Construction of MnOx with abundant surface hydroxyl groups for efficient ozone decomposition

IF 7.2 2区 工程技术 Q1 ENGINEERING, CHEMICAL Journal of Environmental Chemical Engineering Pub Date : 2025-02-01 Epub Date: 2024-12-06 DOI:10.1016/j.jece.2024.115048
Xiao Chen , Changcheng Zhou , Chonglai Chen , Chaoqun Bian , Ying Zhou , Hanfeng Lu
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Abstract

Designing and constructing stable and high-performance catalysts for room-temperature ozone decomposition under humid conditions remains a significant challenge. Herein, we report manganese oxide (MnOx) rich in surface hydroxyl groups (-OH), synthesized through a facile three-step process combining solid-state grinding, heat treatment, and hydrothermal activation using potassium permanganate and ascorbic acid as precursors. The as-prepared catalyst (MnOx-A) demonstrated remarkable stability with 100 % ozone conversion maintained for 240 min under ≤ 50 % relative humidity (RH). Notably, it achieved 90 % ozone conversion after 240 min even under 90 % RH, surpassing its performance (79 % conversion) at 70 % RH. Through comprehensive characterization and density functional theory calculations, we revealed that the abundant surface -OH groups effectively mitigate the water-induced deactivation of MnOx during room-temperature catalytic ozone decomposition under humid conditions. Furthermore, we established a correlation between the catalytic activity of -OH groups and the manganese valence state. These findings provide valuable insights for the rational design of highly efficient and stable catalysts for practical ozone elimination applications.
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具有丰富表面羟基的MnOx的构建及高效臭氧分解
设计和构建稳定、高性能的催化剂用于潮湿条件下的室温臭氧分解仍然是一个重大挑战。在此,我们报道了富含表面羟基(-OH)的氧化锰(MnOx),以高锰酸钾和抗坏血酸为前体,通过简单的三步工艺,结合固态研磨、热处理和水热活化合成。制备的催化剂(MnOx-A)在≤ 50 %的相对湿度(RH)下,臭氧转化率保持在100 %,持续240 min。值得注意的是,即使在90 % RH下,它在240 min后也达到了90 %的臭氧转化率,超过了它在70 % RH下的性能(79 %的转化率)。通过综合表征和密度泛函理论计算,我们发现丰富的表面-OH基团有效地缓解了潮湿条件下室温催化臭氧分解过程中MnOx的水致失活。此外,我们还建立了-OH基团的催化活性与锰价态之间的相关性。这些发现为合理设计高效稳定的臭氧消除催化剂提供了有价值的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Journal of Environmental Chemical Engineering
Journal of Environmental Chemical Engineering Environmental Science-Pollution
CiteScore
11.40
自引率
6.50%
发文量
2017
审稿时长
27 days
期刊介绍: The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.
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