Assembly of g-C3N4-based type II and Z-scheme heterojunction anodes with improved charge separation for photoelectrojunction water oxidation

Document Type

Article

Publication Date

1-1-2017

Abstract

Graphitic carbon nitride (g-C3N4) has been widely studied as a metal-free photocatalyst, leading to some excellent results; however, the rapid recombination of photogenerated charge carriers substantially limits its performance. Here, we establish two types of g-C3N4-based heterojunction (type II and nonmediator assisted Z-scheme) photoanodes on a transparent conducting substrate via coupling with rod-like and nanoparticulate WO3, respectively. In these composites, g-C3N4 film grown by electrophoretic deposition of exfoliated g-C3N4 serves as the host or guest material. The optimized type II WO3/g-C3N4 composite exhibits an enhanced photocurrent of 0.82 mA cm-2 at 1.23 V vs. RHE and an incident photo-to-current conversion efficiency (IPCE) of 33% as compared with pure WO3 nanorods (0.22 mA cm-2 for photocurrent and 15% for IPCE). Relative to pure g-C3N4 film (with a photocurrent of several microampere and an IPCE of 2%), a largely improved photocurrent of 0.22 mA cm-2 and an IPCE of 20% were acquired for the Z-scheme g-C3N4/WO3 composite. The enhancement can be attributed to accelerated charge separation in the heterointerface because of the suitably aligned band gap between WO3 and g-C3N4, as confirmed by optical spectroscopy and ultraviolet photoelectron spectroscopy (UPS) analysis. The photocatalytic process and mechanism of the g-C3N4-based heterojunctions are proposed herein, which potentially explain the origin of the enhanced photoelectrochemical performance. This achievement and the fundamental information supplied here indicate the importance of rationally designing heterojunction photoelectrodes to improve the performance of semiconductors. This is particularly important for materials such as pure g-C3N4 and WO3, as their photoactivities are strongly restricted by high recombination rates.

Identifier

85013754135 (Scopus)

Publication Title

Physical Chemistry Chemical Physics

External Full Text Location

https://doi.org/10.1039/c6cp08066a

ISSN

14639076

PubMed ID

28120968

First Page

4507

Last Page

4515

Issue

6

Volume

19

Grant

1210RJIA001

Fund Ref

National Natural Science Foundation of China

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