Grafting anthraquinone on ultrathin C3N4 for selective toluene photooxidation
摘要
Anthraquinone (AQ), an effective hydrogen atom transfer catalyst, is limited in photocatalytic applications due to its dimerization. In this study, a simple 3-(3-(dimethylamino) propyl)-1-ethylcarbodiimide hydrochloride/N-hydroxysuccinimide (EDC/HNS) assisted linking strategy was developed to covalently graft AQ–COOH onto C3N4 (CN). Using this method, we successfully synthesized amide-bonded CN–AQ ultrathin nanosheets. The amide covalent bond formed between C3N4 and AQ facilitates efficient electron migration from C3N4 to AQ. As a result, charge carrier recombination is prevented and the hydrogen atom transfer capacity of AQ is enhanced. The CN–AQ photocatalyst exhibits high activity and selectivity with a toluene conversion rate of 10274 (mol g−1 h−1 and 85% selectivity for benzaldehyde, which is 31 times and 1.7 times higher than those of pristine C3N4 and AQ–COOH, respectively. Owing to the strong covalent bond in CN–AQ composite, the stability of AQ–COOH was greatly enhanced. This approach provides a new pathway to improve catalytic efficiency and solve the dimerization problem of AQ.