Dual roles of [NCN]2- on anatase TiO2: A fully occupied molecular gap state for direct charge injection into the conduction band and an interfacial mediator for the covalent formation of heterostructured g-C3N4/a-TiO2 nanocomposite
[Display omitted] •The strategy of low melamine/TiO2 ratio isolates a NCN2−—TiO2 transient species.•NCN2−—TiO2 exhibits excellent activities in H2 production, a novel photocatalyst.•Admixture of NCN2− HOMO π2p with Ti 3d upshifts the state into the bandgap of TiO2.•Five-line EPR pattern from a hole...
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| Published in | Applied catalysis. B, Environmental Vol. 273; p. 119036 |
|---|---|
| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Amsterdam
Elsevier B.V
15.09.2020
Elsevier BV |
| Subjects | |
| Online Access | Get full text |
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| Abstract | [Display omitted]
•The strategy of low melamine/TiO2 ratio isolates a NCN2−—TiO2 transient species.•NCN2−—TiO2 exhibits excellent activities in H2 production, a novel photocatalyst.•Admixture of NCN2− HOMO π2p with Ti 3d upshifts the state into the bandgap of TiO2.•Five-line EPR pattern from a hole at NCN1−—TiO2, authentication of a gap state.•Heterostructured g-C3N4/TiO2 formation proceeds via the intermediacy of NCN2−—TiO2.
When low density of melamine is calcined with a-TiO2 at 550 °C, two FT-IR peaks observed at 2048 and 2066 cm−1 are assigned to NCN2- covalently attached to a five-coordinated Ti atom and an oxygen vacancy, respectively, complemented by DFT computation. Admixture of NCN2- HOMO(π2p, 87.5 %) with the high energy Ti(3d, 12.5 %) destabilizes and upshifts the NCN2- HOMO into the a-TiO2 bandgap. A five-line EPR pattern derived from 71 % of atomic spin density localized on two equivalent 14N nuclei, observed under sub-bandgap excitation, verifies the presence of a molecular gap-state. The NCN2--a-TiO2 exhibits excellent H2 production at a rate of 5101 μmol.h-1.g-1. Upon increasing melamine concentration, the rapid and simultaneous decreases of NCN2- FT-IR and NCN1- EPR signals accompanied by transitions of other spectroscopic data to those characteristic of tri-s-triazine demonstrate that the formation of heterostructured g-C3N4/a-TiO2 proceeds via the intermediacy of NCN2--a-TiO2, thereby a mechanism is proposed. |
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| AbstractList | When low density of melamine is calcined with a-TiO2 at 550 °C, two FT-IR peaks observed at 2048 and 2066 cm−1 are assigned to NCN2- covalently attached to a five-coordinated Ti atom and an oxygen vacancy, respectively, complemented by DFT computation. Admixture of NCN2- HOMO(π2p, 87.5 %) with the high energy Ti(3d, 12.5 %) destabilizes and upshifts the NCN2- HOMO into the a-TiO2 bandgap. A five-line EPR pattern derived from 71 % of atomic spin density localized on two equivalent 14N nuclei, observed under sub-bandgap excitation, verifies the presence of a molecular gap-state. The NCN2--a-TiO2 exhibits excellent H2 production at a rate of 5101 μmol.h-1.g-1. Upon increasing melamine concentration, the rapid and simultaneous decreases of NCN2- FT-IR and NCN1- EPR signals accompanied by transitions of other spectroscopic data to those characteristic of tri-s-triazine demonstrate that the formation of heterostructured g-C3N4/a-TiO2 proceeds via the intermediacy of NCN2--a-TiO2, thereby a mechanism is proposed. [Display omitted] •The strategy of low melamine/TiO2 ratio isolates a NCN2−—TiO2 transient species.•NCN2−—TiO2 exhibits excellent activities in H2 production, a novel photocatalyst.•Admixture of NCN2− HOMO π2p with Ti 3d upshifts the state into the bandgap of TiO2.•Five-line EPR pattern from a hole at NCN1−—TiO2, authentication of a gap state.•Heterostructured g-C3N4/TiO2 formation proceeds via the intermediacy of NCN2−—TiO2. When low density of melamine is calcined with a-TiO2 at 550 °C, two FT-IR peaks observed at 2048 and 2066 cm−1 are assigned to NCN2- covalently attached to a five-coordinated Ti atom and an oxygen vacancy, respectively, complemented by DFT computation. Admixture of NCN2- HOMO(π2p, 87.5 %) with the high energy Ti(3d, 12.5 %) destabilizes and upshifts the NCN2- HOMO into the a-TiO2 bandgap. A five-line EPR pattern derived from 71 % of atomic spin density localized on two equivalent 14N nuclei, observed under sub-bandgap excitation, verifies the presence of a molecular gap-state. The NCN2--a-TiO2 exhibits excellent H2 production at a rate of 5101 μmol.h-1.g-1. Upon increasing melamine concentration, the rapid and simultaneous decreases of NCN2- FT-IR and NCN1- EPR signals accompanied by transitions of other spectroscopic data to those characteristic of tri-s-triazine demonstrate that the formation of heterostructured g-C3N4/a-TiO2 proceeds via the intermediacy of NCN2--a-TiO2, thereby a mechanism is proposed. |
| ArticleNumber | 119036 |
| Author | Chen, Jun-Ru Maity, Amarendra N. Nimbalkar, Dipak B. Sahoo, Smruti R. Chang, Chun-Ming Ke, Shyue-Chu Ramacharyulu, P.V.R.K. |
| Author_xml | – sequence: 1 givenname: Dipak B. surname: Nimbalkar fullname: Nimbalkar, Dipak B. – sequence: 2 givenname: P.V.R.K. surname: Ramacharyulu fullname: Ramacharyulu, P.V.R.K. – sequence: 3 givenname: Smruti R. surname: Sahoo fullname: Sahoo, Smruti R. – sequence: 4 givenname: Jun-Ru surname: Chen fullname: Chen, Jun-Ru – sequence: 5 givenname: Chun-Ming surname: Chang fullname: Chang, Chun-Ming – sequence: 6 givenname: Amarendra N. surname: Maity fullname: Maity, Amarendra N. – sequence: 7 givenname: Shyue-Chu surname: Ke fullname: Ke, Shyue-Chu email: ke@gms.ndhu.edu.tw |
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•The strategy of low melamine/TiO2 ratio isolates a NCN2−—TiO2 transient species.•NCN2−—TiO2 exhibits excellent activities in H2 production,... When low density of melamine is calcined with a-TiO2 at 550 °C, two FT-IR peaks observed at 2048 and 2066 cm−1 are assigned to NCN2- covalently attached to a... |
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| SubjectTerms | Anatase Carbon nitride Charge injection Conduction Conduction bands Density Energy gap EPR g-C3N4 H2 production Hydrogen production Mechanism Melamine Nanocomposites Photocatalyst TiO2 Titanium dioxide Triazine |
| Title | Dual roles of [NCN]2- on anatase TiO2: A fully occupied molecular gap state for direct charge injection into the conduction band and an interfacial mediator for the covalent formation of heterostructured g-C3N4/a-TiO2 nanocomposite |
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