Siheng Yang, Woo Jin Byun, Fangming Zhao, Dingwen Chen, Jiawei Mao, Wei Zhang, Jing Peng, Chengyuan Liu, Yang Pan, Jun Hu, Junfa Zhu, Xueli Zheng, Haiyan Fu, Maolin Yuan, Hua Chen, Ruixiang Li, Meng Zhou, Wei Che, Jong‐Beom Baek, Jae Sung Lee, Jiaqi Xu

CO2 Enrichment Boosts Highly Selective Infrared‐Light‐Driven CO2 Conversion to CH4 By UiO‐66/Co9S8 Photocatalyst

  • Mechanical Engineering
  • Mechanics of Materials
  • General Materials Science

AbstractPhotocatalytic 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 low‐energy IR light. To meet this challenge, 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 CO2 affinity. Notably, finite‐element method simulations reveal the porous structure of UiO‐66 enriches local CO2 concentration around Co9S8. As a result, Co9S8 or UiO‐66 alone doesn't show observable IR‐light photocatalytic activity, whereas UiO‐66/Co9S8 reveals exceptional activity. The CH4 evolution rate over UiO‐66/Co9S8 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 XAFS spectra verify the presence of two distinct Co sites and confirm the existence of metallic Co‐Co bond in Co9S8. Energy diagrams analysis and fs‐TA spectra manifest that CO2 reduction mainly occurs on Co9S8 for UiO‐66/Co9S8, while DFT 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 towards CH4.This article is protected by copyright. All rights reserved

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