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导电且超稳定的共价有机框架/碳杂化物作为理想的电催化平台

Conductive and Ultrastable Covalent Organic Framework/Carbon Hybrid as an Ideal Electrocatalytic Platform.

作者信息

Seo Jeong-Min, Noh Hyuk-Jun, Jeon Jong-Pil, Kim Hyeongjun, Han Gao-Feng, Kwak Sang Kyu, Jeong Hu Young, Wang Lianli, Li Feng, Baek Jong-Beom

机构信息

Department of Energy and Chemical Engineering/Center for Dimension-Controllable Organic Frameworks, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulsan 44919, Republic of Korea.

Department of Energy Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulsan 44919, Republic of Korea.

出版信息

J Am Chem Soc. 2022 Nov 2;144(43):19973-19980. doi: 10.1021/jacs.2c08344. Epub 2022 Oct 14.

Abstract

Developing covalent organic frameworks (COFs) with good electrical conductivity is essential to widen their range of practical applications. Thermal annealing is known to be a facile approach for enhancing conductivity. However, at higher temperatures, most COFs undergo amorphization and/or thermal degradation because of the lack of linker rigidity and physicochemical stability. Here, we report the synthesis of a conductive benzoxazole-linked COF/carbon hybrid material (BCOF-600C) by simple thermal annealing. The fused-aromatic benzoxazole and biphenyl building units endow the resulting COF with excellent physicochemical stability against high temperatures and strong acids/bases. This allows heat treatment to further enhance electrical conductivity with minimal structural alteration. The robust crystalline structure with periodically incorporated nitrogen atoms allowed platinum (Pt) atoms to be atomically integrated into the channel walls of BCOF-600C. The resulting electrocatalyst with well-defined active sites exhibited superior catalytic performance toward hydrogen evolution in acidic media.

摘要

开发具有良好导电性的共价有机框架(COF)对于拓宽其实际应用范围至关重要。热退火是一种增强导电性的简便方法。然而,在较高温度下,由于缺乏连接体刚性和物理化学稳定性,大多数COF会发生非晶化和/或热降解。在此,我们报告了通过简单热退火合成一种导电苯并恶唑连接的COF/碳杂化材料(BCOF-600C)。稠合芳族苯并恶唑和联苯构建单元赋予所得COF优异的耐高温和耐强酸/碱的物理化学稳定性。这使得热处理能够在结构变化最小的情况下进一步提高导电性。具有周期性掺入氮原子的坚固晶体结构使铂(Pt)原子能够原子级地整合到BCOF-600C的通道壁中。所得具有明确活性位点的电催化剂在酸性介质中对析氢表现出优异的催化性能。

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