Wang Jihao, Chen Shilong, Ticali Pierfrancesco, Summa Paulina, Mai Simon, Skorupska Katarzyna, Behrens Malte
Institute of Inorganic Chemistry, Kiel University, Max-Eyth-Str. 2, 24118 Kiel, Germany.
Department of Inorganic Chemistry, Fritz-Haber-Institute of the Max-Planck-Society, Faradayweg 4-6, 14195 Berlin, Germany.
Nanoscale. 2024 Sep 26;16(37):17378-17392. doi: 10.1039/d4nr02025a.
Aiming at a comprehensive understanding of support effects on Ni-based bimetallic catalyst for CO hydrogenation, spectroscopy (DRIFTS) with CO as a probe molecule and temperature-programmed techniques were used to investigate the impact of different supports (MgO, CeO, ZrO) on Ni- and Ni,Fe catalysts. Kinetic parameters revealed that the higher selectivity to methanation for Ni and Ni,Fe supported on the reducible oxides (CeO, ZrO) is due to the inhibition of reverse water-gas shift reaction (RWGS) by hydrogen. A promoting effect of Fe on Ni was only observed on MgO-supported catalysts. In situ DRIFTS with CO adsorption showed different electronic properties of Ni sites with partially reduced oxide ( ZrO and CeO). H-TPR and CO-TPD confirmed the significant role of metal-support interaction (MSI) in CeO-supported catalysts for CO activation. The MSI between Ni/Ni,Fe and reducible supports are crucial for catalytic performance, ultimately leading to the higher activity and stability in CO hydrogenation.
为全面了解载体对用于CO加氢的镍基双金属催化剂的影响,采用以CO为探针分子的光谱法(漫反射红外傅里叶变换光谱法,DRIFTS)和程序升温技术,研究了不同载体(MgO、CeO、ZrO)对Ni催化剂和Ni,Fe催化剂的影响。动力学参数表明,负载在可还原氧化物(CeO、ZrO)上的Ni和Ni,Fe对甲烷化的选择性较高,这是由于氢气抑制了逆水煤气变换反应(RWGS)。仅在MgO负载的催化剂上观察到Fe对Ni的促进作用。CO吸附原位DRIFTS表明,部分还原氧化物(ZrO和CeO)负载的Ni位点具有不同的电子性质。H-TPR和CO-TPD证实了金属-载体相互作用(MSI)在CeO负载的CO活化催化剂中的重要作用。Ni/Ni,Fe与可还原载体之间的MSI对催化性能至关重要,最终导致CO加氢具有更高的活性和稳定性。