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<p>Selective dinitrogen (N<sub>2</sub>) capture from coalbed methane (CBM) is significant in chemical industries, but it remains a challenge because of similar physicochemical properties of N<sub>2</sub> and CH<sub>4</sub>. Herein, the adsorption of them on the 2D porphyrin sheets doped with various 3d transition metal ions (marked as MPor, M=Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn) were comparatively investigated by using density functional theory to screen a suitable adsorbent for CBM separation. Though systematical comparison of adsorption energies of gas molecules and Gibbs free energy change the N<sub>2</sub> desorption process on all MPor surfaces, FePor is confirmed to be a promising adsorbent because of its undemanding regeneration conditions and modest chemical bonding state with N<sub>2</sub> molecule. Further mechanism analysis reveals that the charge transferred from lone pair of N<sub>2</sub> molecule to <i>d</i><sub><i>z</i>2</sub> orbital of Fe ion and back-donated from <i>d</i><sub><i>xz</i></sub> and <i>d</i><sub><i>yz</i></sub> orbitals of Fe ion to the unoccupied <i>π</i>* orbital of N<sub>2</sub> molecule. Such hybridization of orbitals improves the selective adsorption of N<sub>2</sub> from CBM.</p>

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Selective Dinitrogen Capture from Coalbed Methane Using 2D Porphyrin-based Sheet with 3d Transition Metal Ion Sites: A First-principles Computational Study

  • 期刊论文

  • 发表日期：

    2025年5月17日

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  • Guangping Lei,
  • Yang Lu,
  • Huiyuan Cheng

摘要

Selective dinitrogen (N2) capture from coalbed methane (CBM) is significant in chemical industries, but it remains a challenge because of similar physicochemical properties of N2 and CH4. Herein, the adsorption of them on the 2D porphyrin sheets doped with various 3d transition metal ions (marked as MPor, M=Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn) were comparatively investigated by using density functional theory to screen a suitable adsorbent for CBM separation. Though systematical comparison of adsorption energies of gas molecules and Gibbs free energy change the N2 desorption process on all MPor surfaces, FePor is confirmed to be a promising adsorbent because of its undemanding regeneration conditions and modest chemical bonding state with N2 molecule. Further mechanism analysis reveals that the charge transferred from lone pair of N2 molecule to dz2 orbital of Fe ion and back-donated from dxz and dyz orbitals of Fe ion to the unoccupied π* orbital of N2 molecule. Such hybridization of orbitals improves the selective adsorption of N2 from CBM.