs on Co9 S8 for UiO-66/Co9 S8 , 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 .
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