中南大学
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返回首页Sulfhydryl-Mediated Thermal Stabilization of Nitrogen Adsorption Sites in Aromatic Heterocyclic Waste-Derived Activated Carbon for Enhanced CO2 Capture
发布时间：2025-09-29
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- DOI码：
- 10.1002/adfm.202522953
- 发表刊物：
- Advanced Functional Materials
- 关键字：
- CO2 adsorption, porous carbon, reaction mechanism, sulfhydryl modification, thermal stability
- 摘要：
- Thermally unstable nitrogen sites impede the synthesis of porous carbons with balanced porosity and surface chemistry for efficient CO2 capture. Using benzimidazole as a model system, this work examines the viability of molecular engineering approaches to improve the thermal stability of aromatic heterocyclic waste materials under high-temperature activation conditions. By integrating machine learning-guided feature importance analysis, nitrogen content quantification, and bond dissociation energy calculations, we identify N-doping percentage as the critical determinant of CO2 adsorption capacity and reveal that sulfhydryl-substituted benzimidazole exhibits higher thermal stability of nitrogen adsorption sites. This modification strengthens intramolecular bonding within the Imidazole ring. The sulfhydryl-functionalized precursor retained a high nitrogen content of 9.66 at% even at 700 °C, resulting in the derived NS700 material achieving a CO2 adsorption capacity of 5.48 mmol g−1 at 25 °C and 1 bar, which is 65% higher than its unmodified counterpart. Comparative analysis of nitrogen content in four base molecules and their sulfhydryl-substituted derivatives, combined with molecular dynamics simulations and HOMO-LUMO gap calculations, visually demonstrates that sulfhydryl substitution enhances thermal stability during high-temperature activation for activated carbon production, thereby improving nitrogen retention rates. This work establishes that molecular structure design optimizes activated carbon preparation from aromatic heterocyclic waste.
- 论文类型：
- 期刊论文
- 论文编号：
- e22953
- 是否译文：
- 否
- 发表时间：
- 2025-09-22
- 收录刊物：
- SCI
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