Fischer-Tropsch Synthesis of C4-C5 Isoparaffins via CoxMn1-xO Nanocomposites with Suppressed CO2.

IF 4.3 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Inorganic Chemistry Pub Date : 2024-07-03 DOI:10.1021/acs.inorgchem.4c02142
Yaozhen Liang, Xueqing Zhang, Yuhu Wang, Haibo Chen, Yuhua Zhang, Jinlin Li, Li Wang
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Abstract

The synthesis of a specific product via the Fischer-Tropsch synthesis remains challenging due to the uncontrollable coupling of CHx on active sites. Isoparaffins, essential high-quality petroleum additives for improving octane numbers, are primarily derived from petroleum or natural gas. With petroleum reserves dwindling and the associated low selectivity, the direct conversion of syngas to isoparaffins has emerged as a promising alternative. This study presents a tandem catalyst comprising CoxMn1-xO and zeolites for catalyzing the direct conversion of syngas to C4-C5 isoparaffins. The relay catalyst exhibited an impressive selectivity of 55.6% toward the desired products while maintaining a low CO2 selectivity of approximately 20%. Notably, the selectivity of isobutane reached 43.5%, exceeding predictions based on the Anderson-Schulz-Flory distribution. Syngas undergoes conversion into olefins on CoxMn1-xO nanocomposites, diffuses into microporous zeolites, and interacts with Brønsted acids to produce isoparaffins. The stability of the relay catalyst relied significantly on the pore characteristics and acidic density of the zeolites.

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通过抑制 CO2 的 CoxMn1-xO 纳米复合材料进行 C4-C5 异链烷烃的费托合成。
由于活性位点上 CHx 的不可控耦合,通过费托合成合成特定产品仍然具有挑战性。异构烷烃是提高辛烷值必不可少的优质石油添加剂,主要来自石油或天然气。随着石油储量的减少以及相关的低选择性,将合成气直接转化为异构烷烃已成为一种前景广阔的替代方法。本研究提出了一种由 CoxMn1-xO 和沸石组成的串联催化剂,用于催化合成气直接转化为 C4-C5 异构烷烃。中继催化剂对所需产物的选择性高达 55.6%,同时保持了约 20% 的低二氧化碳选择性。值得注意的是,异丁烷的选择性达到 43.5%,超过了基于安德森-舒尔茨-弗洛里分布的预测值。合成气在 CoxMn1-xO 纳米复合材料上转化为烯烃,扩散到微孔沸石中,并与布氏酸作用生成异链烷烃。中继催化剂的稳定性在很大程度上取决于沸石的孔隙特征和酸性密度。
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来源期刊
Inorganic Chemistry
Inorganic Chemistry 化学-无机化学与核化学
CiteScore
7.60
自引率
13.00%
发文量
1960
审稿时长
1.9 months
期刊介绍: Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.
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