Innovative biogas reforming in catalytic membrane reactor for CO-free green hydrogen production with carbon capture
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An innovative strategy for one-step CO-free H2 production from biogas was proposed.
The Ce0.8Sm0.15Ni0.05O2-δ catalytic layer was compatible with the ceramic membrane.
An accumulative production rate of 10.35 mL min-1 cm-2 of CO-free H2 was achieved.
A remarkably high hydrogen yield of 94.5% was achieved.
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ABSTRACT
Biogas reforming is an attractive process for green hydrogen production; however, CO residual in the obtained hydrogen is usually eliminated by multiple post-treatment units. Herein, we report an innovative route by coupling water splitting with biogas reforming in a catalytic membrane reactor to directly produce CO-free H2 and capture CO2 on opposite sides of the membrane. Notably, a hollow fiber composite membrane consisting of doped ceria and perovskite is employed, integrated with porous catalytic layer Ce0.8Sm0.15Ni0.05O2-δ over which Ni nanoparticles can be in-situ exsolved. The catalytic layer's compatibility with the ceramic membrane ensures low ionic resistance and effective reaction-diffusion synergy. An accumulative production rate of 10.35 mL min-1 cm-2 of CO-free H2 was achieved from water splitting on the core side, while biogas reforming produced CO2 on the opposite side which was ready for capture. This work provides an alternative option for utilizing sustainable bioenergy to produce negative-emissions green hydrogen. -
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REFERENCES
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Liu M., Hu T., Zhang Y., et al. (2025). Innovative biogas reforming in catalytic membrane reactor for CO-free green hydrogen production with carbon capture. The Innovation Energy 2:100119. https://doi.org/10.59717/j.xinn-energy.2025.100119
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Liu M., Hu T., Zhang Y., et al. (2025). Innovative biogas reforming in catalytic membrane reactor for CO-free green hydrogen production with carbon capture. The Innovation Energy 2:100119. https://doi.org/10.59717/j.xinn-energy.2025.100119
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Figure 1.
Schematic diagram of CO-free green hydrogen production with carbon capture in a membrane reactor by coupling water splitting with biogas reforming.
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Figure 2.
(A&B) The cross section SEM images of the CSO-Ni@CSO-SSTF catalytic membrane. (C) XRD patterns of the CSO-Ni catalyst before and after reduction pretreatment. (D) HAADF-STEM image and corresponding elemental mappings and (E) HR-TEM image of CSO-Ni after 20% H2 reduction at 800 oC for 2h. XPS spectra of the fresh and the reduced CSO-Ni catalyst. (F) Ni 2p3/2, (G) Ce 3d. (H) H2-TPR profiles of CSO-Ni catalyst and CSO support.
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Figure 3.
(A) Effects of CH4 concentration in CSO-Ni@CSO-SSTF reactor. (B) The contribution of POM and DRM to methane conversion (XCH4) in (A) calculated based on the CO2 conversion. (C) CH4-TPSR profiles of CSO-Ni catalyst. (D) The accumulative production rate of CO-free green hydrogen and accumulative selectivity of CO2 in a CSO-Ni@CSO-SSAF reactor.
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Figure 4.
Long-term stability of the CSO-Ni@CSO-SSTF or the Ni/Al2O3@CSO-SSTF by coupling water splitting with biogas reforming at 930 oC. Shell side: 1.25 mL min−1 CO2, 2.5 mL min−1 CH4 and 16.25 mL min−1 N2; Core side: 20 mL min−1 H2O and 10 mL min−1 He.
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Figure 5.
(A) The O2-TPO profiles of the spent CSO-Ni and Ni/Al2O3 catalysts after long-term stability tests. (B) XRD patterns of the outer surface of fresh and spent membranes. SEM images of the surface of the spent membranes in contact with (C) Ni/Al2O3 and (D) CSO-Ni catalysts.
