Role of the TiO2 Crystalline Phase in Pt-TiO2 for Thermocatalytic Mineralization of Gaseous Acetaldehyde

IF 7.4 Q1 ENGINEERING, ENVIRONMENTAL

ACS ES&T engineering Pub Date : 2024-12-16 DOI:10.1021/acsestengg.4c0065410.1021/acsestengg.4c00654

Minhyung Lee, Bupmo Kim, Suho Kim, Hwan Kim, Minjun Park, Wonyong Choi, Wooyul Kim* and Hyoung-il Kim*,

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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.

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TiO2晶相在Pt-TiO2热催化矿化气态乙醛中的作用

Pt-TiO2是一种高效的去除挥发性有机化合物（VOC）的低温热催化剂，通过金属-载体相互作用形成活性氧驱动。虽然Pt的作用已经确定，但TiO2多晶对活性氧生成的影响尚不清楚。本研究探讨了三种TiO2多晶型物（锐钛矿、金红石和板岩）在Pt上的热催化脱除乙醛（CH3CHO）。160℃CH3CHO矿化趋势如下：pt -锐钛矿（99.5%）>；铂金红石（79.3%）>；Pt-brookite(56.7%)。这些差异与氧吸附和活性氧生成能力有关，电化学分析和o2温度程序解吸证明了这一点。密度泛函理论计算进一步表明，锐钛矿负载的Pt具有最高的负电荷密度，这显著促进了活性氧的形成。原位FTIR光谱通过揭示不同的CH3CHO氧化途径提供了额外的证据：*HCOOH在pt锐钛矿和pt brookite上，*CH3COOH在pt金红石上。尽管共享类似的途径，但由于表面活性氧的丰度更高，锐钛矿酶表现出更快的动力学。该研究强调了TiO2多晶型物在形成金属-载体相互作用中的关键作用，并为设计高效的pt基催化剂用于热催化VOC减排提供了重要见解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS ES&T engineering ENGINEERING, ENVIRONMENTAL-

CiteScore

8.50

自引率

0.00%

发文量

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.