title: Significant enhancement of photoreactivity of graphitic carbon nitride catalysts under acidic conditions and the underlying H(+)-mediated mechanism.
abstract: Graphitic carbon nitride (g-C3N4) is an emerging photocatalyst for organic pollutants degradation owing to its excellent stability and metal-free property. In this study, the photocatalytic activity of acidified g-C3N4 (ag-C3N4) was systematically investigated using rhodamine B (rhB) as a model organic pollutant. The results showed the photoreactivity of ag-C3N4 is significantly enhanced with the decrease of pH values. The apparent rate constant (kapp) of rhB degradation over ag-C3N4 is 11.59×10(-3)min(-1) at pH7.0 and it increases to 103.50×10(-3)min(-1) at pH3.0 under visible light. A series of analyses demonstrate that the photodegradation mechanism is a combination of a H(+)-promoted generation of OH and elevation of the redox potential of conduct band of C3N4. The change of surface properties of C3N4 caused by pH variation also affects the degradation of some zwitterionic compounds by changing the adsorption orientation of pollutants. The revealed mechanism of visible light-C3N4-rhB system is meaningful to broaden the usage of C3N4 to the photodegradation of other organic pollutants.
authors.affiliation: CAS Key Laboratory of Urban Pollutant Conversion, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China.
authors.forename: Xue-Song
authors.initials: XS
authors.lastname: Zhang
authors.affiliation: CAS Key Laboratory of Urban Pollutant Conversion, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China.
authors.forename: Ke
authors.initials: K
authors.lastname: Tian
authors.affiliation: CAS Key Laboratory of Urban Pollutant Conversion, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China.
authors.forename: Jian-Yang
authors.initials: JY
authors.lastname: Hu
authors.affiliation: CAS Key Laboratory of Urban Pollutant Conversion, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China. Electronic address: jhong@ustc.edu.cn.
authors.forename: Hong
authors.initials: H
authors.lastname: Jiang
mesh_terms: D000327:Adsorption; D002384:Catalysis; D006863:Hydrogen-Ion Concentration; D008027:Light; D008956:Models, Chemical; D009570:Nitriles / Q000737:chemistry*; D010084:Oxidation-Reduction; D010782:Photolysis; D012235:Rhodamines / Q000032:analysis; D013499:Surface Properties; D014874:Water Pollutants, Chemical / Q000032:analysis*
chemical_list: D009570:Nitriles; D012235:Rhodamines; D014874:Water Pollutants, Chemical; C011206:cyanogen; C029773:rhodamine B
keywords: Degradation; Graphitic carbon; Mechanism; Photocatalyst; Zwitterion