Chatterjee Abhishikta, Mondal Papri, Chakraborty Priyanka, Kumar Bidyapati, Mandal Sourav, Rizzoli Corrado, Saha Rajat, Adhikary Bibhutosh, Dey Subrata K
Department of Chemistry, Sidho-Kanho-Birsha University, 723104, Purulia, WB, India.
Department of Chemistry, Indian Institution of Engineering Science and Technology, 711103, Shibpur, Howrah, India.
Angew Chem Int Ed Engl. 2023 Oct 16;62(42):e202307832. doi: 10.1002/anie.202307832. Epub 2023 Aug 4.
In this research, highly efficient heterogeneous bifunctional (BF) electrocatalysts (ECs) have been strategically designed by Fe coordination (C ) complexes, [Fe L (H O) Cl ] (C1) and [Fe L (H O) (SO )].2(CH O) (C2) where the high seven C number synergistically modifies the electronic environment of the Fe centre for facilitation of H O electrolysis. The electronic status of Fe and its adjacent atomic sites have been further modified by the replacement of -Cl in C1 by -SO in C2. Interestingly, compared to C1, the O-S-O bridged C2 reveals superior BF activity with extremely low overpotential (η) at 10 mA cm (140 mV , 62 mV ) and small Tafel slope (120.9 mV dec , 45.8 mV dec ). Additionally, C2 also facilitates a high-performance alkaline H O electrolyzer with cell voltage of 1.54 V at 10 mA cm and exhibits remarkable long-term stability. Thus, exploration of the intrinsic properties of metal-organic framework (MOF)-based ECs opens up a new approach to the rational design of a wide range of molecular catalysts.
在本研究中，通过铁配位（C）配合物[FeL(H₂O)Cl₂]（C1）和[FeL(H₂O)₂(SO₄)].2(CH₃OH)（C2）精心设计了高效的非均相双功能（BF）电催化剂（ECs），其中高七个C数协同修饰了Fe中心的电子环境以促进H₂O电解。通过将C1中的-Cl替换为C2中的-SO₄，进一步修饰了Fe及其相邻原子位点的电子状态。有趣的是，与C1相比，O-S-O桥连的C2在10 mA cm⁻²时显示出优异的BF活性，过电位（η）极低（140 mV，62 mV）且塔菲尔斜率小（120.9 mV dec⁻¹，45.8 mV dec⁻¹）。此外，C2还促进了高性能碱性H₂O电解槽，在10 mA cm⁻²时电池电压为1.54 V，并表现出显著的长期稳定性。因此，探索基于金属有机框架（MOF）的ECs的内在性质为合理设计各种分子催化剂开辟了一条新途径。
