TY - JOUR
T1 - Interfacial coupling perovskite CeFeO3 on layered graphitic carbon nitride as a multifunctional Z-scheme photocatalyst for boosting nitrogen fixation and organic pollutants demineralization
AU - Choong, Choe Earn
AU - Park, Chang Min
AU - Chang, Yoon Young
AU - Yang, Jae kyu
AU - Kim, Jung Rae
AU - Oh, Sang Eun
AU - Jeon, Byong Hun
AU - Choi, Eun Ha
AU - Yoon, Yeomin
AU - Jang, Min
N1 - Publisher Copyright:
© 2021 Elsevier B.V.
PY - 2022/1/1
Y1 - 2022/1/1
N2 - The application of pristine graphitic carbon nitride (PCN, g-C3N4)/cerium ferrite (CeFeO3, CFO) composites as photocatalysts for energy production and water treatment has not yet been reported despite its great potential. In this study, CFO, an orthorhombic perovskite-type oxide, was covalently coupled to PCN via a facile single-step calcination strategy. Compared to PCN, optimized 1% CFO-doped PCN (PCN@CFO1) exhibited wide ranges of organic-micropollutant removal (sulfamethoxazole (SMX), atrazine, and bisphenol A) and achieved approximately 49.9% of total-organic-carbon (TOC) removal for SMX in 4 h with 5 stable reusable performances. Further, scavenger experiments and the electron paramagnetic resonance (EPR) spin-trap analysis revealed that PCN@CFO1 could produce superoxide (O2−[rad]) and hydroxyl radicals ([rad]OH) for organic-pollutant degradation. Meanwhile, the intermediate species of organic pollutants were investigated using liquid chromatography-tandem mass spectrometry to identify the degradation pathways. Of note, PCN@CFO1 achieved up to 573.12 µmol l−1 g−1 of ammonia production rate and 2.92% of apparent quantum efficiency of nitrogen photo-fixation at 400 nm, which was 8 times higher than that of PCN. Through coupling CFO and PCN, the flat band potential was found to be upshifted, and a high ratio of the Ce3+ interface associated with oxygen vacancies was generated, resulting in the formation of a Z-scheme system. Remarkably, the formation of the Z-scheme structure on PCN@CFO1 showed enhancement in charge transfer, hydrophilicity, and charge separation, significantly improving the photocatalytic performance for organic-micropollutant demineralization and nitrogen photo-fixation under UVA-LED (400 nm) light irradiation. Our study provided a facile and scalable preparation strategy for multifunctional photocatalysts that could be effectively activated under energy-efficient UVA-LED irradiation for energy production and emerging pollutants degradation.
AB - The application of pristine graphitic carbon nitride (PCN, g-C3N4)/cerium ferrite (CeFeO3, CFO) composites as photocatalysts for energy production and water treatment has not yet been reported despite its great potential. In this study, CFO, an orthorhombic perovskite-type oxide, was covalently coupled to PCN via a facile single-step calcination strategy. Compared to PCN, optimized 1% CFO-doped PCN (PCN@CFO1) exhibited wide ranges of organic-micropollutant removal (sulfamethoxazole (SMX), atrazine, and bisphenol A) and achieved approximately 49.9% of total-organic-carbon (TOC) removal for SMX in 4 h with 5 stable reusable performances. Further, scavenger experiments and the electron paramagnetic resonance (EPR) spin-trap analysis revealed that PCN@CFO1 could produce superoxide (O2−[rad]) and hydroxyl radicals ([rad]OH) for organic-pollutant degradation. Meanwhile, the intermediate species of organic pollutants were investigated using liquid chromatography-tandem mass spectrometry to identify the degradation pathways. Of note, PCN@CFO1 achieved up to 573.12 µmol l−1 g−1 of ammonia production rate and 2.92% of apparent quantum efficiency of nitrogen photo-fixation at 400 nm, which was 8 times higher than that of PCN. Through coupling CFO and PCN, the flat band potential was found to be upshifted, and a high ratio of the Ce3+ interface associated with oxygen vacancies was generated, resulting in the formation of a Z-scheme system. Remarkably, the formation of the Z-scheme structure on PCN@CFO1 showed enhancement in charge transfer, hydrophilicity, and charge separation, significantly improving the photocatalytic performance for organic-micropollutant demineralization and nitrogen photo-fixation under UVA-LED (400 nm) light irradiation. Our study provided a facile and scalable preparation strategy for multifunctional photocatalysts that could be effectively activated under energy-efficient UVA-LED irradiation for energy production and emerging pollutants degradation.
KW - Carbon graphitic nitride
KW - Perovskite
KW - Photocatalysis
KW - Z-scheme
UR - http://www.scopus.com/inward/record.url?scp=85112848867&partnerID=8YFLogxK
U2 - 10.1016/j.cej.2021.131406
DO - 10.1016/j.cej.2021.131406
M3 - Article
AN - SCOPUS:85112848867
SN - 1385-8947
VL - 427
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 131406
ER -