{"title":"用于促进氨的选择性氧化的沸石状离子交换铜-凹凸棒石催化剂","authors":"Xuebin Zhang, Tianwei Lan, Qiuying Yi, Yufei Wang, Danhong Cheng and Dengsong Zhang","doi":"10.1039/D4EN00157E","DOIUrl":null,"url":null,"abstract":"<p >The selective catalytic oxidation of ammonia (NH<small><sub>3</sub></small>-SCO) to N<small><sub>2</sub></small> and H<small><sub>2</sub></small>O is a highly efficient method for eliminating NH<small><sub>3</sub></small> pollution. However, it is still a challenge to develop low-cost and high-performance catalysts. Herein, zeolite-like ion-exchanged Cu-attapulgite (Cu-ATP) catalysts have been originally developed for NH<small><sub>3</sub></small>-SCO, and the obtained Cu-ATP catalysts exhibit comparable NH<small><sub>3</sub></small>-SCO performance to the conventional Cu-zeolite catalysts. The dominant Cu<small><sup>2+</sup></small> active sites in Cu-ATP facilitate the adsorption and activation of NH<small><sub>3</sub></small> and O<small><sub>2</sub></small>, leading to high activity (<em>T</em><small><sub>90</sub></small> = 300 °C) and N<small><sub>2</sub></small> selectivity (100%) over a wide temperature range from 180 °C to 390 °C. Temperature-programmed surface reaction and <em>in situ</em> diffuse reflectance infrared Fourier transform spectroscopy studies reveal that the NH<small><sub>3</sub></small>-SCO reaction at Cu<small><sup>2+</sup></small> sites proceeds <em>via</em> the internal selective catalytic reaction (i-SCR) pathway, with NO<small><sub>2</sub></small> serving as the key intermediate. This work paves the way for developing natural clay-based zeolite-like catalysts, which are expected to replace zeolite catalysts in various reactions.</p>","PeriodicalId":73,"journal":{"name":"Environmental Science: Nano","volume":" 6","pages":" 2457-2466"},"PeriodicalIF":5.1000,"publicationDate":"2024-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Zeolite-like ion-exchanged Cu-attapulgite catalysts for promoted selective oxidation of ammonia†\",\"authors\":\"Xuebin Zhang, Tianwei Lan, Qiuying Yi, Yufei Wang, Danhong Cheng and Dengsong Zhang\",\"doi\":\"10.1039/D4EN00157E\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The selective catalytic oxidation of ammonia (NH<small><sub>3</sub></small>-SCO) to N<small><sub>2</sub></small> and H<small><sub>2</sub></small>O is a highly efficient method for eliminating NH<small><sub>3</sub></small> pollution. However, it is still a challenge to develop low-cost and high-performance catalysts. Herein, zeolite-like ion-exchanged Cu-attapulgite (Cu-ATP) catalysts have been originally developed for NH<small><sub>3</sub></small>-SCO, and the obtained Cu-ATP catalysts exhibit comparable NH<small><sub>3</sub></small>-SCO performance to the conventional Cu-zeolite catalysts. The dominant Cu<small><sup>2+</sup></small> active sites in Cu-ATP facilitate the adsorption and activation of NH<small><sub>3</sub></small> and O<small><sub>2</sub></small>, leading to high activity (<em>T</em><small><sub>90</sub></small> = 300 °C) and N<small><sub>2</sub></small> selectivity (100%) over a wide temperature range from 180 °C to 390 °C. Temperature-programmed surface reaction and <em>in situ</em> diffuse reflectance infrared Fourier transform spectroscopy studies reveal that the NH<small><sub>3</sub></small>-SCO reaction at Cu<small><sup>2+</sup></small> sites proceeds <em>via</em> the internal selective catalytic reaction (i-SCR) pathway, with NO<small><sub>2</sub></small> serving as the key intermediate. This work paves the way for developing natural clay-based zeolite-like catalysts, which are expected to replace zeolite catalysts in various reactions.</p>\",\"PeriodicalId\":73,\"journal\":{\"name\":\"Environmental Science: Nano\",\"volume\":\" 6\",\"pages\":\" 2457-2466\"},\"PeriodicalIF\":5.1000,\"publicationDate\":\"2024-04-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Environmental Science: Nano\",\"FirstCategoryId\":\"6\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/en/d4en00157e\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Environmental Science: Nano","FirstCategoryId":"6","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/en/d4en00157e","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Zeolite-like ion-exchanged Cu-attapulgite catalysts for promoted selective oxidation of ammonia†
The selective catalytic oxidation of ammonia (NH3-SCO) to N2 and H2O is a highly efficient method for eliminating NH3 pollution. However, it is still a challenge to develop low-cost and high-performance catalysts. Herein, zeolite-like ion-exchanged Cu-attapulgite (Cu-ATP) catalysts have been originally developed for NH3-SCO, and the obtained Cu-ATP catalysts exhibit comparable NH3-SCO performance to the conventional Cu-zeolite catalysts. The dominant Cu2+ active sites in Cu-ATP facilitate the adsorption and activation of NH3 and O2, leading to high activity (T90 = 300 °C) and N2 selectivity (100%) over a wide temperature range from 180 °C to 390 °C. Temperature-programmed surface reaction and in situ diffuse reflectance infrared Fourier transform spectroscopy studies reveal that the NH3-SCO reaction at Cu2+ sites proceeds via the internal selective catalytic reaction (i-SCR) pathway, with NO2 serving as the key intermediate. This work paves the way for developing natural clay-based zeolite-like catalysts, which are expected to replace zeolite catalysts in various reactions.
期刊介绍:
Environmental Science: Nano serves as a comprehensive and high-impact peer-reviewed source of information on the design and demonstration of engineered nanomaterials for environment-based applications. It also covers the interactions between engineered, natural, and incidental nanomaterials with biological and environmental systems. This scope includes, but is not limited to, the following topic areas:
Novel nanomaterial-based applications for water, air, soil, food, and energy sustainability
Nanomaterial interactions with biological systems and nanotoxicology
Environmental fate, reactivity, and transformations of nanoscale materials
Nanoscale processes in the environment
Sustainable nanotechnology including rational nanomaterial design, life cycle assessment, risk/benefit analysis