Lenef Julia D, Lee Si Young, Fuelling Kalyn M, Rivera Cruz Kevin E, Prajapati Aditya, Delgado Cornejo Daniel O, Cho Tae H, Sun Kai, Alvarado Eugenio, Arthur Timothy S, Roberts Charles A, Hahn Christopher, McCrory Charles C L, Dasgupta Neil P
Department of Materials Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109, United States.
Department of Mechanical Engineering, University of Michigan, Ann Arbor, Michigan 48109, United States.
Nano Lett. 2023 Dec 13;23(23):10779-10787. doi: 10.1021/acs.nanolett.3c02917. Epub 2023 Nov 21.
Electrochemical reduction of CO using Cu catalysts enables the synthesis of C products including CH and CHOH. In this study, Cu catalysts were fabricated using plasma-enhanced atomic layer deposition (PEALD), achieving conformal deposition of catalysts throughout 3-D gas diffusion electrode (GDE) substrates while maintaining tunable control of Cu nanoparticle size and areal loading. The electrochemical CO reduction at the Cu surface yielded a total Faradaic efficiency (FE) > 75% for C products. Parasitic hydrogen evolution was minimized to a FE of ∼10%, and a selectivity of 42.2% FE for CH was demonstrated. Compared to a line-of-sight physical vapor deposition method, PEALD Cu catalysts show significant suppression of C products compared to C, which is associated with improved control of catalyst morphology and conformality within the porous GDE substrate. Finally, PEALD Cu catalysts demonstrated a stable performance for 15 h with minimal reduction in the CH production rate.
使用铜催化剂对CO进行电化学还原能够合成包括CH和CHOH在内的含碳产物。在本研究中,采用等离子体增强原子层沉积(PEALD)制备铜催化剂,实现了催化剂在三维气体扩散电极(GDE)基底上的保形沉积,同时保持对铜纳米颗粒尺寸和面积负载的可调控制。在铜表面进行的电化学CO还原反应中,含碳产物的总法拉第效率(FE)>75%。寄生析氢反应被最小化至FE约为10%,并且展示出对CH的选择性为42.2%FE。与视线物理气相沉积法相比,PEALD铜催化剂对含碳产物的抑制作用明显优于对碳的抑制作用,这与在多孔GDE基底内对催化剂形态和保形性的更好控制有关。最后,PEALD铜催化剂在15小时内表现出稳定的性能,CH生成速率的降低最小。