Improved Visible-Light Photocatalytic H2 Evolution of G-C3N4 Nanosheets by Constructing Heterojunctions with Nano-Sized Poly(3-Thiophenecarboxylic Acid) and Coordinating Fe(III)

Author:

Li Yong12,Zhang Bingmiao1,Pang Xulong1,Li Zhijun1,Zhang Yi1,Hao Ming1,Zhu Yan1,Qin Chuanli1,Jing Liqiang1ORCID

Affiliation:

1. Key Laboratory of Functional Inorganic Material Chemistry (Ministry of Education), School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, China

2. Engineering Research Center for Hemp and Product in Cold Region of Ministry of Education, Qiqihar University, Qiqihar 161006, China

Abstract

It is highly desirable to enhance the photogenerated charge separation of g-C3N4 by constructing efficient heterojunctions, especially with an additional organic constitution for solar–hydrogen conversion. Herein, g-C3N4 nanosheets have been modified controllably with nano-sized poly(3-thiophenecarboxylic acid) (PTA) through in situ photopolymerization and then coordinated with Fe(III) via the -COOH groups of modified PTA, forming an interface of tightly contacted nanoheterojunctions between the Fe(III)-coordinated PTA and g-C3N4. The resulting ratio-optimized nanoheterojunction displays a ~4.6-fold enhancement of the visible-light photocatalytic H2 evolution activity compared to bare g-C3N4. Based on the surface photovoltage spectra, measurements of the amount of •OH produced, photoluminescence (PL) spectra, photoelectrochemical curves, and single-wavelength photocurrent action spectra, it was confirmed that the improved photoactivity of g-C3N4 is attributed to the significantly promoted charge separation by the transfer of high-energy electrons from the lowest unoccupied molecular orbital (LUMO) of g-C3N4 to the modified PTA via the formed tight interface, dependent on the hydrogen bond interaction between the -COOH of PTA and the -NH2 of g-C3N4, and the continuous transfer to the coordinated Fe(III) with -OH favorable for connection with Pt as the cocatalyst. This study demonstrates a feasible strategy for solar-light-driven energy production over the large family of g-C3N4 heterojunction photocatalysts with exceptional visible-light activities.

Funder

National Natural Science Foundation of China

the Joint guidance project of Natural Science Foundation of Heilongjiang Province

Publisher

MDPI AG

Subject

General Materials Science,General Chemical Engineering

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