Minhyung Lee, Bupmo Kim, Suho Kim, Hwan Kim, Minjun Park, Wonyong Choi, Wooyul Kim* and Hyoung-il Kim*,
{"title":"Role of the TiO2 Crystalline Phase in Pt-TiO2 for Thermocatalytic Mineralization of Gaseous Acetaldehyde","authors":"Minhyung Lee, Bupmo Kim, Suho Kim, Hwan Kim, Minjun Park, Wonyong Choi, Wooyul Kim* and Hyoung-il Kim*, ","doi":"10.1021/acsestengg.4c0065410.1021/acsestengg.4c00654","DOIUrl":null,"url":null,"abstract":"<p >Pt-TiO<sub>2</sub> is an efficient low-temperature thermocatalyst for volatile organic compound (VOC) removal, driven by active oxygen species formation through metal–support interactions. While the role of Pt is well established, the influence of TiO<sub>2</sub> polymorphs on active oxygen generation is less understood. This study explores the thermocatalytic removal of acetaldehyde (CH<sub>3</sub>CHO) over Pt supported on three TiO<sub>2</sub> polymorphs: anatase, rutile, and brookite. CH<sub>3</sub>CHO mineralization at 160 °C follows the trend: Pt-anatase (99.5%) > Pt-rutile (79.3%) > Pt-brookite (56.7%). These differences correlate with the oxygen adsorption and active oxygen generation capabilities, as evidenced by electrochemical analyses and O<sub>2</sub>-temperature-programmed desorption. Density functional theory calculations further indicate that Pt supported on anatase has the highest negative charge density, which significantly enhances the formation of active oxygen species. <i>In situ</i> FTIR spectroscopy provides additional evidence by revealing distinct CH<sub>3</sub>CHO oxidation pathways: *HCOOH on Pt-anatase and Pt-brookite, and *CH<sub>3</sub>COOH on Pt-rutile. Despite sharing a similar pathway, Pt-anatase displayed faster kinetics due to a higher abundance of surface-active oxygen species. This study highlights the pivotal role of TiO<sub>2</sub> polymorphs in shaping metal–support interactions and provides critical insights for designing efficient Pt-based catalysts for thermocatalytic VOC abatement.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":"5 3","pages":"743–755 743–755"},"PeriodicalIF":7.4000,"publicationDate":"2024-12-16","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://pubs.acs.org/doi/10.1021/acsestengg.4c00654","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
引用次数: 0
Abstract
Pt-TiO2 is an efficient low-temperature thermocatalyst for volatile organic compound (VOC) removal, driven by active oxygen species formation through metal–support interactions. While the role of Pt is well established, the influence of TiO2 polymorphs on active oxygen generation is less understood. This study explores the thermocatalytic removal of acetaldehyde (CH3CHO) over Pt supported on three TiO2 polymorphs: anatase, rutile, and brookite. CH3CHO mineralization at 160 °C follows the trend: Pt-anatase (99.5%) > Pt-rutile (79.3%) > Pt-brookite (56.7%). These differences correlate with the oxygen adsorption and active oxygen generation capabilities, as evidenced by electrochemical analyses and O2-temperature-programmed desorption. Density functional theory calculations further indicate that Pt supported on anatase has the highest negative charge density, which significantly enhances the formation of active oxygen species. In situ FTIR spectroscopy provides additional evidence by revealing distinct CH3CHO oxidation pathways: *HCOOH on Pt-anatase and Pt-brookite, and *CH3COOH on Pt-rutile. Despite sharing a similar pathway, Pt-anatase displayed faster kinetics due to a higher abundance of surface-active oxygen species. This study highlights the pivotal role of TiO2 polymorphs in shaping metal–support interactions and provides critical insights for designing efficient Pt-based catalysts for thermocatalytic VOC abatement.
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.