Efficient charge separation and rapid interfacial reaction kinetics are crucial factors that determine the efficiency of photocatalytic hydrogen evolution.Herein,a fascinating 2D heterojunction photocatalyst with supe...Efficient charge separation and rapid interfacial reaction kinetics are crucial factors that determine the efficiency of photocatalytic hydrogen evolution.Herein,a fascinating 2D heterojunction photocatalyst with superior photocatalytic hydrogen evolution performance–holey C_(3)N_(4)nanosheets nested with TiO_(2)nanocrystals(denoted as HCN/TiO_(2))–is designed and fabricated via an in situ exfoliation and conversion strategy.The HCN/TiO_(2)is found to exhibit an ultrathin 2D heteroarchitecture with intimate interfacial contact,highly porous structures and ultrasmall TiO_(2)nanocrystals,leading to drastically improved charge carrier separation,maximized active sites and the promotion of mass transport for photocatalysis.Consequently,the HCN/TiO_(2)delivers an impressive hydrogen production rate of 282.3 lmol h^(-1)per10 mg under AM 1.5 illumination and an apparent quantum efficiency of 13.4%at a wavelength of 420 nm due to the synergetic enhancement of surface reactions and charge separation.The present work provides a promising strategy for developing high-performance 2D heterojunctions for clean energy applications.展开更多
基金the National Key R&D Program of China(2018YFE0201704 and 2018YFE0201701)the National Natural Science Foundation of China(21673256,21533011,2163100,and 21603036)Shanghai Rising-Star Program.
文摘Efficient charge separation and rapid interfacial reaction kinetics are crucial factors that determine the efficiency of photocatalytic hydrogen evolution.Herein,a fascinating 2D heterojunction photocatalyst with superior photocatalytic hydrogen evolution performance–holey C_(3)N_(4)nanosheets nested with TiO_(2)nanocrystals(denoted as HCN/TiO_(2))–is designed and fabricated via an in situ exfoliation and conversion strategy.The HCN/TiO_(2)is found to exhibit an ultrathin 2D heteroarchitecture with intimate interfacial contact,highly porous structures and ultrasmall TiO_(2)nanocrystals,leading to drastically improved charge carrier separation,maximized active sites and the promotion of mass transport for photocatalysis.Consequently,the HCN/TiO_(2)delivers an impressive hydrogen production rate of 282.3 lmol h^(-1)per10 mg under AM 1.5 illumination and an apparent quantum efficiency of 13.4%at a wavelength of 420 nm due to the synergetic enhancement of surface reactions and charge separation.The present work provides a promising strategy for developing high-performance 2D heterojunctions for clean energy applications.