{"title":"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","authors":"Feiyang He, Wenji Feng, Xinru Chen, Yunshuo Wu, Haiqiang Wang, Zhongbiao Wu","doi":"10.1021/acsestengg.4c00404","DOIUrl":null,"url":null,"abstract":"To improve the water resistance of manganese oxide (MnO<sub><i>x</i></sub>) in the catalytic ozonation of dimethyl sulfide (DMS) under humid conditions, polymorphic MnO<sub><i>x</i></sub> was synthesized based on δ-MnO<sub>2</sub> with reference to the in situ layer-to-tunnel (L–T) transition of minerals in a natural environment. The constructed polymorphic MnO<sub><i>x</i></sub>(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 H<sub>2</sub>O dissociation, which can participate in ozone (O<sub>3</sub>) activation and avoid the deactivation caused by H<sub>2</sub>O. Simultaneously, more Brønsted acid sites formed through H<sub>2</sub>O 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 MnO<sub><i>x</i></sub> with enhanced water resistance, which can be applied to existing MnO<sub><i>x</i></sub> used for catalytic ozonation of sulfur-containing compounds from livestock farms and the petroleum industries.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4000,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Flower-like Polymorphic MnOx Constructed by In Situ L–T Transition with Superior Performance in the Catalytic Ozonation of Dimethyl Sulfide under Humid Conditions\",\"authors\":\"Feiyang He, Wenji Feng, Xinru Chen, Yunshuo Wu, Haiqiang Wang, Zhongbiao Wu\",\"doi\":\"10.1021/acsestengg.4c00404\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"To improve the water resistance of manganese oxide (MnO<sub><i>x</i></sub>) in the catalytic ozonation of dimethyl sulfide (DMS) under humid conditions, polymorphic MnO<sub><i>x</i></sub> was synthesized based on δ-MnO<sub>2</sub> with reference to the in situ layer-to-tunnel (L–T) transition of minerals in a natural environment. The constructed polymorphic MnO<sub><i>x</i></sub>(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 H<sub>2</sub>O dissociation, which can participate in ozone (O<sub>3</sub>) activation and avoid the deactivation caused by H<sub>2</sub>O. Simultaneously, more Brønsted acid sites formed through H<sub>2</sub>O 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 MnO<sub><i>x</i></sub> with enhanced water resistance, which can be applied to existing MnO<sub><i>x</i></sub> used for catalytic ozonation of sulfur-containing compounds from livestock farms and the petroleum industries.\",\"PeriodicalId\":7008,\"journal\":{\"name\":\"ACS ES&T engineering\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.4000,\"publicationDate\":\"2024-09-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS ES&T engineering\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1021/acsestengg.4c00404\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS ES&T engineering","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1021/acsestengg.4c00404","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
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.
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.