近日，课题组博士生刘森论文“High-throughput computational screening of functionalized MOFs for energy-efficient CO₂ capture: balancing selective CO₂ adsorption performance and energy inputs”被Journal of Energy Chemistry（2025中科院SCI一区TOP，IF=14.9）接收！

Abstract

The rational design of high-performance CO₂ adsorbents  remains a critical challenge in addressing global carbon emissions, with  metal-organic frameworks (MOFs) emerging as promising candidates due to  their tunable pore environments. However, the lack of systematic  guidelines for functional group selection has hindered their practical  implementation in carbon capture applications. Here, this gap was  addressed by developing a comprehensive design framework through  high-throughput computational screening. Through construction of a  topology-directed database of 4797, integrating 10 metal centers with  144 functionalized ligands (18 ligands modified by –NH₂, –NO₂, –CH₃, –CF₃, –SH₂, –SO₂, –OH, and –OLi) across 36 topologies, the fundamental structure-property relationships governing CO₂ capture performance was established. Multi-metric evaluation reveals that –NO₂, –SO₂, and –OLi dramatically enhance CO₂ selectivity over CH₄/N₂ via selectivity (S_ads), working capacity (ΔN), adsorbent performance score (APS), sorbent selection parameter (S_sp), and renewability R. Specially, ΔN rises from 2.34 (pristine) to 5.91–7.94 mmol g⁻¹ and S_ads surges from 24.94/40.36 to 121.11/176.87 (–NO₂), 149.94/215.54 (–SO₂),  and 58.64/267.44 (–OLi). Besides, the critical trade-off between  adsorption strength and renewability demonstrates that enhanced  performance comes at the cost of reduced renewability, where stronger CO₂ affinity (isosteric heat of −29.15, −29.96, and −30.09 for –NO₂, –SO₂, and –OLi) compromises renewability (R reduced by ∼50%). To resolve this trade-off, a novel energy efficiency (η) metric was introduced, which holistically evaluates both adsorption performance (S_ads, ΔN, APS, S_sp, and R) and energy inputs (desorption heat, pressure-swing energy, net loss). This leads to the identification of –SO₂ as the optimal functional group that balances exceptional CO₂ capture (η = 6.17/12.78 for CO₂ over CH₄/N₂), surpassing the second higher of 4.74/8.80 in –CF₃  and 0.99/2.18 in non-functionalized counterparts. Adopting  high-throughput computational screening methods, this work provides both  fundamental insights into host-guest interactions in functionalized  MOFs and a practical framework for designing next-generation adsorbents,  bridging the gap between materials discovery and process engineering  considerations in carbon capture technologies.

https://doi.org/10.1016/j.jechem.2025.09.070