Multiscale analysis of CO2 adsorption mechanisms on porous carbon: An investigation into the impact of intrinsic defects and pore size

Mingqi He; Haiqian Zhao; Jiuyang Jia; Wei Zhou; Zhonghua Wang; Kaibo An; Yiyang Jiao; Xue Yang; Xiaolong Zhang; Tianhang Fan

doi:10.1016/j.envres.2024.120701

Multiscale analysis of CO₂ adsorption mechanisms on porous carbon: An investigation into the impact of intrinsic defects and pore size

Environ Res. 2024 Dec 25:267:120701. doi: 10.1016/j.envres.2024.120701. Online ahead of print.

Authors

Mingqi He¹, Haiqian Zhao², Jiuyang Jia³, Wei Zhou⁴, Zhonghua Wang⁵, Kaibo An⁶, Yiyang Jiao⁴, Xue Yang⁷, Xiaolong Zhang¹, Tianhang Fan¹

Affiliations

¹ School of Mechanical Science and Engineering, Northeast Petroleum University, Daqing, 163318, China.
² School of Environmental Science and Engineering, Suzhou University of Science and Technology, Suzhou, 215009, China. Electronic address: dqzhaohaiqian@163.com.
³ School of Energy and Environment, Southeast University, Nanjing, 210096, China.
⁴ School of Energy Science and Engineering, Harbin Institute of Technology, Harbin, 150001, China.
⁵ School of Civil and Architectural Engineering, Northeast Petroleum University, Daqing, 163318, China.
⁶ Key Laboratory of Thermo-Fluid Science and Engineering of MOE, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an, 710049, China.
⁷ College of New Energy & Materials, Northeast Petroleum University, Daqing, 163318, China.

PMID: 39730042
DOI: 10.1016/j.envres.2024.120701

Abstract

Porous carbon adsorption represents a critical component of CCUS technologies, with microporous structures playing an essential role in CO₂ capture. The preparation of porous carbon introduces intrinsic defects, making it essential to consider both pore size and these defects for a comprehensive understanding of the CO₂ adsorption mechanism. This study investigates the mechanisms of CO₂ adsorption influenced by intrinsic defects and pore size using multiscale methods, incorporating experimental validation, Grand Canonical Monte Carlo simulations, and Density Functional Theory simulations. Intrinsic defects increase structural disorder and microporous content in porous carbon by distorting the graphene framework, thereby creating additional spaces for CO₂ adsorption. Moreover, atomic charge redistribution induced by intrinsic defects disrupts the balance of van der Waals and electrostatic potentials, generating more active adsorption sites and enhancing the strength of CO₂ adsorption. This research aims to clarify the facilitative mechanisms of intrinsic defects and pore size on CO₂ adsorption in porous carbons and to provide a theoretical basis for designing efficient carbon-based adsorbents.

Keywords: CO(2) capture; Micropore; Stone-wales defects; Structural distortion; Vacancy defect.