Linking catalyst synthesis strategies to CO2-modified Fischer-Tropsch performance in iron-carbon systems

doi:10.1016/S1872-2067(26)65007-3

Abstract

Abstract:

The direct thermocatalytic hydrogenation of CO₂ into value-added hydrocarbons is vital for advancing a sustainable carbon economy. However, the structural complexity and multi-step nature of catalyst synthesis often obscure the direct relationship between synthesis protocol and catalytic performance. To address this gap, we present an operationally simpler, safer to start up, and scalable strategy to develop carbon-coated iron-based catalysts (Fe@C and Fe@NC) through ball milling or impregnation of commercial iron salts with simple organic ligands (trimesic acid or salicylic acid), followed by pyrolysis. These catalysts feature tunable porosity, particle size, and surface composition, enabling systematic performance optimization in CO₂-modified Fischer-Tropsch synthesis (CO₂-FTS). Ball milling proved more effective for Fe@C systems, while impregnation was superior for Fe@NC systems, both achieving high selectivity for long-chain (C₅⁺) hydrocarbons and suppressing undesired C₁ byproducts. Ball milling promotes active site dispersion and carburization via porous frameworks, whereas impregnation facilitates cavity formation favorable for catalysis. Coupling these iron-based catalysts with ZSM-5 zeolites enabled aromatics production with enhanced stability. Correlations between synthesis route, catalyst architecture, and performance (activity, selectivity, structural control) were established. This work offers a practical synthesis-performance framework for designing CO₂-FTS catalysts, supporting future developments in carbon valorization and e-fuel production.

Key words: Heterogeneous catalysis, CO₂ hydrogenation, Fischer-Tropsch synthesis, Hydrocarbons, Iron-carbide

Shican Jiang, Mingyu Yi, Zuozheng Liu, Abhishek Dutta Chowdhury. Linking catalyst synthesis strategies to CO₂-modified Fischer-Tropsch performance in iron-carbon systems[J]. Chinese Journal of Catalysis, 2026, 84: 236-249.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65007-3

https://www.cjcatal.com/EN/Y2026/V84/I5/236

Figures/Tables 8

Fig. 1. The schematic presentation of catalyst synthesis strategies (ball milling vs. impregnation) used in this work, including their nomenclature (ferrous glycinate-FG, ferric acetylacetonate-FAC, trimesic acid-BTC, salicylic acid-SA).

Fig. 2. XRD patterns of standalone ligand, commercial iron salt, and iron-ligand complexes (a), Fe@C-FAC+BTC-based (b), and Fe@C-FAC+SA-based (c) pyrolyzed catalysts (ferric acetylacetonate-FAC, trimesic acid-BTC, salicylic acid-SA, ball milling-BM, impregnation-IM).

Fig. 3. Preliminary catalytic performance evaluation of pyrolyzed K-promoted Fe@C-catalysts after adding organic ligands at different mass ratios and using different protocols (i.e., BM vs. IM). The comparison between K/Fe@C-FAC and K/Fe@C-FAC catalysts with different Fe salts/BTC mass ratios (a) and their synthesis method (b). (c) The comparison between K/Fe@C-FAC and K/Fe@C-FAC catalysts with different mass ratios of Fe salts/SA. Reaction conditions: without any reductive treatment, H2/CO2?=?3, 350?°C, 3?MPa, 18000?mL g-1 h-1 at a time on stream of 6-7 h. See Figs. S19-S30 for the full TOS data. Note that synthesized materials were presented in a “Fe@C-FAC+BTC (or SA)-x-y+ BM (or IM) manner, where x and y refer to the mass ratio of commercial iron salts to carbon sources (ligands), respectively (ferric acetylacetonate-FAC, trimesic acid-BTC, salicylic acid-SA, ball milling-BM, impregnation-IM).

Fig. 4. XRD patterns of ligand, commercial iron salt and iron-ligand complexes (a), Fe@NC+BTC-based catalysts (b), and Fe@NC+SA-based catalysts (c). Ferrous glycinate-FG, trimesic acid-BTC, salicylic acid-SA, ball milling-BM, impregnation-IM.

Fig. 5. Preliminary catalytic performance evaluation of pyrolyzed K-promoted Fe@NC-catalysts after adding organic ligands at different mass ratios and using different protocols (i.e., BM vs. IM). Evaluation of K/Fe@NC-FG catalysts with a different mass ratio of commercial iron salts to BTC (a) and their different synthesis methods (b). (c) Evaluation of K/Fe@NC-FG catalysts with a different mass ratio of commercial iron salts to SA. Reaction conditions: without any reductive treatment, H2/CO2 = 3, 350 °C, 3 MPa, 18000 mL g-1 h-1 at a time on stream of 6-7 h. See Figs. S43-S54 for the full TOS data. Note that synthesized materials were presented in a “Fe@NC-FG+BTC (or SA)-x-y+ BM (or IM) manner, where x and y refer to the mass ratio of commercial iron salts to carbon sources (ligands), respectively (ferrous glycinate-FG trimesic acid-BTC, salicylic acid-SA, ball milling-BM, impregnation-IM).

Fig. 6. Impact of synthesis method and reaction parameters on FTS performance over K-promoted K/Fe@NC-FG (a) and K/Fe@C-FAC (b) catalytic systems, along with their net selectivity increase/decrease with respect to organic-free catalytic systems (c,d). Reaction conditions: without any reductive treatment, H2/CO2 = 3, 350-240 °C, 3 MPa, 18000-4800 mL g-1 h-1 at a time on stream of 6-7 h. See Figs.S19-S30, S43-69 for the full TOS data. Note that synthesized materials were presented in a “Fe@NC-FG+BTC (or SA)-x-y+ BM (or IM) manner, where x and y refer to the mass ratio of commercial iron salts to carbon sources (ligands), respectively (ferrous glycinate-FG, ferric acetylacetonate-FAC, trimesic acid-BTC, salicylic acid-SA, ball milling-BM, impregnation-IM).

Fig. 7. Catalyst performance evaluation of bifunctional (K/Fe@NC-FG+SA-1-1+IM + zeolite ZSM-5)-based catalytic systems during CO2-derived FTS process. Combined with ZSM-5 zeolites with different silica-alumina ratios (a) and different integration manners (b). Reaction conditions: H2/CO2 = 3, 350 °C, 3 MPa, F = 12 mL/min, K/Fe@NC-FG+SA-1-1+IM: 40 mg, ZSM-5: 80 mg at a time on stream of 20 h We refer to Figs. S76?S81 for additional catalysis figures (ferrous glycinate-FG, salicylic acid-SA, impregnation-IM).

Fig. 8. The hypothesized working protocol is based on the understanding of this work. Direct pyrolysis of iron salts causes agglomeration, reducing active site exposure and activity. Ball milling with trimesic acid or impregnation with salicylic acid before pyrolysis improves dispersion, reduces particle size, and forms porous structures. These features enhance CO2 and H2 adsorption, promote long-chain hydrocarbon growth, and achieve high CO2 conversion with superior preferential multi-carbon product selectivity and lower undesired C1 selectivity. Our catalytic system features a high degree of graphitization, an additional carbon source that enhances the dispersion of metal particles within the carbon matrix, a unique pore geometry that ensures rapid diffusion, and suitable K and N promoters acting as effective electron donors to influence CO2 dissociation and carbon-carbon coupling.

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Linking catalyst synthesis strategies to CO₂-modified Fischer-Tropsch performance in iron-carbon systems

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