Selective oxidation of sulfides with oxygen over a pyrene covalent organic framework photocatalyst with TEMPO

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2023-12-25 DOI:10.1016/j.apcatb.2023.123660

Xiaoyun Dong, Fulin Zhang, Yuexin Wang, Fengwei Huang, Xianjun Lang

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Abstract

Covalent organic frameworks (COFs) can be precisely modulated through the covalent linkage of organic building blocks. Therefore, developing COFs to high-performance photocatalysts is highly applicable. Herein, with trifluoroacetic acid as the catalyst, Py-Azine-COF is constructed by aldimine condensation between 1,3,6,8-tetrakis(4-formylphenyl)pyrene and hydrazine hydrate. The highly crystalline Py-Azine-COF possesses a remarkable specific surface area of 1428 m² g⁻¹. Intriguingly, selective aerobic conversion is achieved over Py-Azine-COF photocatalyst with (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO). Significantly, TEMPO accelerates the hole transfer and cooperates with superoxide formed from oxygen for selective oxidation of organic sulfides. With the assistance of 2 mol% TEMPO, the performance of Py-Azine-COF photocatalyst is increased markedly. Gratifyingly, TEMPO, a hole mediator, enables expeditious conversions of various sulfides into sulfoxides over Py-Azine-COF photocatalyst in methanol. Generally, COFs can be customized by modulating the covalent connection of organic building blocks to meet the requirements of selective aerobic oxidations.

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用 TEMPO 在芘共价有机框架光催化剂上用氧选择性氧化硫化物

共价有机框架（COFs）可通过有机结构单元的共价连接进行精确调节，从而展现出理想的光催化性能。因此，定制 COF 以开发高性能光催化剂是一种可取的方法。以 CF3COOH 为催化剂，1,3,6,8-四(4-甲酰基苯基)芘和水合肼通过醛缩合反应生成 Py-Azine-COF。高结晶的 Py-Azine-COF 具有 1428 平方米 g-1 的显著比表面积。有趣的是，Py-Azine-COF 光催化剂与（2,2,6,6-四甲基哌啶-1-基）羰基（TEMPO）实现了选择性转化。值得注意的是，TEMPO 加快了空穴传输，并与氧气形成的超氧化物合作完成了有机硫化物的选择性氧化。在 2 mol% TEMPO 的帮助下，Py-Azine-COF 光催化剂的活性显著提高。令人欣慰的是，空穴介质 TEMPO 使 Py-Azine-COF 光催化剂在原生溶剂甲醇中迅速将各种硫化物转化为硫氧化物。这项工作表明，可以通过调节有机构件的共价连接来定制 COF，以满足选择性光催化氧化的要求。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.