Unraveling Volcano Trend in OER of Metal–Organic Frameworks with Asymmetric Configuration through Energy Band Engineering
Applied Catalysis B: Environment and Energy(2024)
摘要
Local symmetry breaking of catalysts has emerged as an effective strategy for finely tuning oxygen evolution reaction (OER) activity, yet the fundamental comprehension regarding asymmetric structure-activity relationships remains limited. Here, we propose the energy band engineering to bridge the correlation between established asymmetric electronic structure and adsorption/desorption ability of reaction intermediates within metal-organic frameworks (MOFs). The deliberate synthesis of CoM-MOFs (M=Cu, Ni, and Fe) with distinct coordination microenvironments enables the customization of asymmetric Co-O-M electronic structure. A volcano-shaped relationship can be revealed between calculated OER overpotential and average d-band center (Ed) energy level for both active Co sites and substituted M. The CoFe-MOF, located close to the summit, showcases the balanced reaction intermediate behavior and thus for enhanced OER activity. This work presents a promising approach to thoroughly understand asymmetric electronic structure-activity relationships from the perspective of energy band engineering and further guide the discovery of high-efficiency MOF-based OER catalysts.
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关键词
metal-organic frameworks,energy band engineering,asymmetric electronic structure,d-band center,oxygen evolution reaction
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