含铁双金属氰化物催化剂 CO2 加氢合成短链烯烃的对比研究,ACS Sustainable Chemistry & Engineering

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含铁双金属氰化物催化剂 CO2 加氢合成短链烯烃的对比研究
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2023-07-14 , DOI: 10.1021/acssuschemeng.3c01893
Gaje Singh _{1,

2} , Satyajit Panda _{1,

2} , Jyoti Gahtori _{1,

2} , Pranay Rajendra Chandewar ₃ , Pradeep Kumar ₁ , Indrajit K. Ghosh _{2,

4} , Ankush Biradar _{2,

5} , Debaprasad Shee ₃ , Ankur Bordoloi _{1,

2}

Affiliation

在本文中，我们使用一步传统沉淀法制备了一系列由铁和后 3d 过渡金属（Mn、Co、Cu 和 Zn）组成的 K 促进的双金属氰化物 (DMC) 催化剂，并检查了它们的性能。通过改进的费-托路线CO ₂对短链烯烃进行增值。进行了几次异位/原位结合程序升温脱附（TPD）实验来识别催化剂中的物质并评估还原催化剂的吸附/脱附特性。双金属催化剂的CO 2 转化率按以下顺序增加： Fe-Mn (R): 24.85% < Fe-Zn (R): 28.60 < Fe-Cu (R): 29.40% < Fe-Co (R) : _39.10 % 而短链烯烃 (C ₂ –C ₄⁼ )在碳氢化合物中按以下顺序降低: Fe-Mn (R): 56.1% > Fe-Cu (R): 55.4% > Fe-Zn (R): 50.8% > Fe-Co (R): 44.3%,在 20 bar 压力、320 °C 温度和 3600 mL·g _cat^–1 ·h ^–1气时空速 (GHSV) 下。值得注意的是，在反应条件优化过程中，Fe-Mn (R)催化剂对烃类的短链烯烃选择性前所未有地达到了63.8%，CO 2 转化率为30.56 _%。TPD结果和反应性能表明Fe-Co(R)催化剂对弱吸附的CO ₂、H ₂和CO具有较高的吸附性，从而导致较高的CO ₂转化率、较低的 CO 和较高的烃选择性以及较低的 O/P 比。相反，Fe-Mn (R) 催化剂表现出与 Fe-Co (R) 催化剂相反的反应结果，因为它对弱吸附的 CO 2 、_H 2_和CO 的吸附较低。这些发现揭示了反应物如何转化产物分布受催化剂对反应物和重要中间体的吸附/解吸特性影响。

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Comparative Study of Short-Chain Olefins Synthesis via CO2 Hydrogenation over Iron-Containing Double Metal Cyanide-Derived Catalysts

In this article, we prepared a series of K-promoted double metal cyanide (DMC) catalysts consisting of iron with a late 3d transition metal (Mn, Co, Cu, and Zn) using a single-step conventional precipitation method and examined them for CO₂ value addition to short-chain olefins via modified Fischer–Tropsch route. Several ex situ/in situ combined with temperature-programmed desorption (TPD) experiments were carried out to identify the species in the catalysts and evaluate the adsorption/desorption characteristics of the reduced catalysts. The CO₂ conversion for bimetallic catalysts increases in the following order: Fe–Mn (R): 24.85% < Fe–Zn (R): 28.60 < Fe–Cu (R): 29.40% < Fe–Co (R): 39.10% whereas selectivity of the short-chain olefins (C₂–C₄⁼) in hydrocarbons decreases in the following order: Fe–Mn (R): 56.1% > Fe–Cu (R): 55.4% > Fe–Zn (R): 50.8% > Fe–Co (R): 44.3%, at 20 bar pressure, 320 °C temperature, and a gas hour space velocity (GHSV) of 3600 mL·g_cat^–1·h^–1. Remarkably, during the optimization of the reaction conditions, short-chain olefins selectivity over the Fe–Mn (R) catalyst unprecedently reached up to 63.8% in hydrocarbons with 30.56% CO₂ conversion. The TPD results and reaction performance reveal that the Fe–Co (R) catalyst has higher adsorption for weakly adsorbed CO₂, H₂, and CO, which results in higher CO₂ conversion, lower CO, and higher hydrocarbon selectivity with a lower O/P ratio. Contrarily, the Fe–Mn (R) catalyst exhibits opposite reaction outcomes to the Fe–Co (R) catalyst owing to its lower adsorption for weakly adsorbed CO₂, H₂, and CO. These findings shed light on how the conversion of reactant and product distribution is affected by the adsorption/desorption characteristics of the catalysts for the reactant and important intermediates.

更新日期：2023-07-14

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