Enhancement of H2O2 generation rate in porphyrin photocatalysts via crystal facets regulation to create strong internal electric field

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI:10.1016/S1872-2067(24)60039-2

Yunhang Shao , Yaning Zhang , Chaofeng Chen , Shuai Dou , Yang Lou , Yuming Dong , Yongfa Zhu , Chengsi Pan

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Abstract

Three TCPP porphyrin-based nanosheet photocatalysts with exposed (400), (022), and (020) planes were synthesized using a dissolution-recrystallization method in a mixture of water and tetrahydrofuran (THF), methanol (MeOH), and ethylene glycol (EG). The TCPP photocatalyst with the exposed (400) surface exhibited the highest H₂O₂ production rate of 29.33 mmol L⁻¹ h⁻¹ g⁻¹ from only H₂O and O₂, surpassing the rates observed for ones with exposed (022) and (020) surfaces by factors of 2.7 and 4.1, respectively, and 1.3 times as that of the reported TCPP prepared by a base/acid self-assembling method. This enhancement can be attributed to the strong internal electric field and high carboxyl group content on the (400) surface, which hindered rapid charge recombination and facilitated challenging water oxidation. Hence, successful manipulation of porphyrin exposure to robust IEF planes enhances the photocatalytic activity of the system and provides valuable insights for the design and development of more efficient organic photocatalysts.

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通过调节晶面以产生强内电场，提高卟啉光催化剂中 H2O2 的生成率

在水与四氢呋喃（THF）、甲醇（MeOH）和乙二醇（EG）的混合物中，采用溶解-重结晶法合成了三种具有暴露（400）、（022）和（020）平面的 TCPP 卟啉基纳米片光催化剂。表面（400）裸露的 TCPP 光催化剂仅从 H2O 和 O2 产生 H2O2 的速率最高，达到 29.33 mmol L-1 h-1 g-1，分别比表面（022）和（020）裸露的 TCPP 的速率高出 2.7 倍和 4.1 倍，是已报道的用碱/酸自组装方法制备的 TCPP 的 1.3 倍。这种增强可归因于（400）表面的强内电场和高羧基含量，它们阻碍了电荷的快速重组，促进了具有挑战性的水氧化。因此，成功地将卟啉暴露在强大的内电场平面上增强了系统的光催化活性，为设计和开发更高效的有机光催化剂提供了宝贵的启示。

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来源期刊

Chinese Journal of Catalysis 工程技术-工程：化工

CiteScore

25.80

自引率

10.30%

发文量

235

审稿时长

1.2 months

期刊介绍： The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.