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OA
Interfacial stabilization of alkali metal oxides on carbon spheres for high-performance CO2 chemisorption
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.
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.
赵非凡;徐飞燕;余家国
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||Instituto Universitario de Tecnología Química,CSIC-UPV,Universitat Politècnica de València,Valencia 46022,Spain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
化学化工
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
Alkali metal oxidesHollow carbon spheresCO2 chemisorptionLow-concentration CO2 captureFlue gas purification
《物理化学学报》 2026 (5)
152-164,13
国家重点研发计划(2022YFE0115900)国家自然科学基金(22238009,22378371,U23A20102和22361142704)以及湖北省自然科学基金(2022CFA001和2023AFA088).
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