通过a位取代优化mn基高熵钙钛矿氧化物对挥发性有机化合物的增强催化氧化

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-09-12 DOI:10.1016/j.apcata.2025.120566

Tiantian Qi, Weidong Zhang, Jingchong Yan, Zhanku Li, Shigang Kang, Shibiao Ren, Zhiping Lei, Zhicai Wang, Hengfu Shui

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引用次数: 0

摘要

开发具有优异低温活性、稳定性和成本效益的高效VOCs减排催化剂仍然是一个挑战。本研究采用蔗糖溶胶-凝胶法制备了新型a位取代mn基高熵钙钛矿氧化物（标称成分：RE0.8Mg0.05Ca0.05Sr0.05Ba0.05MnO3, RE = La, Nd, Sm），并评价了其对代表性VOCs、丙烷和甲苯的总氧化性能。表征结果表明，用Nd （NdMn-HEO）取代a位后，晶格畸变最大，Mn−O键强度最弱，比表面积最大（31.5 m2 g−1），氧空位浓度最高，Mn4+/Mn3+比最大，低温还原性好。结果表明，NdMn-HEPO表现出最佳活性（对丙烷T90 = 311℃，对甲苯T90 = 236℃），优于lam - heo和SmMn-HEO。这种性能的增强是由于多组分a位元素的协同作用，促进了晶格畸变、氧空位的形成和氧化还原性能的优化。此外，NdMn-HEO在丙烷氧化中表现出优异的稳定性和耐久性，在4个循环和22 h的连续测试后保持高活性。该催化剂还表现出良好的适应性，高WHSV，优异的耐水性和强的抗硫性（活性损失最小，ΔT90 = 5°C），突出了其工业应用潜力。高熵钙钛矿的a位点工程优化了活性位点环境，为设计实用的VOCs氧化催化剂提供了强有力的策略。

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Optimizing Mn-based high-entropy perovskite oxides via A-site substitution for enhanced catalytic oxidation of VOCs

Developing efficient catalysts for VOCs abatement with superior low-temperature activity, stability, and cost-effectiveness remains challenging. This study synthesized novel Mn-based high-entropy perovskite oxides with A-site substitution (nominal composition: RE_0.8Mg_0.05Ca_0.05Sr_0.05Ba_0.05MnO₃, RE = La, Nd, Sm) via sucrose sol-gel method and evaluated their performance for total oxidation of representative VOCs, propane and toluene. Characterization results show that substituting the A-site with Nd (NdMn-HEO) induced the highest lattice distortion, the weakest Mn−O bond strength, the largest specific surface area (31.5 m² g⁻¹), the highest oxygen vacancy concentration, the greatest Mn⁴⁺/Mn³⁺ ratio, and superior low-temperature reducibility. As a result, NdMn-HEPO exhibits optimal activity (T₉₀ = 311°C for propane; 236°C for toluene), surpassing LaMn-HEO and SmMn-HEO. This performance enhancement is attributed to the synergistic effect of multi-component A-site elements, which promotes lattice distortion, oxygen vacancy formation, and optimization of redox properties. Furthermore, NdMn-HEO demonstrates excellent stability and durability in propane oxidation, maintaining high activity after four cycles and 22 h of continuous testing. The catalyst also shows good adaptability high WHSV, excellent water resistance, and strong sulfur resistance (minimal activity loss, ΔT₉₀ = 5°C), highlighting its potential for industrial applications. A-site engineering in high-entropy perovskites optimizes active-site environments, offering a robust strategy for designing practical VOCs oxidation catalysts.

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.