Docking MOF crystals on graphene support for highly selective electrocatalytic peroxide production
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Tailoring the reaction kinetics is the central theme of designer electrocatalysts, which enables the selective conversion of abundant and inert atmospheric species into useful products. Here we show a supporting effect in tuning the electrocatalytic kinetics of oxygen reduction reaction (ORR) from four-electron to two-electron mechanism by docking metalloporphyrin-based metal-organic frameworks (MOFs) crystals on graphene support, leading to highly selective peroxide production with faradaic efficiency as high as 93.4%. A magic angle of 38.1° tilting for the co-facial alignment was uncovered by electron diffraction tomography, which is attributed to the maximization of π-π interaction for mitigating the lattice and symmetry mismatch between MOF and graphene. The facilitated electron migration and oxygen chemisorption could be ascribed to the supportive effect of graphene that disperses of the electron state of the active center, and ultimately regulates rate-determining step.
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Docking MOF crystals on graphene support for highly selective electrocatalytic peroxide production
)
Abstract
Tailoring the reaction kinetics is the central theme of designer electrocatalysts, which enables the selective conversion of abundant and inert atmospheric species into useful products. Here we show a supporting effect in tuning the electrocatalytic kinetics of oxygen reduction reaction (ORR) from four-electron to two-electron mechanism by docking metalloporphyrin-based metal-organic frameworks (MOFs) crystals on graphene support, leading to highly selective peroxide production with faradaic efficiency as high as 93.4%. A magic angle of 38.1° tilting for the co-facial alignment was uncovered by electron diffraction tomography, which is attributed to the maximization of π-π interaction for mitigating the lattice and symmetry mismatch between MOF and graphene. The facilitated electron migration and oxygen chemisorption could be ascribed to the supportive effect of graphene that disperses of the electron state of the active center, and ultimately regulates rate-determining step.
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Acknowledgements
This work is supported by the National Natural Science Foundation of China (Nos. 21522105 and 51861145313) and the Science & Technology Commission of Shanghai Municipality (17JC1404000). We acknowledge the support from the ShanghaiTech-SARI Joint Laboratory of Low-Carbon Energy Science, the Centre for High-resolution Electron Microscopy (CħEM, contract No. EM02161943), and the Analytical Instrumentation Center (Contract no. SPST-AIC10112914), SPST, ShanghaiTech University. The synchrotron X-ray portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, a Directorate of SLAC National Accelerator Laboratory and an Office of Science User Facility operated for the US Department of Energy Office of Science by Stanford University. L. M. and F. L. acknowledge Department of Chemistry Startup fund at Virginia Tech; A. M. acknowledge the support of National Natural Science Foundation of China (Nos. 21850410448 and 21835002). We thank the STEM support from Dr. Weiyan Liu in CħEM. We also thank Prof. O. Terasaki, Prof. Z. Liu, Prof. Y. Ma, and Mr. T. Sun for their guidance in electron diffraction and XPS analyses. We thank and will remember Prof. Frank Tsung for his kind suggestion and encouragement, who left us forever on January 5, 2021 due to COVID-19.
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