期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 62, 期 4, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202216008
关键词
Defect Engineering; Metal-Organic Frameworks; Multivariate MOFs; Oxygen Evolution Reaction; iDPC-STEM
The atomic structure of multivariate metal-organic frameworks (MTV-MOFs) was visualized using the iDPC-STEM technique, guiding the design of bulk MOFs for efficient oxygen evolution reaction (OER). Incorporating Fe3+ or 2-aminoterephthalate (ATA) into Ni-BDC weakened the coordination bonds, allowing for selective cleavage via mild heat treatment to generate coordinatively unsaturated metal sites, conductive Ni@C, and hierarchical porous structure. The defective MOFs exhibited excellent OER activity, with current densities of 10 and 100 mA cm(-2) achieved at small overpotentials of 286 mV and 365 mV, respectively, surpassing commercial RuO2 catalyst and most bulk MOFs.
The direct utilization of metal-organic frameworks (MOFs) for electrocatalytic oxygen evolution reaction (OER) has attracted increasing interests. Herein, we employ the low-dose integrated differential phase contrast-scanning transmission electron microscopy (iDPC-STEM) technique to visualize the atomic structure of multivariate MOFs (MTV-MOFs) for guiding the structural design of bulk MOFs for efficient OER. The iDPC-STEM images revealed that incorporating Fe3+ or 2-aminoterephthalate (ATA) into Ni-BDC (BDC: benzenedicarboxylate) can introduce inhomogeneous lattice strain that weaken the coordination bonds, which can be selectively cleaved via a mild heat treatment to simultaneously generate coordinatively unsaturated metal sites, conductive Ni@C and hierarchical porous structure. Thus, excellent OER activity with current densities of 10 and 100 mA cm(-2) are achieved over the defective MOFs at small overpotentials of 286 mV and 365 mV, respectively, which is superior to the commercial RuO2 catalyst and most of the bulk MOFs.
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