Facilitating Molecular Activation and Proton Feeding by Dual Active Sites on Polymeric Carbon Nitride for Efficient CO2 Photoreduction.
Angew Chem Int Ed Engl
; 61(46): e202212706, 2022 Nov 14.
Article
de En
| MEDLINE
| ID: mdl-36138516
ABSTRACT
Photoreduction of CO2 provides an appealing way to alleviate the energy crisis and manage the global carbon balance but is limited by the high activation energy and the rate-limiting proton transfer. We now develop a dual-site strategy for high-efficiency CO2 conversion through polarizing CO2 molecules at pyridine N vacancies and accelerating the intermediate protonation by protonated pyridine N adjacent to nitrogen vacancies on polymeric carbon nitride. Our photocatalysts with atomic-level engineered active sites manifest a high CO production rate of 1835â
µmol g-1 h-1 , 183 times higher than the pristine bulk carbon nitride. Theoretical prediction and experimental studies confirm that such excellent performance is attributed to the synergistic effect between vacant and protonated pyridine N in decreasing the formation energy of the key *COOH intermediates and the efficient electron transfer relay facilitated by the defect-induced shallow trap state and homogeneous charge mediators.
Texte intégral:
1
Collection:
01-internacional
Base de données:
MEDLINE
Langue:
En
Journal:
Angew Chem Int Ed Engl
Année:
2022
Type de document:
Article
Pays d'affiliation:
Chine