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Lead-Free, Ultrastable, Tungsten-Based Ruddlesden-Popper and Hybrid Perovskite Frameworks for Aqueous Pseudocapacitive Charge Storage
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DOI：10.1002/ente.202400531.png)
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Abstract
En 中文
The instability of hybrid organic-inorganic perovskites (HOIPs) in several electrolytes and the toxicity of heavy metals such as lead hinder their application in many electrochemical devices. Herein, an already existing Ruddlesden-Popper (R-P) structure of tungstic acid variants as a generic framework to achieve ultrastable HOIPs, serving as stable and safer alternatives to lead-based HOIPs in aqueous electrochemical devices, is introduced. An enormous improvement (of the tungsten-based framework) in electrochemical performance is achieved by converting electrochemically sluggish H2W2O7 to oxygen-deficient H2W2O7-delta to leverage a facile and reversible W6+ -> W5+ transition along with local defect-mediated H+ insertion/extraction. This local structural modification results in a remarkable pseudocapacitive performance (specific capacitance of approximate to 622 F g(-1) or specific capacity 155.5 mAh g(-1) at 64 C) with no observable capacity fade (approximate to 100% specific capacity retention after thousands of cycles) in 0.5 m H2SO4 aqueous solution. To extend the scope of utilization of this R-P phase in aqueous electrochemical energy storage devices, OA(2)W(2)O(7)(-)(delta) (OA = octylammonium), a HOIP, which similarly displays impressive EES performance is synthesized. Most importantly, when used as an electrode material, this HOIP exhibits remarkably high stability in aqueous acidic electrolyte.
Keywords:
hybrid perovskites
lead free
pseudocapacitances
Ruddlesden-Popper
water stable
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