Surface Restructuring of Zeolite‐Encapsulated Halide Perovskite to Activate Lattice Oxygen Oxidation for Water Electrolysis

Abstract

Metal‐halide perovskites possess great potential for electrochemical water splitting that has not been realized due to their intolerance to water. Here, methylammonium lead halide perovskites (MAPbX3) are used to electrocatalyze water oxidation in aqueous electrolytes by creating MAPbX3@AlPO‐5 host–guest composites. Due to the protective feature of the zeolite matrix, halide perovskite nanocrystals (NCs) confined in aluminophosphate AlPO‐5 zeolites achieve an excellent stability in water. The resultant electrocatalyst undergoes dynamic surface restructuring during the oxygen evolution reaction (OER) with the formation of an edge‐sharing α‐PbO2 active layer. The existence of charge‐transfer interactions at the MAPbX3/α‐PbO2 interface significantly modulates the surface electron density of the α‐PbO2 and optimizes the adsorption free energy of oxygen‐containing intermediate species. Furthermore, the soft‐lattice nature of halide perovskites enables more facile triggering of lattice‐oxygen oxidation of nanostructured α‐PbO2, exhibiting pH‐dependent OER activity and non‐concerted proton‐electron transfer for MAPbX3@AlPO‐5 composite. As a result, the developed MAPbBr3@AlPO‐5 composite manifests an ultralow overpotential of 233 mV at 10 mA cm−2 in 1 m KOH. These findings offer facile access to halide perovskite applied to water electrolysis with enhanced intrinsic activity, providing a new paradigm for designing high‐efficiency OER electrocatalysts.

Rapid Surface Reconstruction of Te-Doped NiFe Layered Double Hydroxide for Robust Oxygen Evolution at High Current Density

“…The presence of oxidation peaks at different sweep rates corresponding to the surface restructuring before the OER process (Figure S5). − To elucidate the reaction mechanism deeply, we obtained the b value by analyzing the slope of the logarithmic relationship between the scan rate and the peak current. In scenarios where substance diffusion primarily governs the reaction, the parameter b value tends to be approximately 0.5, while when the electrochemical reaction process is solely dictated by surface capacitive behavior, the value of b approaches 1.0 .…”

FeCoCuMnRuB Nanobox with Dual Driving of High-Entropy and Electron-Trap Effects as the Efficient Electrocatalyst for Water Oxidation

“…5,6 Although noble metal oxides (RuO 2 and IrO 2 ) have splendid OER catalytic properties, the low reserve and poor stability have hindered their large-scale deployment. 7 Therefore, it is significant to search for earth-abundant catalysts.…”

“…Various renewable energy devices, such as water electrolyzers, rechargeable metal–air batteries, fuel cells, etc., rely on the oxygen evolution reaction (OER). However, its sluggish dynamics impede the progress of the energy technologies. , Although noble metal oxides (RuO 2 and IrO 2 ) have splendid OER catalytic properties, the low reserve and poor stability have hindered their large-scale deployment . Therefore, it is significant to search for earth-abundant catalysts.…”

Regulating Lattice Oxygen of Co3O4/CeO2 Heterojunction Nanonetworks for Enhanced Oxygen Evolution

“…Hence, exploring OER electrocatalysts with low cost and high efficiency has received increasing attention, but may pose a huge challenge. [7,8] Up to now, considerable efforts have been made to design appropriate OER electrocatalysts by optimizing their components and compositions, including chalcogenides, carbides, hydroxide, nitrides, phosphides, and oxides. [9][10][11][12][13][14] For instance, Jia et al successfully prepared oxygen-modified nanotubes with hierarchical structure as electrocatalyst, which exhibited outstanding OER performance through the surface modification with oxygen.…”