Two-dimensional interface engineering of g-C3N4/g-C3N4 nanohybrid: synergy between isotype and p-n heterojunctions for highly efficient photocatalytic CO2 reduction
The creation of an isotype phase junction has been recognized as an effective means of improving the spatial charge separation and migration in g-C3N4 materials. Nevertheless, due to a lack of electrostatic control in the internal electric field, isotype heterojunction alone is incapable of providin...
| Main Authors: | , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2024
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| Online Access: | https://hdl.handle.net/10356/174566 |
| _version_ | 1826118232654741504 |
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| author | Tang, Jie-Yinn Er, Chen-Chen Kong, Xin Ying Ng, Boon-Junn Chew, Yi-Hao Tan, Lling-Lling Abdul Rahman Mohamed Chai, Siang-Piao |
| author2 | School of Chemistry, Chemical Engineering and Biotechnology |
| author_facet | School of Chemistry, Chemical Engineering and Biotechnology Tang, Jie-Yinn Er, Chen-Chen Kong, Xin Ying Ng, Boon-Junn Chew, Yi-Hao Tan, Lling-Lling Abdul Rahman Mohamed Chai, Siang-Piao |
| author_sort | Tang, Jie-Yinn |
| collection | NTU |
| description | The creation of an isotype phase junction has been recognized as an effective means of improving the spatial charge separation and migration in g-C3N4 materials. Nevertheless, due to a lack of electrostatic control in the internal electric field, isotype heterojunction alone is incapable of providing a sufficient driving force to maximize charge carrier transfer. Herein, we present an interface engineering strategy for co-integrating isotype and p-n heterojunctions to fabricate g-C3N4/g-C3N4 nanohybrids using a facile ultrasonic-assisted self-assembly method. The coherent boundary between the two distinct phases of g-C3N4 demonstrates that an intimate 2D interfacial contact can be easily established by π-π stacking interactions because of their high structural similarities and low lattice strain. Furthermore, their compatible and well-matched electronic band structures led to a staggered type II alignment in the lateral heterojunction, which confers the resulting composite with strong redox ability, efficient exciton dissociation, and desirable optoelectronic characteristics beyond those of the two constituents. Essentially, the isotype and p-n heterojunctions work in tandem to create a robust built-in electric field, allowing for effective interfacial charge steering for directional electron migration from BCN to CNx. Benefiting from these merits, the BCN/CNx nanohybrid manifested remarkable CH4 generation from photocatalytic CO2 reduction, outperforming its CNx and BCN counterparts by 1.91 and 6.88-fold, respectively. The midgap states induced by nitrogen defects in CNx also pose a positive effect on the improved photoactivity of the binary composite by acting as an electron reservoir to mediate electron transfer and further impede charge carrier recombination. This proof-of-concept study highlights the significance of interface engineering in charge flow manipulation and utilization for photocatalytic enhancement. |
| first_indexed | 2024-10-01T04:40:00Z |
| format | Journal Article |
| id | ntu-10356/174566 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:40:00Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1745662024-04-05T15:31:44Z Two-dimensional interface engineering of g-C3N4/g-C3N4 nanohybrid: synergy between isotype and p-n heterojunctions for highly efficient photocatalytic CO2 reduction Tang, Jie-Yinn Er, Chen-Chen Kong, Xin Ying Ng, Boon-Junn Chew, Yi-Hao Tan, Lling-Lling Abdul Rahman Mohamed Chai, Siang-Piao School of Chemistry, Chemical Engineering and Biotechnology Engineering Two-dimensional interface engineering Isotype heterojunction The creation of an isotype phase junction has been recognized as an effective means of improving the spatial charge separation and migration in g-C3N4 materials. Nevertheless, due to a lack of electrostatic control in the internal electric field, isotype heterojunction alone is incapable of providing a sufficient driving force to maximize charge carrier transfer. Herein, we present an interface engineering strategy for co-integrating isotype and p-n heterojunctions to fabricate g-C3N4/g-C3N4 nanohybrids using a facile ultrasonic-assisted self-assembly method. The coherent boundary between the two distinct phases of g-C3N4 demonstrates that an intimate 2D interfacial contact can be easily established by π-π stacking interactions because of their high structural similarities and low lattice strain. Furthermore, their compatible and well-matched electronic band structures led to a staggered type II alignment in the lateral heterojunction, which confers the resulting composite with strong redox ability, efficient exciton dissociation, and desirable optoelectronic characteristics beyond those of the two constituents. Essentially, the isotype and p-n heterojunctions work in tandem to create a robust built-in electric field, allowing for effective interfacial charge steering for directional electron migration from BCN to CNx. Benefiting from these merits, the BCN/CNx nanohybrid manifested remarkable CH4 generation from photocatalytic CO2 reduction, outperforming its CNx and BCN counterparts by 1.91 and 6.88-fold, respectively. The midgap states induced by nitrogen defects in CNx also pose a positive effect on the improved photoactivity of the binary composite by acting as an electron reservoir to mediate electron transfer and further impede charge carrier recombination. This proof-of-concept study highlights the significance of interface engineering in charge flow manipulation and utilization for photocatalytic enhancement. Published version This work was financially supported by the Malaysia Research University Network (MRUN) from the Ministry of Higher Education (MOHE) Malaysia (Grant No. 304/PJKIMIA/656501/829K145). 2024-04-02T08:24:17Z 2024-04-02T08:24:17Z 2023 Journal Article Tang, J., Er, C., Kong, X. Y., Ng, B., Chew, Y., Tan, L., Abdul Rahman Mohamed & Chai, S. (2023). Two-dimensional interface engineering of g-C3N4/g-C3N4 nanohybrid: synergy between isotype and p-n heterojunctions for highly efficient photocatalytic CO2 reduction. Chemical Engineering Journal, 466, 143287-. https://dx.doi.org/10.1016/j.cej.2023.143287 1385-8947 https://hdl.handle.net/10356/174566 10.1016/j.cej.2023.143287 2-s2.0-85156252320 466 143287 en Chemical Engineering Journal © 2023 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/). application/pdf |
| spellingShingle | Engineering Two-dimensional interface engineering Isotype heterojunction Tang, Jie-Yinn Er, Chen-Chen Kong, Xin Ying Ng, Boon-Junn Chew, Yi-Hao Tan, Lling-Lling Abdul Rahman Mohamed Chai, Siang-Piao Two-dimensional interface engineering of g-C3N4/g-C3N4 nanohybrid: synergy between isotype and p-n heterojunctions for highly efficient photocatalytic CO2 reduction |
| title | Two-dimensional interface engineering of g-C3N4/g-C3N4 nanohybrid: synergy between isotype and p-n heterojunctions for highly efficient photocatalytic CO2 reduction |
| title_full | Two-dimensional interface engineering of g-C3N4/g-C3N4 nanohybrid: synergy between isotype and p-n heterojunctions for highly efficient photocatalytic CO2 reduction |
| title_fullStr | Two-dimensional interface engineering of g-C3N4/g-C3N4 nanohybrid: synergy between isotype and p-n heterojunctions for highly efficient photocatalytic CO2 reduction |
| title_full_unstemmed | Two-dimensional interface engineering of g-C3N4/g-C3N4 nanohybrid: synergy between isotype and p-n heterojunctions for highly efficient photocatalytic CO2 reduction |
| title_short | Two-dimensional interface engineering of g-C3N4/g-C3N4 nanohybrid: synergy between isotype and p-n heterojunctions for highly efficient photocatalytic CO2 reduction |
| title_sort | two dimensional interface engineering of g c3n4 g c3n4 nanohybrid synergy between isotype and p n heterojunctions for highly efficient photocatalytic co2 reduction |
| topic | Engineering Two-dimensional interface engineering Isotype heterojunction |
| url | https://hdl.handle.net/10356/174566 |
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