Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
Adv Mater. 2018 Feb;30(7). doi: 10.1002/adma.201705872. Epub 2018 Jan 8.
Electroreduction of CO is a sustainable approach to produce syngas with controllable ratios, which are required as specific reactants for the optimization of different industrial processes. However, it is challenging to achieve tunable syngas production with a wide ratio of CO/H , while maintaining a high current density. Herein, cadmium sulfoselenide (CdS Se ) alloyed nanorods are developed, which enable the widest range of syngas proportions ever reported at the current density above 10 mA cm in CO electroreduction. Among CdS Se nanorods, CdS nanorods exhibit the highest Faradaic efficiency (FE) of 81% for CO production with a current density of 27.1 mA cm at -1.2 V vs. reversible hydrogen electrode. With the increase of Se content in CdS Se nanorods, the FE for H production increases. At -1.2 V vs. RHE, the ratios of CO/H in products vary from 4:1 to 1:4 on CdS Se nanorods (x from 1 to 0). Notably, all proportions of syngas are achieved with current density higher than ≈25 mA cm . Mechanistic study reveals that the increased Se content in CdS Se nanorods strengthens the binding of H atoms, resulting in the increased coverage of H* and thus the enhanced selectivity for H production in CO electroreduction.
电还原 CO 是一种可持续的方法,可以生产出具有可控比例的合成气,这些合成气是优化不同工业过程所需的特定反应物。然而,在维持高电流密度的同时,实现可调谐的合成气生产,具有较宽的 CO/H 比例,是具有挑战性的。在此,开发了硫化镉硒(CdS Se)合金纳米棒,其在 CO 电还原的电流密度高于 10 mA cm 时,实现了迄今为止报道的最宽的合成气比例范围。在 CdS Se 纳米棒中,CdS 纳米棒在 -1.2 V 相对于可逆氢电极时,具有最高的 81%的 CO 生产法拉第效率(FE),电流密度为 27.1 mA cm -1 。随着 CdS Se 纳米棒中 Se 含量的增加,H 生产的 FE 增加。在 -1.2 V 相对于 RHE 时,产物中 CO/H 的比例在 CdS Se 纳米棒(x 从 1 到 0)上从 4:1 变化到 1:4。值得注意的是,所有比例的合成气都是在高于 ≈25 mA cm 的电流密度下实现的。机理研究表明,CdS Se 纳米棒中增加的 Se 含量增强了 H 原子的结合,导致 H*的覆盖率增加,从而增强了 CO 电还原中 H 生产的选择性。