期刊
ACS APPLIED MATERIALS & INTERFACES
卷 11, 期 50, 页码 46756-46766出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b15537
关键词
ionothermal copolymerization; tetracyanoquinodimethane (TCNQ); polymeric carbon nitride (PCN); hydrogen evolution rate (HER); oxygen evolution rate (OER); full water splitting
资金
- University Grants Commission (UGC) Major Research Project (MRP) [37-171/2009(SR)]
- Basic Scientific Research (BRNS) [F25-1/2013-14(BSR)/7-226/2009]
- New Delhi, India
Photocatalytic full water splitting remains the perfect way to generate oxygen (O-2) and hydrogen (H-2) gases driven by sunlight to address the future environmental issues as well as energy demands. Owing to its exceptional properties, polymeric carbon nitride (PCN) has been one of the most widely investigated semiconductor photocatalysts. Nevertheless, blank PCN characteristically displays restrained photocatalytic performance due to high-density defects in its framework that may perhaps perform the part of the recombination midpoint for photoproduced electron-hole pairs. Therefore, to overcome this problem, a simple approach to introduce 7,7,8,8-tetracyanoquinodimethane (TCNQ) with an electron-withdrawing characteristic modifier into the pristine PCN framework by the ionothermal method to enhance its optical, conductive, and photocatalytic properties has been undertaken. Results show that such integration of TCNQ results in the delocalization of the pi-conjugated structure; significant changes in its chemical electronic configuration, band gap, and surface area; and enhanced production of electrons under visible light. As a result of this facile integration, our best sample (CNU-TCNQ(9.0)) produced a hydrogen evolution rate (HER) of 164.6 mu mol h(-1) for H-2 and an oxygen evolution rate (OER) of 14.8 mu mol h(-1) for O-2, which were found to be 2.4- and 2.6-fold greater than those produced with pure carbon nitride (CNU) sample, respectively. Hence, this work provides a reasonable alternative method to synthesize and design novel CNU-TCNQ backbone photocatalyst for organic photosynthesis, CO2 reduction, hydrogen evolution, etc.
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