Abstract

The use of photocatalysts to purify wastewater and simultaneously convert solar energy into clean hydrogen energy is of considerable significance in environmental science. However, it is still a challenge due to their relatively high costs, low efficiencies, and poor stabilities. In this study, a metal-free carbon quantum dots (CQDs) modified graphitic carbon nitride photocatalyst (CCN) was synthesized by a facile method. The characterization and theoretical calculation results reveal that the incorporation of CQDs into the g-C3N4 matrix significantly improves the charge transfer and separation efficiency, exhibits a redshift of absorption edge, narrows the bandgap, and prevents the recombination of photoexcited carriers. The hydrogen production and simultaneous degradation of methylene blue (MB) or rhodamine B (RhB) in simulated wastewaters were further tested. In the simulated wastewater, the CCN catalyst showed enhanced photodegradation efficiency, accompanied with the increased hydrogen evolution rate (1291 µmol·h−1·g−1). The internal electrical field between the g-C3N4 and the CQDs is the main reason for the spatial separation of photoexcited electron-hole pairs. Overall, this work could offer a new protocol for the design of highly efficient photocatalysts for dye wastewater purification with simultaneous hydrogen production.

Highlights

  • The application of photocatalysts to purify wastewater with simultaneous hydrogen production has received persistent interest [1]

  • Since the report of Wang and Domen documented that a polymer semiconductor based on defective graphitic carbon nitride (g-C3N4) owns the performance of hydrogen evolution from water [7], the research towards this promising nontoxic metal-free photocatalyst has attracted considerable attention, due to its facile synthesis, visible-light responding energy gap (Eg = 2.68 eV), high physicochemical stability, and “earth-abundant” nature [8,9]

  • The TG and DTG analytical results (Figure S1 in Supporting Materials) indicated that the synthesized carbon quantum dots (CQDs) were stable under nitrogen

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Summary

Introduction

The application of photocatalysts to purify wastewater with simultaneous hydrogen production has received persistent interest [1]. Current photocatalysts still have several fundamental problems that need to be solved, such as low photoabsorption efficiency (which leads to the low quantum efficiency), high electron-hole recombination rate, high cost, and poor stability [6] It still needs a follow-up study to solve these defects and develop an efficient photocatalyst. G-C3N4 is fabricated by thermal polymerization of abundant nitrogen-rich precursors such as melamine [9], dicyandiamide [10], cyanamide [11], urea [12], thiourea, and ammonium thiocyanate [13] This material has enormous application potential, such as organic pollutant degradation [14]. To the best of our knowledge, only a few reports have studied both the theoretical basis and the possible applications in dye wastewater purification with simultaneous hydrogen production [22,23,24]

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