Hydrogen Energy and Sonochemistry Research Group, Department of Energy and Process Engineering, Norwegian University of Science and Technology (NTNU), Trondheim, Norway.
Microelectronics-Photonics Program, University of Arkansas, Fayetteville, AR, USA.
Ultrason Sonochem. 2021 Apr;72:105401. doi: 10.1016/j.ultsonch.2020.105401. Epub 2020 Dec 3.
The electrochemical CO reduction reaction (CO2RR) on polycrystalline copper (Cu) electrode was performed in a CO-saturated 0.10 M NaCO aqueous solution at 278 K in the absence and presence of low-frequency high-power ultrasound (f = 24 kHz, P ~ 1.23 kW/dm) in a specially and well-characterized sonoelectrochemical reactor. It was found that in the presence of ultrasound, the cathodic current (I) for CO reduction increased significantly when compared to that in the absence of ultrasound (silent conditions). It was observed that ultrasound increased the faradaic efficiency of carbon monoxide (CO), methane (CH) and ethylene (CH) formation and decreased the faradaic efficiency of molecular hydrogen (H). Under ultrasonication, a ca. 40% increase in faradaic efficiency was obtained for methane formation through the CO2RR. In addition, and interestingly, water-soluble CO reduction products such as formic acid and ethanol were found under ultrasonic conditions whereas under silent conditions, these expected electrochemical CO2RR products were absent. It was also found that power ultrasound increases the formation of smaller hydrocarbons through the CO2RR and may initiate new chemical reaction pathways through the sonolytic di-hydrogen splitting yielding other products, and simultaneously reducing the overall molecular hydrogen gas formation.
在 278 K 下,在不存在和存在低频高功率超声波(f=24 kHz,P~1.23 kW/dm)的情况下,在特殊且经过良好表征的声电化学反应器中,在 CO 饱和的 0.10 M NaCO 水溶液中对多晶铜(Cu)电极上的电化学 CO 还原反应(CO2RR)进行了研究。结果发现,与不存在超声波(无声条件)相比,存在超声波时,CO 还原的阴极电流(I)显着增加。观察到超声波增加了一氧化碳(CO)、甲烷(CH)和乙烯(CH)形成的法拉第效率,并降低了氢气(H)的法拉第效率。在超声作用下,通过 CO2RR 获得了甲烷形成的约 40%的法拉第效率增加。此外,有趣的是,在超声条件下发现了甲酸和乙醇等水溶性 CO 还原产物,而在无声条件下,这些预期的电化学 CO2RR 产物不存在。还发现,功率超声通过 CO2RR 增加了较小碳氢化合物的形成,并可能通过超声致氢分裂产生其他产物,同时减少整体氢气气体形成,从而引发新的化学反应途径。