Weiss John C, He Yanghua, Cullen David A, Benavidez Angelica, Jernigen Jeremy D, Zhang Hanguang, Osmieri Luigi, Zelenay Piotr
Materials Physics and Applications Division, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA.
Center for Nanophase Materials Science, Oak Ridge National Laboratory, Oak Ridge, TN, 37830, USA.
Small. 2025 Mar;21(10):e2412162. doi: 10.1002/smll.202412162. Epub 2025 Jan 16.
The atomic dispersion of nickel in Ni-N-C catalysts is key for the selective generation of carbon monoxide through the electrochemical carbon dioxide reduction reaction (CORR). Herein, the study reports a highly selective, atomically dispersed Ni-N-C catalyst with reduced Ni loading compared to previous reports. Extensive materials characterization fails to detect Ni crystalline phases, reveals the highest concentration of atomically dispersed Ni metal, and confirms the presence of the proposed Ni-N active site at this reduced loading. The catalyst shows excellent activity and selectivity toward CO generation, with a faradaic efficiency for CO generation (FE) of 97% and partial current density for CO (j) of -9.0 mA cm at -0.9 V in an electrochemical H-type cell. CORR activity and selectivity are also studied by rotating disk electrode (RDE) measurements where transport limitations can be suppressed. It is expected that the utility of these Ni-N-C catalysts will lie with tandem CORR reaction schemes to multi-carbon (C) products.
镍在Ni-N-C催化剂中的原子分散对于通过电化学二氧化碳还原反应(CORR)选择性生成一氧化碳至关重要。在此,该研究报告了一种高选择性、原子分散的Ni-N-C催化剂,与之前的报道相比,其镍负载量有所降低。大量的材料表征未能检测到镍晶相,揭示了原子分散镍金属的最高浓度,并证实了在这种降低的负载量下存在所提出的Ni-N活性位点。该催化剂对一氧化碳的生成表现出优异的活性和选择性,在电化学H型电池中,在-0.9 V时,一氧化碳生成的法拉第效率(FE)为97%,一氧化碳的分电流密度(j)为-9.0 mA cm²。还通过旋转圆盘电极(RDE)测量研究了CORR活性和选择性,其中可以抑制传输限制。预计这些Ni-N-C催化剂的用途将在于串联CORR反应方案以生成多碳(C)产物。