Chernyak Sergei A, Stolbov Dmitrii N, Maslakov Konstantin I, Kazantsev Ruslan V, Eliseev Oleg L, Moskovskikh Dmitry O, Savilov Serguei V
Department of Chemistry, Lomonosov Moscow State University, Leninskie Gory 1-3, Moscow 119991, Russia.
N.D. Zelinsky Institute of Organic Chemistry, Russian Academy of Sciences, Leninsky prosp. 47, Moscow 119991, Russia.
Nanomaterials (Basel). 2022 Dec 19;12(24):4491. doi: 10.3390/nano12244491.
Transformation of carbon oxides into valuable feedstocks is an important challenge nowadays. Carbon oxide hydrogenation to hydrocarbons over iron-based catalysts is one of the possible ways for this transformation to occur. Carbon supports effectively increase the dispersion of such catalysts but possess a very low bulk density, and their powders can be toxic. In this study, spark plasma sintering was used to synthesize new bulk and dense potassium promoted iron-based catalysts, supported on N-doped carbon nanomaterials, for hydrocarbon synthesis from syngas. The sintered catalysts showed high activity of up to 223 μmol/g/s at 300-340 °C and a selectivity to C fraction of ~70% with a high portion of olefins. The promising catalyst performance was ascribed to the high dispersity of iron carbide particles, potassium promotion of iron carbide formation and stabilization of the active sites with nitrogen-based functionalities. As a result, a bulk N-doped carbon-supported iron catalyst with 3D structure was prepared, for the first time, by a fast method, and demonstrated high activity and selectivity in hydrocarbon synthesis. The proposed technique can be used to produce well-shaped carbon-supported catalysts for syngas conversion.
如今，将碳氧化物转化为有价值的原料是一项重大挑战。在铁基催化剂上将碳氧化物加氢转化为碳氢化合物是实现这种转化的一种可能途径。碳载体可有效提高此类催化剂的分散性，但堆积密度很低，且其粉末可能有毒。在本研究中，采用放电等离子烧结法合成了负载在氮掺杂碳纳米材料上的新型块状致密钾促进铁基催化剂，用于由合成气合成碳氢化合物。烧结后的催化剂在300 - 340°C下表现出高达223 μmol/g/s的高活性，对C馏分的选择性约为70%，其中烯烃含量较高。这种有前景的催化剂性能归因于碳化铁颗粒的高分散性、钾对碳化铁形成的促进作用以及含氮官能团对活性位点的稳定作用。结果，首次通过一种快速方法制备了具有三维结构的块状氮掺杂碳负载铁催化剂，并在碳氢化合物合成中表现出高活性和选择性。所提出的技术可用于制备形状良好的碳负载催化剂用于合成气转化。
