Deactivation-Tolerance of Heterojunction Anatase and Bronze TiO2 in the Photocatalytic Mineralization of Toluene

IF 7.4 Q1 ENGINEERING, ENVIRONMENTAL ACS ES&T engineering Pub Date : 2024-07-23 DOI:10.1021/acsestengg.4c0028110.1021/acsestengg.4c00281

Dong Jin Kim, Jiyeon Park, Gayoung Ham, Hyojung Cha, Dong Suk Han, Minho Kim* and Hyunwoong Park*,

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Abstract

Heterojunctioning anatase (A) and rutile (R) TiO₂ is considered a benchmark strategy for high photocatalytic activity. In this study, we synthesized heterojunctions of anatase (A) and bronze (B) TiO₂ via hydrothermal and annealing processes using low-cost commercial A-TiO₂. The as-synthesized AB-TiO₂ shows remarkable activity for toluene mineralization and a strong tolerance to deactivation. The activity and durability of AB-TiO₂ far exceed those of A-, R-, B-, and AR-TiO₂, which are bare and even Pt-deposited (a total of 10 TiO₂ samples). AB-TiO₂ exhibits highly active {001} facets for the generation of hydroxyl radicals and oxygen vacancies beneficial for O₂ adsorption. Transient absorption and time-resolved photoluminescence spectroscopies reveal the characteristic lifetimes of electrons and holes. Density functional theory calculations demonstrate facile charge separation and identify the catalytically active surface for oxidation as the anatase surface in AB-TiO₂. The observed high activity and durability are analyzed in terms of photochemical and catalytic factors.

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异质结 Anatase 和青铜 TiO2 在甲苯光催化矿化过程中的失活耐受性

锐钛矿（A）和金红石（R）二氧化钛异质结被认为是实现高光催化活性的基准策略。在本研究中，我们利用低成本的商用 A-TiO2 通过水热法和退火工艺合成了锐钛矿（A）和青铜矿（B）TiO2 的异质结。合成的 AB-TiO2 对甲苯矿化显示出显著的活性和很强的失活耐受性。AB-TiO2 的活性和耐久性远远超过 A-、R-、B- 和 AR-TiO2（共 10 个 TiO2 样品），后者是裸露的，甚至是铂沉积的。AB-TiO2 显示出高度活跃的 {001} 面，可产生羟基自由基和有利于吸附 O2 的氧空位。瞬态吸收和时间分辨光致发光光谱揭示了电子和空穴的特征寿命。密度泛函理论计算证明了电荷分离的简易性，并确定了 AB-TiO2 中具有催化活性的氧化表面为锐钛矿表面。从光化学和催化因素的角度分析了观察到的高活性和耐久性。

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来源期刊

ACS ES&T engineering ENGINEERING, ENVIRONMENTAL-

CiteScore

8.50

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0.00%

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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.