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논문 해외 국제전문학술지(SCI급) Fine tuning of Co3O4-encapsulated mesoporous silica as the core@shell bifunctional catalyst toward efficient CH4 carboxylation using CO2 to CH3COOH

  • 학술지 구분 국제전문학술지(SCI급)
  • 게재년월 2026-08
  • 저자명 Yang, H., Kwon, S., Lee, W., Lim, G., Kim, J.-C.*, and Na, K.*
  • 학술지명 Journal of CO2 Utilization
  • 발행처명 ELSEVIER
  • 발행국가 해외
  • 논문언어 외국어
  • 전체저자수 6
  • 논문 다운로드 링크(외부) https://www.sciencedirect.com/science/article/pii/S2212982026001952
  • 연구분야 공학 > 화학공학

논문 초록 (Abstract)

Recently, it was reported that CO2 can serve as a carboxylating agent for the selective conversion of CH4 into CH3COOH using Co3O4 as a bifunctional catalyst. However, despite the sequential activation of both reactants, the practical CH3COOH productivity remained insufficient for industrial applications. Herein, a series of Co3O4-encapsulated mesoporous silica catalysts (denoted as Co3O4@mSiO2) were synthesized. These bifunctional core@shell architectures featured precisely tuned core diameters and shell thicknesses, achieved by systematic control of the precursor ratios. TEM and XRD analyses confirmed the successful encapsulation of nanocrystalline Co3O4 within the mesoporous silica framework, with dimensions ranging from 4.7–18.8 nm (core) and 16.9–60.1 nm (shell). Catalytic evaluations revealed that the CH3COOH yield is governed by a synergistic interplay between the core and shell dimensions. Specifically, the optimized architecture (9.9 nm core and 24.4 nm shell) delivered a peak yield of 194.2 μmol gCo3O4−1, significantly outperforming counterparts with smaller cores or thinner shells. Ex situ FT-IR spectroscopy elucidated that this optimal configuration maximized CO2 activation as surface carbonate species, facilitating the subsequent reaction with CH4. Furthermore, the mesoporous silica shell effectively suppressed sintering, ensuring structural integrity and stable performance over 10 consecutive reaction cycles.