Hou Pengfei, Song Wenli, Wang Xiuping, Hu Zhenpeng, Kang Peng
Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
University of Chinese Academy of Sciences, 19A Yuquan Road, Beijing, 100049, China.
Small. 2020 Jun;16(24):e2001896. doi: 10.1002/smll.202001896. Epub 2020 May 13.
Single-atom Co catalyst Co-Tpy-C with well-defined sites is synthesized by pyrolysis of a Co terpyridine (Tpy) organometallic complex. The Co-Tpy-C catalyst exhibits excellent activity for the electrochemical CO reduction reaction in aqueous electrolyte, with CO faradaic efficiency (FE) of over 95% from -0.7 to -1.0 V (vs RHE). By comparison, catalysts without Co or Tpy ligand added do not show any high CO FE. When simulated flue gas with 15% of CO is used as the source of CO , CO FE is kept at 90.1% at -0.5 V versus RHE. During gas phase flow electrolysis using simulated flue gas, the CO partial current density is further increased to 86.4 mA cm and CO FE reached >90% at the cell voltage of 3.4 V. Experiments and density functional theory calculations indicate that uniform single-atom Co-N sites mainly contribute to the high activity for CO reduction.
通过热解钴三联吡啶（Tpy）有机金属配合物合成了具有明确位点的单原子钴催化剂Co-Tpy-C。Co-Tpy-C催化剂在水性电解质中对电化学CO还原反应表现出优异的活性，在-0.7至-1.0 V（相对于可逆氢电极，RHE）范围内，CO法拉第效率（FE）超过95%。相比之下，未添加Co或Tpy配体的催化剂没有显示出任何高的CO FE。当使用含15%CO的模拟烟道气作为CO源时，在相对于RHE为-0.5 V的条件下，CO FE保持在90.1%。在使用模拟烟道气的气相流动电解过程中，CO分电流密度进一步提高到86.4 mA cm，在3.4 V的电池电压下，CO FE达到>90%。实验和密度泛函理论计算表明，均匀的单原子Co-N位点主要促成了CO还原的高活性。
