{"title":"在中硼酸盐工程层状多孔钯/SSZ-13 沸石上催化甲烷减排","authors":"Gaozhou Liang, Anqi Guo, Wuwan Xiong, Dongdong Chen, Ulrich Simon, Daiqi Ye, Haibao Huang, Peirong Chen","doi":"10.1021/acsestengg.4c00347","DOIUrl":null,"url":null,"abstract":"Palladium-zeolites are active catalysts for abating methane (CH<sub>4</sub>), the second largest greenhouse gas contributing to climate change, via catalytic combustion. Yet, it remains challenging to improve the activity of Pd-zeolites in CH<sub>4</sub> combustion, in particular under humid conditions. Here, using small-pore SSZ-13 zeolite as a showcase, we demonstrate mesoporosity engineering as an effective approach to boost the CH<sub>4</sub> combustion performance of Pd-zeolites. A newly designed gemini quaternary ammonium surfactant, namely C<sub>18–4</sub>N<sub>2</sub>MP, was fabricated using inexpensive reagents and employed as a mesoporogen in the hydrothermal synthesis of hierarchically micro–meso–macro–porous SSZ-13 product. High-dispersion Pd catalysts were achieved by using the hierarchically porous SSZ-13 zeolites as supports. Physicochemical characterization and reaction kinetics disclosed that rational mesoporosity engineering of the hierarchically porous SSZ-13, simply by optimizing C<sub>18–4</sub>N<sub>2</sub>MP addition in the precursor gel prior to hydrothermal crystallization, favored the formation of highly dispersed PdO<i><sub>x</sub></i> active phase and, in turn, the CH<sub>4</sub> combustion without noticeable accumulation of carbonaceous intermediates on the surface. Additionally, mesoporosity-optimized Pd/SSZ-13 displayed improved durability and outstanding moisture resistance during CH<sub>4</sub> combustion. This study sheds new light on the fabrication of high-performance Pd-zeolite catalysts for CH<sub>4</sub> emission abatement by facile engineering of zeolite mesoporosity.","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4000,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Catalytic Methane Mitigation Over Mesoporosity-Engineered Hierarchically Porous Pd/SSZ-13 Zeolites\",\"authors\":\"Gaozhou Liang, Anqi Guo, Wuwan Xiong, Dongdong Chen, Ulrich Simon, Daiqi Ye, Haibao Huang, Peirong Chen\",\"doi\":\"10.1021/acsestengg.4c00347\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Palladium-zeolites are active catalysts for abating methane (CH<sub>4</sub>), the second largest greenhouse gas contributing to climate change, via catalytic combustion. Yet, it remains challenging to improve the activity of Pd-zeolites in CH<sub>4</sub> combustion, in particular under humid conditions. Here, using small-pore SSZ-13 zeolite as a showcase, we demonstrate mesoporosity engineering as an effective approach to boost the CH<sub>4</sub> combustion performance of Pd-zeolites. A newly designed gemini quaternary ammonium surfactant, namely C<sub>18–4</sub>N<sub>2</sub>MP, was fabricated using inexpensive reagents and employed as a mesoporogen in the hydrothermal synthesis of hierarchically micro–meso–macro–porous SSZ-13 product. High-dispersion Pd catalysts were achieved by using the hierarchically porous SSZ-13 zeolites as supports. Physicochemical characterization and reaction kinetics disclosed that rational mesoporosity engineering of the hierarchically porous SSZ-13, simply by optimizing C<sub>18–4</sub>N<sub>2</sub>MP addition in the precursor gel prior to hydrothermal crystallization, favored the formation of highly dispersed PdO<i><sub>x</sub></i> active phase and, in turn, the CH<sub>4</sub> combustion without noticeable accumulation of carbonaceous intermediates on the surface. Additionally, mesoporosity-optimized Pd/SSZ-13 displayed improved durability and outstanding moisture resistance during CH<sub>4</sub> combustion. This study sheds new light on the fabrication of high-performance Pd-zeolite catalysts for CH<sub>4</sub> emission abatement by facile engineering of zeolite mesoporosity.\",\"PeriodicalId\":7008,\"journal\":{\"name\":\"ACS ES&T engineering\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.4000,\"publicationDate\":\"2024-08-30\",\"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.4c00347\",\"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.4c00347","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Catalytic Methane Mitigation Over Mesoporosity-Engineered Hierarchically Porous Pd/SSZ-13 Zeolites
Palladium-zeolites are active catalysts for abating methane (CH4), the second largest greenhouse gas contributing to climate change, via catalytic combustion. Yet, it remains challenging to improve the activity of Pd-zeolites in CH4 combustion, in particular under humid conditions. Here, using small-pore SSZ-13 zeolite as a showcase, we demonstrate mesoporosity engineering as an effective approach to boost the CH4 combustion performance of Pd-zeolites. A newly designed gemini quaternary ammonium surfactant, namely C18–4N2MP, was fabricated using inexpensive reagents and employed as a mesoporogen in the hydrothermal synthesis of hierarchically micro–meso–macro–porous SSZ-13 product. High-dispersion Pd catalysts were achieved by using the hierarchically porous SSZ-13 zeolites as supports. Physicochemical characterization and reaction kinetics disclosed that rational mesoporosity engineering of the hierarchically porous SSZ-13, simply by optimizing C18–4N2MP addition in the precursor gel prior to hydrothermal crystallization, favored the formation of highly dispersed PdOx active phase and, in turn, the CH4 combustion without noticeable accumulation of carbonaceous intermediates on the surface. Additionally, mesoporosity-optimized Pd/SSZ-13 displayed improved durability and outstanding moisture resistance during CH4 combustion. This study sheds new light on the fabrication of high-performance Pd-zeolite catalysts for CH4 emission abatement by facile engineering of zeolite mesoporosity.
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.