文献类型：期刊文献

英文题名：Bronsted base site engineering of graphitic carbon nitride for enhanced photocatalytic activity

作者：Wang, Xue Lu[1];Fang, Wen Qi[1];Liu, Wenqing[3];Jia, Yi[2];Jing, Dengwei[6];Wang, Yun[5];Yang, Ling-Yun[3];Gong, Xue-Qing[4];Yao, Ye-Feng[3,7];Yang, Hua Gui[1];Yao, Xiangdong[2]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Key Lab Ultrafine Mat, Minist Educ, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Griffith Univ, Sch Nat Sci, Nathan, Qld 4111, Australia;[3]East China Normal Univ, Shanghai Key Lab Magnet Resonance, Phys Dept, Shanghai 200062, Peoples R China;[4]East China Univ Sci & Technol, Ctr Computat Chem, Res Inst Ind Catalysis, Key Lab Adv Mat, Shanghai 200037, Peoples R China;[5]Griffith Univ, Ctr Clean Environm & Energy, Gold Coast Campus, Nathan, Qld 4222, Australia;[6]Xi An Jiao Tong Univ, State Key Lab Multiphase Flow Power Engn, Int Res Ctr Renewable Energy, Xian 710049, Shaanxi, Peoples R China;[7]NYU Shanghai, NYU ECNU Inst Phys, 3663 Zhongshan Rd North, Shanghai 200062, Peoples R China

年份：2017

卷号：5

期号：36

起止页码：19227

外文期刊名：JOURNAL OF MATERIALS CHEMISTRY A

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000411232100035)】；

基金：This work was financially supported by the National Natural Science Foundation of China (21573068, 21574043 and 21603073), Fundamental Research Funds for the Central Universities (222201514303), Program of Shanghai Subject Chief Scientist (15XD1501300), China Postdoctoral Science Foundation Funded Project (2016M591615 and 2017T100276), National High-tech R&D Program of China (863 Program) (2014AA123400 and 2014AA123401) and National Key Basic Research Program of China (973 program) (Grant No. 2013CB921801). The authors also thank the crew of the 1W1B beamline of the Beijing Synchrotron Radiation Facility for the constructive assistance in the XAFS measurements and data analyses.

语种：英文

摘要：Graphitic carbon nitride (g-C3N4) is a promising two-dimensional polymeric photocatalyst in the field of solar energy conversion. In the past few years many modifications of g-C3N4 have been studied extensively; however, the difficulty in obtaining detailed structural information both on its intrinsic covalent interactions and surrounding bonding environments largely restricts the rational design and development of inherent structure-controlled g-C3N4 based photocatalysts and fundamental understanding of their mechanistic operations. Herein, we demonstrate a high-pressure hydrogenation treatment method for g-C3N4 and introduce 1D C-13 and N-15 and 2D N-15 Radio Frequency-driven Dipolar Recoupling (RFDR) solid-state nuclear magnetic resonance spectroscopy for identifying the structural information and surrounding hydrogen-bonding environment of treated g-C3N4 samples. The surface Bronsted base sites of g-C3N4 samples can be tuned systematically through changing the treatment conditions. We find that the terminal isolated -NH2 and the hydrogenated nitrogen species in treated gC(3)N(4) samples seem to be the origin of their improved activities for photocatalytic hydrogen evolution and favor the enhancement of light harvesting and carrier transport. The as-prepared HCN400-4-2 sample treated at a pressure of 4 MPa and a temperature of 400 degrees C for 2 h in a hydrogen atmosphere displays the highest H-2 evolution reaction (HER) activity, which is over 26 times higher than that of pristine g-C3N4.