碳球上碱金属氧化物的界面稳定化用于高性能CO<sub>2</sub>化学吸附

引用本文: 赵非凡, 徐飞燕, 余家国. 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[J]. 物理化学学报, 2026, 42(5): 100234. doi: 10.1016/j.actphy.2025.100234 shu

Citation: Feifan Zhao, Feiyan Xu, Jiaguo Yu. Interfacial stabilization of alkali metal oxides on carbon spheres for high-performance CO₂ chemisorption[J]. Acta Physico-Chimica Sinica, 2026, 42(5): 100234. doi: 10.1016/j.actphy.2025.100234 shu

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.
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 Politècnica de València, Valencia 46022, Spain

通讯作者: Email: xufeiyan@cug.edu.cn (徐飞燕); yujiaguo93@cug.edu.cn (余家国)

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:

English

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

Feifan Zhao ^1, ,
Feiyan Xu ^{1, 2,
,} ,
Jiaguo Yu ^{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 Politècnica de València, Valencia 46022, Spain

Corresponding author: Email: xufeiyan@cug.edu.cn (Feiyan Xu); yujiaguo93@cug.edu.cn (Jiaguo Yu)

Received Date: 12 December 2025
Accepted Date: 23 December 2025
Revised Date: 22 December 2025
Available Online: 15 May 2026

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:

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沈阳化工大学材料科学与工程学院沈阳 110142

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

通讯作者: Email: xufeiyan@cug.edu.cn (徐飞燕); yujiaguo93@cug.edu.cn (余家国)

English

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

Corresponding author: Email: xufeiyan@cug.edu.cn (Feiyan Xu); yujiaguo93@cug.edu.cn (Jiaguo Yu)

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中国化学会秘书处

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

通讯作者: Email: xufeiyan@cug.edu.cn (徐飞燕); yujiaguo93@cug.edu.cn (余家国)

English

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

Corresponding author: Email: xufeiyan@cug.edu.cn (Feiyan Xu); yujiaguo93@cug.edu.cn (Jiaguo Yu)

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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

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

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs