Enhanced CO2 hydrogenation to heavy hydrocarbons through diffusion-limited intermediate enrichment: Semi-open vs. open systems

doi:10.1016/S1872-2067(26)65161-3

Abstract

Abstract:

Precisely tuning the nanoconfined microenvironment to optimize heterogeneous catalytic reaction pathways represents one of the critical challenges for achieving efficient and directional CO₂ conversion. In this study, we systematically investigated the impact of confinement dimensions on CO₂ hydrogenation performance by constructing a series of semi-open porous carbon spheres (MPCS_x) with tunable pore sizes (x = 0, 10, 14, 30, 100 nm) supported CoFe alloy catalysts. Experimental results revealed that the catalyst Fe₁₀Co₂@MPCS₁₄ with a pore size of 14 nm exhibits C₅₊ selectivity was twice that of open systems. To gain deeper insights into the structural origins of this optimal performance, we further elucidated the underlying microscopic mechanisms by combining Finite element method simulation with in-situ diffuse reflectance Fourier transform infrared spectroscopy. The 14 nm semi-open structure established a unique “enrichment-diffusion” dynamic equilibrium around the active sites, which not only substantially enhanced the local concentrations of CO₂/H₂ but also effectively stabilized key C1 intermediates such as HCOO^*, HCO₃^*, and CO₃^*. thereby promoting C-C coupling and carbon chain growth. This work provides important mechanistic insights into the regulation of selectivity in heterogeneous catalytic reactions through spatial confinement microenvironment modulation.

Key words: CO₂ hydrogenation, Nanopore domain, Semi-open system, CoFe alloy, Self-assembly

Lisheng Guo, Liru Zheng, Xinyu Zhang, Xin Wang, Jie Cheng, Mengdie Cai, Na Liu, Kaige Wang, Youfeng Tian, Jie Li, Song Sun. Enhanced CO₂ hydrogenation to heavy hydrocarbons through diffusion-limited intermediate enrichment: Semi-open vs. open systems[J]. Chinese Journal of Catalysis, 2027, 92: 300-315.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65161-3

https://www.cjcatal.com/EN/Y2027/V92/I1/300

Figures/Tables 6

Fig. 1. FEMS results of the concentration and distribution of CO2 and C1-C3 species on Fe10Co2@MPCS0 (A), Fe10Co2@MPCS10 (B), Fe10Co2@MPCS14 (C), and Fe10Co2@MPCS30 (D).

Fig. 2. (A) Schematic diagram of solvent-mediated PISA strategy for synthesizing porous carbon spheres and subsequent active metal site anchoring. (B-K) SEM images of MPCS0, MPCS10, MPCS14, MPCS30 and MPCS100.

Fig. 3. (A,B) SEM images of fresh Fe10Co2@MPCS14 and Fe10Co2@MPCS0. TEM image (C) and corresponding EDS elemental maps (D-H) of the fresh Fe10Co2@MPCS14. (I) XRD patterns of the fresh catalysts. (J) XRD patterns of the spent catalysts. (K) Raman spectra of the spent catalysts. Fe 2p (L) and Co 2p (M) XPS spectra of spent catalysts. (N) 57Fe Mössbauer spectra of spent MPCS0 and MPCS14. For clarity, the Fe10Co2@MPCSx samples are denoted simply as MPCSx (where x = 0, 10, 14, 30, 100). Unless specified otherwise, MPCSx refers to the Fe-based catalysts supported on porous spherical carbon.

Fig. 4. Coordination environment analysis of spent catalyst. Normalized XANES spectra of the spent catalyst at Fe K-edge (A) and Co K-edge (C). k3-weighted Fourier transformed EXAFS spectra of spent catalyst (B) and (D). (E-H) Wavelet transform spectra of the catalysts.

Fig. 5. (A) STY values of C5+ over different catalysts. (B) Catalytic performances of the Fe10Co2@MPCSx catalysts. (C) Chain growth factor α of different catalysts. (D,E) Catalytic performances over different catalysts. (F) The catalytic performance of the Fe10Co2@MPCS14 catalyst under different reaction temperatures (with all other conditions kept consistent). (G) The long-term experimental performance plot of the Fe10Co2@MPCS14 catalyst over 100 h of reaction. Reaction conditions: weight of catalyst = 0.25 g, 2.0 MPa, 320 °C, 4800 mL/(g·h), H2/CO2 = 3, TOS = 100 h. To simplify the presentation, the Fe10Co2@MPCSx shown in the Fig. is uniformly named as MPCSx (where x = 0, 10, 14, 30, 100). Unless otherwise specified, MPCSx consistently refers in this Fig. to the iron catalysts supported on porous spherical carbon.

Fig. 6. The in-situ DRIFTS spectra of Fe10Co2@MPCS0 (A) and Fe10Co2@MPCS14 (B). (C) Proposed reaction pathways for the directional synthesis of different hydrocarbons from CO2 hydrogenation over different catalysts.

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Enhanced CO₂ hydrogenation to heavy hydrocarbons through diffusion-limited intermediate enrichment: Semi-open vs. open systems

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