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<p>The development of efficient, metal-free materials for the detoxification of chemical warfare agents remains a significant challenge. Nitrogen-doped graphene represents a promising candidate; yet, the atomistic mechanism by which specific N configurations govern the adsorption and activation of simulants like 2-chloroethyl ethyl sulfide (2-CEES) is not fully elucidated. Herein, density functional theory (DFT) calculations are employed to systematically unravel the interface electronic modulation and adsorption and electronic activation mechanism of 2-CEES on pristine and N-doped graphene (graphitic N, pyridinic N, and pyrrolic N). Our results demonstrate that nitrogen doping, particularly in the pyrrolic configuration, dramatically enhances the adsorption strength and electronic interaction with 2-CEES compared to pristine graphene. Pyrrolic N doping induces the most significant charge polarization, creates a highly complementary electrostatic interface, and facilitates strong interfacial electronic coupling and charge polarization, as evidenced by a multifaceted electronic structure analysis (DOS, PDOS, FMO, ED, and ESP). This work identifies pyrrolic N as the most potent active site for 2-CEES activation and establishes the critical role of localized electronic structure over generalized N doping. The insights provide definitive design principles for engineering high-performance, metal-free carbon materials for adsorption and potential subsequent catalytic transformation in future studies.</p> Graphical abstract <p></p>

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Interface electronic modulation of N-doped graphene and its interfacial electronic activation toward 2-chloroethyl ethyl sulfide: a DFT study

  • 期刊论文

  • 发表日期：

    2026年2月28日

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  • Beibei Lu,
  • Chen Li,
  • Zhichao Fan,
  • Xiao Fan,
  • Xinna Wang,
  • Xiaohui Ji,
  • Lingxia Jin,
  • Jinlong Lai,
  • Qian Fu,
  • Minjuan Zhao

摘要

The development of efficient, metal-free materials for the detoxification of chemical warfare agents remains a significant challenge. Nitrogen-doped graphene represents a promising candidate; yet, the atomistic mechanism by which specific N configurations govern the adsorption and activation of simulants like 2-chloroethyl ethyl sulfide (2-CEES) is not fully elucidated. Herein, density functional theory (DFT) calculations are employed to systematically unravel the interface electronic modulation and adsorption and electronic activation mechanism of 2-CEES on pristine and N-doped graphene (graphitic N, pyridinic N, and pyrrolic N). Our results demonstrate that nitrogen doping, particularly in the pyrrolic configuration, dramatically enhances the adsorption strength and electronic interaction with 2-CEES compared to pristine graphene. Pyrrolic N doping induces the most significant charge polarization, creates a highly complementary electrostatic interface, and facilitates strong interfacial electronic coupling and charge polarization, as evidenced by a multifaceted electronic structure analysis (DOS, PDOS, FMO, ED, and ESP). This work identifies pyrrolic N as the most potent active site for 2-CEES activation and establishes the critical role of localized electronic structure over generalized N doping. The insights provide definitive design principles for engineering high-performance, metal-free carbon materials for adsorption and potential subsequent catalytic transformation in future studies.

Graphical abstract