A Thiadiazole-Based Covalent Organic Framework: A Metal-Free Electrocatalyst toward Oxygen Evolution Reaction
A Thiadiazole-Based Covalent Organic Framework: A Metal-Free Electrocatalyst toward Oxygen Evolution Reaction
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DOI：
10.1021/acscatal.9b05470
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发表时间：
2020-05-15
期刊：
影响因子：
12.9
通讯作者：
Bhaumik, Asim
中科院分区：
文献类型：
--
作者：
Mondal, Sujan;Mohanty, Bishnupad;Bhaumik, Asim
共价有机骨架（COF）由于其在气体存储、传感、光伏、燃料电池、活性催化剂载体等多个前沿应用领域的广泛潜力，最近引起了人们的广泛关注。然而，关于 COF 上的无金属电催化的报道很少。在此，我们通过1,3,5-三(4-甲酰基苯基)苯和2,5-二肼基-1,3,4-噻二唑之间的反应开发了一种新型噻二唑基COF，C4-SHz COF，其具有高达1224 m(2) g(-1)的比表面积、独特的分子结构、高孔隙率和丰富的活性位点。合成的C4-SHz COF表现出优异的电催化析氧反应（OER）活性和优异的长期耐久性。 C4-SHz COF的电催化性能在320 mV的过电位下实现了10 mA/cm(2)的电流密度。 C4-SHz COF 的较高活性可归因于 pi 共轭有机构建块的高 Brunauer-Emmett-Teller 表面积、孔隙率和网络结构，从而允许快速充电和质量传输过程。这项工作验证了无金属 COF 电催化剂在 OER 方面的巨大潜力及其替代碳基电催化剂的能力。
Covalent organic frameworks (COFs) have attracted surging interest lately due to their wide potential in several frontline application areas like gas storage, sensing, photovoltaics, fuel cells, active catalyst supports, and so on. However, only very few reports are available for the metal-free electrocatalysis over COFs. Herein, we developed a new thiadiazole-based COF, C4-SHz COF, through the reaction between 1,3,5-tris(4-formylphenyl)benzene and 2,5-dihydrazinyl- 1,3,4-thiadiazole that possesses a very high specific surface area of 1224 m(2) g(-1), unique molecular architecture, high porosity, and abundant active sites. The synthesized C4-SHz COF displayed superior electrocatalytic oxygen evolution reaction (OER) activity and excellent long-term durability. The electrocatalytic performance of the C4-SHz COF achieved a current density of 10 mA/cm(2) at an overpotential of 320 mV. The higher activity of the C4-SHz COF could be attributed to the high Brunauer-Emmett-Teller surface area, porosity, and network structure of the pi-conjugated organic building blocks, which allowed fast charge and mass transport processes. This work validates the promising potential of a metal-free COF electrocatalyst toward the OER and its capability to replace carbon-based electrocatalysts.