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Metal‐Phthalocyanine‐Based Two‐Dimensional Conjugated Metal‐Organic Frameworks for Electrochemical Glycerol Oxidation Reaction

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Li,  Xiaodong       
Department of Synthetic Materials and Functional Devices (SMFD), Max Planck Institute of Microstructure Physics, Max Planck Society;

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Feng,  Xinliang       
Department of Synthetic Materials and Functional Devices (SMFD), Max Planck Institute of Microstructure Physics, Max Planck Society;

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Citation

Huang, X., Wang, M., Zhong, H., Li, X., Wang, H., Lu, Y., et al. (2024). Metal‐Phthalocyanine‐Based Two‐Dimensional Conjugated Metal‐Organic Frameworks for Electrochemical Glycerol Oxidation Reaction. Angewandte Chemie International Edition, e202416178. doi:10.1002/anie.202416178.


Cite as: https://hdl.handle.net/21.11116/0000-0010-4C03-6
Abstract
Electrochemical glycerol oxidation reaction (GOR) is a promising candidate to couple with cathodic reaction, like hydrogen evolution reaction, to produce high-value product with less energy consumption. Two dimensional conjugated metal–organic frameworks (2D c-MOFs), comprising square-planar metal-coordination motifs (e.g., MO4, M(NH)4, MS4), are notable for their programable active sites, intrinsic charge transport, and excellent stability, making them promising catalyst candidates for GOR. In this study, we introduce a novel class of 2D c-MOFs electrocatalysts, M2[NiPcS8] (M=Co/Ni/Cu), which are synthesized via coordination of octathiolphthalocyaninato nickel (NiPc(SH)8) with various metal centers. Due to a fast kinetic and high activity of CoS4 sites for GOR, the electrocatalytic tests demonstrate that Co2[NiPcS8] supported on carbon paper displays a low GOR potential of 1.35 V vs. RHE at 10 mA cm−2, significantly reducing the overall water-electrolysis-voltage reduction by 0.27 V from oxygen evolution reaction to GOR, thereby outperforming Ni2[NiPcS8] and Cu2[NiPcS8]. Additionally, we have determined that the GOR activity of CoX4 linkage sites varies with different heteroatoms, following an experimentally and theoretically confirmed activity order of CoS4>CoO4>Co(NH)4. The GOR performance of Co2[NiPcS8] not only demonstrate superior performance among non-noble metal complex, but also provides critical insights on designing high-performance MOF electrocatalysts upon optimizing the electronic environment of active sites.