An increase of carrier concentration is one of the most important routes for enhancing the catalytic performance of semiconductor photocatalysts. In this study, the Sillén–Aurivillius oxychloride Bi4NbO8Cl with hole doping was successfully prepared by a solid-state reaction method. X-ray powder diffraction (XRD), scanning electron microscopy (SEM), ultraviolet–visible diffuse reflectance spectra (UV–vis DRS), X-ray photoelectron spectrometry (XPS) and photoluminescence spectra (PL) were used to characterize and analyze the prepared samples. The experimental results and density functional theory calculations demonstrate that hole doping can be formed in Bi4NbO8Cl by inserting zinc into the niobium site, and the photocatalytic activity can be improved by introducing additional holes into Bi4NbO8Cl. The photogenerated hole (h+) is considered to be the main active species to degrade trypan blue (TB) through trapping experiments. The optimal photocatalyst of Bi4Nb0.8Zn0.2O8Cl exhibits excellent photocatalytic activity in degradation of trypan blue under visible light irritation. Moreover, a possible photocatalytic degradation mechanism is discussed according the experimental and analytical results.Keywords:Bi4NbO8Cl;hole doping;visible light;photocatalytic degradation
Gaoliang Fu,Ruipeng Hou,Li Sun,Huili Liu,Yaru Wei,Ruixue Wei,Xiangyu Meng,Shouren Zhang,Baocheng Yang
Due to the high configuration entropy, unique atomic arrangement, and electronic structures, high-entropy materials are being actively pursued as bifunctional catalysts for both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in rechargeable zinc–air batteries (ZABs). However, a relevant strategy to enhance the catalytic activity of high-entropy materials is still lacking. Herein, a hole doping strategy has been employed to enable the high-entropy perovskite La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 to effectively catalyze the ORR and OER. Hole doping experiments rely on the substitution of Sr2+ for La3+. The optimized La0.7Sr0.3(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 displays remarkable activity for the ORR and the OER, with a low potential difference of 0.880 V between the half-wave potential of the ORR and the OER potential at 10 mA cm–2, exceeding the majority of perovskite bifunctional catalysts. Further analysis of the electronic structures reveals that hole doping could regulate the eg-orbital filling of the transition-metal cations in high-entropy perovskites to an ideal position and thereby generate many highly active sites to promote the redox activity of oxygen. The assembled rechargeable ZAB with the targeted high-entropy perovskite as the cathode affords a specific capacity of 774.5 mAh gZn–1 under 10 mA cm–2 and durability for a period of 300 cycles, comparable to that of the 20%Pt/C + RuO2 ZAB. This work offers an important approach for the advancement of efficient high-entropy perovskites for ZABs.
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