Li Wanlu, Bandosz Teresa J
Department of Chemistry and Biochemistry, The City College of New York, New York, NY, 10031, USA.
Ph.D. Program in Chemistry, The Graduate Center of the City University of New York, New York, NY, 10016, USA.
ChemSusChem. 2018 Sep 11;11(17):2987-2999. doi: 10.1002/cssc.201801073. Epub 2018 Jul 19.
Thiourea-modified wood-based activated carbon materials were evaluated as catalysts for the CO electrochemical reduction reaction (CO ERR). The materials obtained at 950 °C showed long-term stability. The results indicated that thiophenic sulfur provides the catalytic activity for CO formation. However, it was not as active for CH formation as was pyridinic N. Tafel plots suggested that the nanoporous structure enhanced the kinetics for CO reduction. The electric conductivity limited the activity for CO ERR in the materials modified at 600, 800, and 900 °C. The effect of visible light on CO ERR was also investigated in this study. Upon irradiation, photocurrent was generated, and the current density increased during the CO reduction process. Combined with a band-gap alignment, the results indicate that thiophenic S in the carbon matrix contributed to the sample's photoactivity in visible light. These species enhance the overall reduction process, promoting both the hydrogen evolution reaction and CO reduction to CO.
硫脲改性的木质基活性炭材料被评估为用于CO电化学还原反应（CO ERR）的催化剂。在950°C下获得的材料表现出长期稳定性。结果表明，噻吩硫为CO的形成提供了催化活性。然而，它对CH形成的活性不如吡啶氮。塔菲尔曲线表明，纳米多孔结构增强了CO还原的动力学。在600、800和900°C改性的材料中，电导率限制了CO ERR的活性。本研究还研究了可见光对CO ERR的影响。辐照时会产生光电流，并且在CO还原过程中电流密度会增加。结合带隙排列，结果表明碳基质中的噻吩硫有助于样品在可见光下的光活性。这些物质增强了整体还原过程，促进了析氢反应以及CO还原为CO。
