物理化学学报 >> 2026, Vol. 42 >> Issue (5): 100234.doi: 10.1016/j.actphy.2025.100234

论文 上一篇    

碳球上碱金属氧化物的界面稳定化用于高性能CO2化学吸附

赵非凡1, 徐飞燕1,2,*(), 余家国1,*()   

  1. 1 中国地质大学(武汉)材料与化学学院太阳能燃料实验室, 湖北 武汉 430078
    2 Instituto Universitario de Tecnología Química, CSIC-UPV, Universitat Polite?cnica de Vale?ncia, Valencia 46022, Spain
  • 收稿日期:2025-12-12 修回日期:2025-12-22 录用日期:2025-12-23 发布日期:2026-01-23
  • 通讯作者: Email: xufeiyan@cug.edu.cn (徐飞燕)yujiaguo93@cug.edu.cn (余家国)

Interfacial stabilization of alkali metal oxides on carbon spheres for high-performance CO2 chemisorption

Feifan Zhao1, Feiyan Xu1,2,*(), Jiaguo Yu1,*()   

  1. 1 Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei Province, China
    2 Instituto Universitario de Tecnología Química, CSIC-UPV, Universitat Polite?cnica de Vale?ncia, Valencia 46022, Spain
  • Received:2025-12-12 Revised:2025-12-22 Accepted:2025-12-23 Published:2026-01-23
  • Contact: Email: xufeiyan@cug.edu.cn (Feiyan Xu)yujiaguo93@cug.edu.cn (Jiaguo Yu)

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摘要：

高效捕集低浓度二氧化碳(CO2)需要兼具强反应活性与长期结构稳定性的化学吸附剂。碱金属氧化物虽具潜力，但存在快速烧结问题，会严重减少可接触活性位点。本研究开发了一种普适性界面策略，将Li2O、Na2O和K2O以高度分散的非晶态域形式锚定于空心碳球(分别命名为Li-HCS、Na-HCS和K-HCS)，形成稳定的M–O–C键合位点。这种界面结构既可阻止氧化物迁移，又能增强表面碱性，显著强化CO2结合能力。在碱金属负载空心碳球中，K-HCS表现出最优异的CO2吸附容量(273 K、1 bar (1 bar = 105 Pa)条件下4.9 mmol g−1)、最快吸附动力学(313 K、1 bar条件下13.56 mol kg−1 h−1)，以及最佳低压脱除效率(273 K、0.15 bar条件下44%)。密度泛函理论计算进一步揭示，随着电子给体能力与极化率从Li到Na再到K的增强，其吸附强度与分子活化能呈现单调递增规律。该研究为稳定碱金属氧化物提供了普适性方案，并为发展低压CO2捕集材料提供了机理层面的新见解。

关键词: 碱金属氧化物, 空心碳球, 二氧化碳化学吸附, 低浓度二氧化碳捕集, 烟气净化

Abstract:

Efficient capture of low-concentration carbon dioxide (CO2) requires chemisorbents that couple strong reactivity with long-term structural stability. Alkali metal oxides are promising candidates but suffer from rapid sintering that severely reduces accessible active sites. Here we develop a universal interfacial strategy that immobilizes Li2O, Na2O, and K2O as highly dispersed amorphous domains on hollow carbon spheres (named Li-HCS, Na-HCS, and K-HCS) forming robust M–O–C anchor sites. These interfacial structures prevent oxide migration, enhance surface basicity, and significantly strengthen CO2 binding. Among the alkali metal-loaded hollow carbon spheres, K-HCS exhibits the highest CO2 uptake (4.9 mmol g−1 at 273 K and 1bar), fastest adsorption kinetics (13.56 mol kg−1 h−1 at 313 K and 1bar), and optimal low-pressure removal efficiency (44% at 273 K and 0.15 bar). Density functional theory calculations further reveal a monotonic increase in adsorption strength and molecular activation from Li to Na to K, driven by enhanced electron donation and polarizability. This work establishes a broadly applicable route for stabilizing alkali metal oxides and provides mechanistic insights for advancing low-pressure CO2 capture materials.

Key words: Alkali metal oxides, Hollow carbon spheres, CO2 chemisorption, Low-concentration CO2 capture, Flue gas purification