Abstract
Efficient transfer of photo-generated charges is a key kinetic factor of photocatalytic water (H2O) overall splitting. Herein, conversion of polypyrrole nanowire (PPyWs) insulator into delocalized ferroelectric semiconductor by transforming pyrrole into graphene structure containing azide (CNxFs) and subsequently integrating Ni2P (CNxFs/Ni2P) has been achieved for efficiently photocatalytic H2O overall splitting into hydrogen (H2) energy through a joint thermal and hydrothermal treatment. Theoretical prediction and detailed experimental results reveal that band gap of PPyWs insulator narrows from 4.63 eV to 2.36 eV of CNxFs (redox potentials: −0.85/1.51 V vs NHE), and the constructed delocalized ferroelectric CNxFs/Ni2P show efficient charge directional migration from generation sites to surface redox active sites. As a result, stoichiometric H2 and O2 evolution and a solar-to-H2 (STH) efficiency of 1.273 ± 0.051 % in photocatalytic H2O overall splitting have been completed under AM 1.5 G solar simulator irradiation along with gas bubbles under visible and even natural solar light. This research aims to solve the kinetic barrier of photocatalytic H2O splitting fundamentally through delocalized ferroelectric engineering, which will greatly boost the development of solar to H2 energy conversion.
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