Abstract
Mixed-addenda polyoxometalate (e.g., PMoxW12-x) by “orbital engineering” allows the functionalization of the single-addenda cluster surface, which offers new electronic properties. However, the well-known agglomeration phenomenon greatly limits the full understanding of its unique redox properties. It makes sense to fully stimulate the intrinsic multi-electron activity of mixed-addenda polyoxometalate by confining engineering to apply in energy technology. With the verification of potential candidate PMo6W6 possessing remarkable stability with fully exposed activity sites in a confined state by theoretical analysis, we achieve the precise confinement of the single PMo6W6 molecule in porous carbon (PC) with a matched pore aperture (PMo6W6@PC). As a result, PMo6W6@PC-based supercapacitor shows high energy densities of 0.308 mWh cm−2 at power densities of 43.2 mW cm−2, outperforming most polyoxometalate-based supercapacitors. Moreover, the device exhibits a capacity retention of over 80.4 % at 8 mA cm−2 after 8000 cycles. This improved electrochemical redox activity may be ascribed to the strong orbital electronic coupling between W and Mo atoms of PMo6W6 by confinement engineering. This work proves that the confined PMo6W6 can maximize the advantages of PMo12O40 and PW12O40, which provides a theoretical basis for other mixed-addenda polyoxometalate species.
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