Stable Black Phosphorus Encapsulation in Porous Mesh-like UiO-66 Promoted Charge Transfer for Photocatalytic Oxidation of Toluene and o-Dichlorobenzene: Performance, Degradation Pathway, and Mechanism,ACS Catalysis

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Stable Black Phosphorus Encapsulation in Porous Mesh-like UiO-66 Promoted Charge Transfer for Photocatalytic Oxidation of Toluene and o-Dichlorobenzene: Performance, Degradation Pathway, and Mechanism
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-06-22 , DOI: 10.1021/acscatal.2c01375
Jinfeng Chen ₁ , Yang Yang ₁ , Shenghao Zhao ₁ , Fukun Bi ₁ , Liang Song ₁ , Ning Liu ₁ , Jingcheng Xu ₂ , Yuxin Wang ₃ , Xiaodong Zhang ₁

Affiliation

This work presents a new strategy to enhance the charge transfer from Zr atoms in UiO-66 to black phosphorus (BP) via an atomic-level charge-transfer channel provided by Zr–P bonds for photocatalytic degradation of toluene and o-dichlorobenzene. The formation of Zr–P bonds is the key to covering BP with the UiO-66 encapsulation layer and improving the charge-transfer capability of BP–UiO, which is also verified by a series of characterization and theoretical calculations. The hydrophilic porous mesh-like UiO-66 encapsulation layer endows BP–UiO with enhanced visible-light-harvesting ability, charge transport capability, and photocatalytic activity. Additionally, BP–UiO demonstrates the promoted redox/acidity properties, significantly improving catalytic activity for the degradation of toluene and o-dichlorobenzene even in the presence of water. The degradation pathways of contaminants are investigated via the study of transient variations by in situ infrared (IR) methods, refined by the static analysis of intermates accumulated on the BP–UiO surface by gas chromatography–mass spectrometry (GC–MS). The electron transfer via bond construction and the combination of in situ IR and GC–MS are expected to provide a more complete theoretical basis for environmental catalysis.

中文翻译：

多孔网状 UiO-66 中稳定的黑磷封装促进了甲苯和邻二氯苯光催化氧化的电荷转移：性能、降解途径和机理

这项工作提出了一种新的策略，通过 Zr-P 键提供的原子级电荷转移通道增强从 UiO-66 中的 Zr 原子到黑磷 (BP) 的电荷转移，用于光催化降解甲苯和邻二氯苯。Zr-P键的形成是用UiO-66包封层覆盖BP，提高BP-UiO电荷转移能力的关键，一系列表征和理论计算也验证了这一点。亲水性多孔网状 UiO-66 封装层赋予 BP-UiO 增强的可见光捕获能力、电荷传输能力和光催化活性。此外，BP-UiO 表现出促进的氧化还原/酸性特性，显着提高了降解甲苯和o-二氯苯，即使有水存在。通过原位红外 (IR) 方法研究瞬态变化来研究污染物的降解途径，并通过气相色谱 - 质谱 (GC-MS) 对积累在 BP-UiO 表面上的互化物进行静态分析来改进污染物的降解途径。通过键结构的电子转移以及原位IR和GC-MS的结合有望为环境催化提供更完整的理论基础。

更新日期：2022-06-22

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