通过原位 L-T 转变构建的花状多晶氧化锰在潮湿条件下催化臭氧氧化二甲基硫醚时性能卓越

IF 7.4 Q1 ENGINEERING, ENVIRONMENTAL ACS ES&T engineering Pub Date : 2024-09-05 DOI:10.1021/acsestengg.4c00404
Feiyang He, Wenji Feng, Xinru Chen, Yunshuo Wu, Haiqiang Wang, Zhongbiao Wu
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引用次数: 0

摘要

为了提高氧化锰(MnOx)在潮湿条件下催化臭氧氧化二甲基硫醚(DMS)时的耐水性,研究人员参考了自然环境中矿物的原位层-隧道(L-T)转变,在δ-MnO2 的基础上合成了多晶态氧化锰(MnOx)。所构建的多晶态 MnOx(Mn-SH)具有丰富的α-δ(α(Mn)-O-δ(Mn))界面,对 DMS 的转化表现出卓越的催化活性,在苛刻条件[相对湿度 (RH) = 80%]下可确保 DMS 的去除率超过 91%,并且在测试 20 小时(相对湿度 = 60-80%)后具有极佳的稳定性。原位 DRIFTS 光谱和理论计算表明,α-δ 界面有利于通过 H2O 离解形成活性羟基 (-OH),从而参与臭氧 (O3) 激活,避免 H2O 导致的失活。同时,通过 H2O 解离形成了更多的布氏酸位点,从而促进了 DMS 的吸附和分解。这项研究让人们了解了 α-δ 界面在促进催化臭氧活性方面的作用,并为构建具有更强耐水性的多晶态氧化锰提供了一种简便的策略,这种策略可应用于现有的氧化锰,用于催化氧化畜牧场和石油工业中的含硫化合物。
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Flower-like Polymorphic MnOx Constructed by In Situ L–T Transition with Superior Performance in the Catalytic Ozonation of Dimethyl Sulfide under Humid Conditions
To improve the water resistance of manganese oxide (MnOx) in the catalytic ozonation of dimethyl sulfide (DMS) under humid conditions, polymorphic MnOx was synthesized based on δ-MnO2 with reference to the in situ layer-to-tunnel (L–T) transition of minerals in a natural environment. The constructed polymorphic MnOx(Mn–SH) possessed abundant α–δ (α(Mn)-O-δ(Mn)) interfaces and exhibited superior catalytic activity for the conversion of DMS, ensuring more than 91% of DMS removal under harsh conditions [relative humidity (RH) = 80%] and excellent stability after testing for 20 h (RH = 60–80%). In situ DRIFTS spectra and theoretical calculations demonstrated that α–δ interfaces facilitated the formation of active hydroxyl groups (−OH) through H2O dissociation, which can participate in ozone (O3) activation and avoid the deactivation caused by H2O. Simultaneously, more Brønsted acid sites formed through H2O dissociation, which promoted DMS adsorption and decomposition. This study gives an understanding of the role of α–δ interfaces in promoting activity for catalytic ozonation and provides a convenient strategy to construct polymorphic MnOx with enhanced water resistance, which can be applied to existing MnOx used for catalytic ozonation of sulfur-containing compounds from livestock farms and the petroleum industries.
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ACS ES&T engineering
ACS ES&T engineering ENGINEERING, ENVIRONMENTAL-
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期刊介绍: ACS ES&T Engineering publishes impactful research and review articles across all realms of environmental technology and engineering, employing a rigorous peer-review process. As a specialized journal, it aims to provide an international platform for research and innovation, inviting contributions on materials technologies, processes, data analytics, and engineering systems that can effectively manage, protect, and remediate air, water, and soil quality, as well as treat wastes and recover resources. The journal encourages research that supports informed decision-making within complex engineered systems and is grounded in mechanistic science and analytics, describing intricate environmental engineering systems. It considers papers presenting novel advancements, spanning from laboratory discovery to field-based application. However, case or demonstration studies lacking significant scientific advancements and technological innovations are not within its scope. Contributions containing experimental and/or theoretical methods, rooted in engineering principles and integrated with knowledge from other disciplines, are welcomed.
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