Study on CO<sub>2</sub> Adsorption Properties and DFT Mechanism of Sulfur-resistant Potassium-based Adsorbents

Yanhong LI; Baihe GUO; Ruibin SUN; Yilin SHI; Kaixuan GAO; Xiaolei QIAO; Yan JIN

doi:10.13334/j.0258-8013.pcsee.232567

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Study on CO₂ Adsorption Properties and DFT Mechanism of Sulfur-resistant Potassium-based Adsorbents

Power Generation | 更新时间：2026-02-06

- Study on CO₂ Adsorption Properties and DFT Mechanism of Sulfur-resistant Potassium-based Adsorbents
- Proceedings of the CSEE Vol. 45, Issue 10, Pages: 3934-3945(2025)
- 作者机构：
  
  1. 太原理工大学电气与动力工程学院, 山西省太原市 030024
  2. 天津大学机械工程学院, 天津市南开区 300301
- 作者简介：
- 基金信息：
  
  Project Supported by Natural Science Foundation of Shanxi Province(202103021223076)
- DOI：10.13334/j.0258-8013.pcsee.232567
  CLC： X773
- Received：22 November 2023，
  
  Online First：28 February 2024，
  
  Published：20 May 2025
- 稿件说明：
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Yanhong LI, Baihe GUO, Ruibin SUN, et al. Study on CO₂ Adsorption Properties and DFT Mechanism of Sulfur-resistant Potassium-based Adsorbents[J]. Proceedings of the CSEE, 2025, 45(10): 3934-3945.
DOI：

Yanhong LI, Baihe GUO, Ruibin SUN, et al. Study on CO₂ Adsorption Properties and DFT Mechanism of Sulfur-resistant Potassium-based Adsorbents[J]. Proceedings of the CSEE, 2025, 45(10): 3934-3945. DOI： 10.13334/j.0258-8013.pcsee.232567.

摘要

燃煤电厂经脱硫脱硝后存在的痕量SO

会导致钾基吸附剂失效。该文采用溶胶-凝胶法制备气凝胶载体，浸渍法掺杂MnO

制备改性钾基吸附剂，借助固定床脱碳试验系统，在不同条件下对吸附剂进行脱碳试验。利用Avrami吸附动力学模型拟合，并结合表征手段对吸附剂孔隙、物相组成和微观形貌进行分析，基于密度泛函理论(density functional theory，DFT)深入探究Mn掺杂改性吸附剂抗硫机理。结果表明：在含150 mg/m

气氛中，MnO

与SO

反应生成MnSO

，减少SO

与K

反应，CO

吸附量提升29.7%，吸附剂有一定的抗硫性。MnO

最佳掺杂量为2.5%，最佳吸附条件为CO

浓度12.5%，反应温度为60℃，H

O浓度为15%。SO

在吸附剂表面的吸附能最大，SO

分子中S、O原子的2p轨道和Mn原子3d轨道发生共振，发生相互作用，从而有一定的抗硫作用。Mn掺杂反应能垒降低为143.71 kJ/mol，反应热增加为−164.92 kJ/mol，进而减少SO

对吸附剂脱碳性能影响。MnO

掺杂改性钾基吸附剂在含SO

气氛中表现出显著的抗硫性和较高的CO

吸附能力。

Abstract

After desulfurization and denitrification in coal-fired power plants

the trace amount of SO

can lead to the failure of potassium-based adsorbents. In this paper

aerogel

carriers are prepared by using sol-gel method

and modified potassium-based adsorbents are prepared by using the impregnation method doped with MnO

. With the help of a fixed bed decarburization experimental system

the decarburization experiments of the adsorbents are carried out under different conditions. Avrami adsorption kinetic model is used to fit

and the pore

phase composition and microscopic appearance of the adsorbents are analyzed by combining characterization methods. Based on density functional theory (DFT)

the anti-sulfur mechanism of Mn-doped modified adsorbents is explored in depth. The results show that: in an atmosphere containing 150 mg/m

MnO

reacts with SO

to form MnSO

reducing the reaction between SO

and K

and the CO

adsorption capacity is increased by 29.7%. The adsorbents have certain sulfur resistance. The optimal doping amount of MnO

is 2.5%

the optimal adsorption conditions are 12.5% CO

concentration

60℃ reaction temperature

and 15% H

O concentration. The adsorption energy of SO

on the adsorbent surface is the largest

and the 2p orbitals of S and O atoms and the 3d orbitals of Mn atom in SO

molecule resonate and interact with each other

thus having a certain anti-sulfur effect. After Mn doping

the reaction energy barrier is decreased to 143.71 kJ/mol

and the reaction heat is increased to −164.92 kJ/ mol

thereby reducing the influence of SO

on the decarburization performance of the adsorbent. MnO

-doped modified potassium-based adsorbents exhibit significant sulfur resistance and high CO

adsorption capacity in SO

-containing atmosphere.

关键词

Keywords

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Study on CO2 Adsorption Properties and DFT Mechanism of Sulfur-resistant Potassium-based Adsorbents

DOI：10.13334/j.0258-8013.pcsee.232567

摘要

Abstract

关键词

Keywords

references

Study on CO₂ Adsorption Properties and DFT Mechanism of Sulfur-resistant Potassium-based Adsorbents