Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterial Science, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht, The Netherlands.
Nat Commun. 2019 Jan 11;10(1):167. doi: 10.1038/s41467-018-08019-7.
Due to the surge of natural gas production, feedstocks for chemicals shift towards lighter hydrocarbons, particularly methane. The success of a Gas-to-Chemicals process via synthesis gas (CO and H) depends on the ability of catalysts to suppress methane and carbon dioxide formation. We designed a Co/Mn/Na/S catalyst, which gives rise to negligible Water-Gas-Shift activity and a hydrocarbon product spectrum deviating from the Anderson-Schulz-Flory distribution. At 240 °C and 1 bar, it shows a C-C olefins selectivity of 54%. At 10 bar, it displays 30% and 59% selectivities towards lower olefins and fuels, respectively. The spent catalyst consists of 10 nm Co nanoparticles with hcp Co metal phase. We propose a synergistic effect of Na plus S, which act as electronic promoters on the Co surface, thus improving selectivities towards lower olefins and fuels while largely reducing methane and carbon dioxide formation.
由于天然气产量的激增,化工原料转向更轻的碳氢化合物,特别是甲烷。通过合成气(CO 和 H)转化为化学品的工艺的成功取决于催化剂抑制甲烷和二氧化碳形成的能力。我们设计了一种 Co/Mn/Na/S 催化剂,它几乎没有水煤气变换活性,烃产物谱偏离安德森-舒尔茨-弗洛里分布。在 240°C 和 1 巴下,它表现出 54%的 C-C 烯烃选择性。在 10 巴下,它对低级烯烃和燃料的选择性分别为 30%和 59%。废催化剂由 10nm 的 hcp Co 金属相 Co 纳米颗粒组成。我们提出了 Na 和 S 的协同作用,它们在 Co 表面起到电子促进剂的作用,从而提高了低级烯烃和燃料的选择性,同时大大减少了甲烷和二氧化碳的形成。