Microscopic Revelation of Charge-Trapping Sites in Polymeric Carbon Nitrides for Enhanced Photocatalytic Activity by Correlating with Chemical and Electronic Structures
Source abstract
Abstract
The influences of chemical and electronic structures on the photophysical properties of polymeric carbon nitrides (PCNs) photocatalysts, which govern the microscopic mechanisms of the superior photocatalytic activity under visible-light irradiation, have been resolved in this work. Time-resolved photoluminescence and in situ electron paramagnetic resonance measurements indicate that the photoexcited electrons in the fractured PCNs swiftly transfer to the C2p-localized states where the trapped photoelectrons exhibit longer lifetime compared to those in the ordinary PCNs. Moreover, the structure deviation at the carbon (Cb) atoms around the bridging sites of heptazine ring units, where trapped photoelectrons are localized, has been determined in the fractured PCNs based on the 13C solid-state nuclear magnetic resonance spectra and the density functional theory calculations. Accordingly, the formation of fractured PCNs by breaking the in-plane hydrogen bonds at a high temperature is a promising strategy for the enhancement of photocatalytic activity.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Advanced Photocatalysis Techniques · Gas Sensing Nanomaterials and Sensors · Ga2O3 and related materials
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Department of Chemical Engineering, National Cheng Kung University, Tainan 70101, Taiwan
Department of Physics, National Dong Hwa University, Hualien 97401, Taiwan
Department of Physical Chemistry and Molecular Modeling, Opole University, Opole 45052, Poland
Funding
Ministry of Science and Technology, Taiwan · Wroclaw Centre for Networking and Supercomputing
References (53)
Show source-provided references
1. 10.1038/nmat231710.1038/nmat2317 ↗
2. 10.1021/acs.chemrev.6b0007510.1021/acs.chemrev.6b00075 ↗
3. 10.1039/c2ee03479d10.1039/c2ee03479d ↗
4. 10.1039/C5CS00767D10.1039/C5CS00767D ↗
5. 10.1021/ja809307s10.1021/ja809307s ↗
6. 10.1039/C6CP02453J10.1039/C6CP02453J ↗
7. 10.1002/adma.20150003310.1002/adma.201500033 ↗
8. 10.1021/ja308249k10.1021/ja308249k ↗
9. 10.1021/jp510187c10.1021/jp510187c ↗
10. 10.1021/jp711483t10.1021/jp711483t ↗
11. 10.1021/acs.chemmater.7b0096510.1021/acs.chemmater.7b00965 ↗
12. 10.1021/jacs.6b1187810.1021/jacs.6b11878 ↗
13. 10.1002/aenm.20160225110.1002/aenm.201602251 ↗
14. 10.1038/ncomms1216510.1038/ncomms12165 ↗
15. 10.1021/jacs.7b0154710.1021/jacs.7b01547 ↗
16. 10.1021/acs.accounts.8b0054210.1021/acs.accounts.8b00542 ↗
17. 10.1039/C7CY01623A10.1039/C7CY01623A ↗
18. 10.1021/cm500034p10.1021/cm500034p ↗
19. 10.1039/C4NR07645A10.1039/C4NR07645A ↗
20. 10.1039/C4RA16362A10.1039/C4RA16362A ↗
21. 10.1103/PhysRevLett.77.386510.1103/PhysRevLett.77.3865 ↗
22. 10.1039/C2CS35394F10.1039/C2CS35394F ↗
23. 10.1103/PhysRevB.37.78510.1103/PhysRevB.37.785 ↗
24. 10.1021/ct800013z10.1021/ct800013z ↗
25. Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Scalmani, G.; Barone, V.; Petersson, G. A.; Nakatsuji, H.; Li, X.; Caricato, M.; Marenich, A. V.; Bloino, J.; Janesko, B. G.; Gomperts, R.; Mennucci, B.; Hratchian, H. P.; Ortiz, J. V.; Izmaylov, A. F.; Sonnenberg, J. L.; Williams; Ding, F.; Lipparini, F.; Egidi, F.; Goings, J.; Peng, B.; Petrone, A.; Henderson, T.; Ranasinghe, D.; Zakrzewski, V. G.; Gao, J.; Rega, N.; Zheng, G.; Liang, W.; Hada, M.; Ehara, M.; Toyota, K.; Fukuda, R.; Hasegawa, J.; Ishida, M.; Nakajima, T.; Honda, Y.; Kitao, O.; Nakai, H.; Vreven, T.; Throssell, K.; Montgomery, J. A., Jr.; Peralta, J. E.; Ogliaro, F.; Bearpark, M. J.; Heyd, J. J.; Brothers, E. N.; Kudin, K. N.; Staroverov, V. N.; Keith, T. A.; Kobayashi, R.; Normand, J.; Raghavachari, K.; Rendell, A. P.; Burant, J. C.; Iyengar, S. S.; Tomasi, J.; Cossi, M.; Millam, J. M.; Klene, M.; Adamo, C.; Cammi, R.; Ochterski, J. W.; Martin, R. L.; Morokuma, K.; Farkas, O.; Foresman, J. B.; Fox, D. J. Gaussian 16, revision. B.01; Gaussian Inc.: Wallingford, CT, 2016.
26. 10.1021/acs.chemmater.7b0531610.1021/acs.chemmater.7b05316 ↗
27. 10.1021/acs.chemmater.5b0041110.1021/acs.chemmater.5b00411 ↗
28. 10.1088/0953-8984/24/16/16220110.1088/0953-8984/24/16/162201 ↗
29. 10.1002/chem.20060175910.1002/chem.200601759 ↗
30. 10.1103/PhysRevB.87.20520410.1103/PhysRevB.87.205204 ↗
31. 10.1021/acs.chemmater.8b0074010.1021/acs.chemmater.8b00740 ↗
32. 10.1088/0953-8984/25/39/39540210.1088/0953-8984/25/39/395402 ↗
33. 10.1016/j.apsusc.2015.08.03510.1016/j.apsusc.2015.08.035 ↗
34. 10.1016/j.apsusc.2016.07.03010.1016/j.apsusc.2016.07.030 ↗
35. 10.1002/adfm.20120092210.1002/adfm.201200922 ↗
36. 10.1021/acscatal.6b0092210.1021/acscatal.6b00922 ↗
37. 10.1002/anie.20170687010.1002/anie.201706870 ↗
38. 10.1016/j.apsusc.2018.07.16410.1016/j.apsusc.2018.07.164 ↗
39. 10.1016/j.apcatb.2014.07.05310.1016/j.apcatb.2014.07.053 ↗
40. 10.1021/ja103798k10.1021/ja103798k ↗
41. 10.1021/jp503477x10.1021/jp503477x ↗
42. 10.1002/ange.20180227810.1002/ange.201802278 ↗
43. 10.1021/ja511802c10.1021/ja511802c ↗
44. 10.1021/cm503258z10.1021/cm503258z ↗
45. 10.1039/C2CS35305A10.1039/C2CS35305A ↗
46. 10.1063/1.200981710.1063/1.2009817 ↗
47. 10.1021/acs.chemmater.7b0006910.1021/acs.chemmater.7b00069 ↗
48. 10.1021/ja035768910.1021/ja0357689 ↗
49. 10.1021/jp072001k10.1021/jp072001k ↗
50. 10.1039/b919918g10.1039/b919918g ↗
51. 10.1002/adma.20150193910.1002/adma.201501939 ↗
52. 10.1002/adma.20160156710.1002/adma.201601567 ↗
53. 10.1021/acsnano.7b0810010.1021/acsnano.7b08100 ↗