Direct Z‑Scheme Water Splitting Photocatalyst Based on Two-Dimensional Van Der Waals Heterostructures
Mimicking the natural photosynthesis in plants, Z-scheme water splitting is a promising strategy to improve photocatalytic activity. Searching for the direct Z-scheme photocatalysts is urgent and the crucial factor for the photocatalytic efficiency is the photogenerated electron–hole (e–h) recombina...
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| Published in | The journal of physical chemistry letters Vol. 9; no. 18; pp. 5419 - 5424 |
|---|---|
| Main Authors | , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
20.09.2018
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| Online Access | Get full text |
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| Abstract | Mimicking the natural photosynthesis in plants, Z-scheme water splitting is a promising strategy to improve photocatalytic activity. Searching for the direct Z-scheme photocatalysts is urgent and the crucial factor for the photocatalytic efficiency is the photogenerated electron–hole (e–h) recombination rate at the interface of two photosystems. In this report, based on time-dependent ab initio nonadiabatic molecular dynamics (NAMD) investigation, we first report a two-dimensional (2D) metal-free van der Waals (vdW) heterostructure consisting of monolayer BCN and C2N as a promising candidate for direct Z-scheme photocatalysts for water splitting. It is shown that the time scale of e–h recombination of BCN/C2N is within 2 ps. Among such e–h recombination events, more than 85% are through the e–h recombination at the interface. NAMD simulations based on frozen phonon method prove that such an ultrafast interlayer e–h recombination is assisted by intralayer optical phonon modes and the interlayer shear phonon mode induced by vdW interaction. In these crucial phonon modes, the interlayer relative movements which are lacking in traditional heterostructures with strong interactions, yet exist generally in various 2D vdW heterostructures, are significant. Our results prove that the 2D vdW heterostructure family is convincing for a new type of direct Z-scheme photocatalysts searching. |
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| AbstractList | Mimicking the natural photosynthesis in plants, Z-scheme water splitting is a promising strategy to improve photocatalytic activity. Searching for the direct Z-scheme photocatalysts is urgent and the crucial factor for the photocatalytic efficiency is the photogenerated electron-hole ( e-h) recombination rate at the interface of two photosystems. In this report, based on time-dependent ab initio nonadiabatic molecular dynamics (NAMD) investigation, we first report a two-dimensional (2D) metal-free van der Waals (vdW) heterostructure consisting of monolayer BCN and C2N as a promising candidate for direct Z-scheme photocatalysts for water splitting. It is shown that the time scale of e-h recombination of BCN/C2N is within 2 ps. Among such e-h recombination events, more than 85% are through the e-h recombination at the interface. NAMD simulations based on frozen phonon method prove that such an ultrafast interlayer e-h recombination is assisted by intralayer optical phonon modes and the interlayer shear phonon mode induced by vdW interaction. In these crucial phonon modes, the interlayer relative movements which are lacking in traditional heterostructures with strong interactions, yet exist generally in various 2D vdW heterostructures, are significant. Our results prove that the 2D vdW heterostructure family is convincing for a new type of direct Z-scheme photocatalysts searching.Mimicking the natural photosynthesis in plants, Z-scheme water splitting is a promising strategy to improve photocatalytic activity. Searching for the direct Z-scheme photocatalysts is urgent and the crucial factor for the photocatalytic efficiency is the photogenerated electron-hole ( e-h) recombination rate at the interface of two photosystems. In this report, based on time-dependent ab initio nonadiabatic molecular dynamics (NAMD) investigation, we first report a two-dimensional (2D) metal-free van der Waals (vdW) heterostructure consisting of monolayer BCN and C2N as a promising candidate for direct Z-scheme photocatalysts for water splitting. It is shown that the time scale of e-h recombination of BCN/C2N is within 2 ps. Among such e-h recombination events, more than 85% are through the e-h recombination at the interface. NAMD simulations based on frozen phonon method prove that such an ultrafast interlayer e-h recombination is assisted by intralayer optical phonon modes and the interlayer shear phonon mode induced by vdW interaction. In these crucial phonon modes, the interlayer relative movements which are lacking in traditional heterostructures with strong interactions, yet exist generally in various 2D vdW heterostructures, are significant. Our results prove that the 2D vdW heterostructure family is convincing for a new type of direct Z-scheme photocatalysts searching. Mimicking the natural photosynthesis in plants, Z-scheme water splitting is a promising strategy to improve photocatalytic activity. Searching for the direct Z-scheme photocatalysts is urgent and the crucial factor for the photocatalytic efficiency is the photogenerated electron-hole ( e-h) recombination rate at the interface of two photosystems. In this report, based on time-dependent ab initio nonadiabatic molecular dynamics (NAMD) investigation, we first report a two-dimensional (2D) metal-free van der Waals (vdW) heterostructure consisting of monolayer BCN and C N as a promising candidate for direct Z-scheme photocatalysts for water splitting. It is shown that the time scale of e-h recombination of BCN/C N is within 2 ps. Among such e-h recombination events, more than 85% are through the e-h recombination at the interface. NAMD simulations based on frozen phonon method prove that such an ultrafast interlayer e-h recombination is assisted by intralayer optical phonon modes and the interlayer shear phonon mode induced by vdW interaction. In these crucial phonon modes, the interlayer relative movements which are lacking in traditional heterostructures with strong interactions, yet exist generally in various 2D vdW heterostructures, are significant. Our results prove that the 2D vdW heterostructure family is convincing for a new type of direct Z-scheme photocatalysts searching. Mimicking the natural photosynthesis in plants, Z-scheme water splitting is a promising strategy to improve photocatalytic activity. Searching for the direct Z-scheme photocatalysts is urgent and the crucial factor for the photocatalytic efficiency is the photogenerated electron–hole (e–h) recombination rate at the interface of two photosystems. In this report, based on time-dependent ab initio nonadiabatic molecular dynamics (NAMD) investigation, we first report a two-dimensional (2D) metal-free van der Waals (vdW) heterostructure consisting of monolayer BCN and C2N as a promising candidate for direct Z-scheme photocatalysts for water splitting. It is shown that the time scale of e–h recombination of BCN/C2N is within 2 ps. Among such e–h recombination events, more than 85% are through the e–h recombination at the interface. NAMD simulations based on frozen phonon method prove that such an ultrafast interlayer e–h recombination is assisted by intralayer optical phonon modes and the interlayer shear phonon mode induced by vdW interaction. In these crucial phonon modes, the interlayer relative movements which are lacking in traditional heterostructures with strong interactions, yet exist generally in various 2D vdW heterostructures, are significant. Our results prove that the 2D vdW heterostructure family is convincing for a new type of direct Z-scheme photocatalysts searching. |
| Author | Zhang, Lili Gao, Pengfei Zhao, Jin Zhang, Ruiqi Zheng, Qijing Yang, Jinlong |
| AuthorAffiliation | University of Science and Technology of China Key Laboratory of Strongly-Coupled Quantum Matter Physics, Chinese Academy of Sciences, and Department of Physics Hefei National Laboratory for Physical Sciences at the Microscale Synergetic Innovation Center of Quantum Information & Quantum Physics |
| AuthorAffiliation_xml | – name: University of Science and Technology of China – name: Key Laboratory of Strongly-Coupled Quantum Matter Physics, Chinese Academy of Sciences, and Department of Physics – name: Synergetic Innovation Center of Quantum Information & Quantum Physics – name: Hefei National Laboratory for Physical Sciences at the Microscale |
| Author_xml | – sequence: 1 givenname: Ruiqi orcidid: 0000-0002-7820-6020 surname: Zhang fullname: Zhang, Ruiqi organization: Hefei National Laboratory for Physical Sciences at the Microscale – sequence: 2 givenname: Lili surname: Zhang fullname: Zhang, Lili organization: Hefei National Laboratory for Physical Sciences at the Microscale – sequence: 3 givenname: Qijing orcidid: 0000-0003-0022-3442 surname: Zheng fullname: Zheng, Qijing organization: Hefei National Laboratory for Physical Sciences at the Microscale – sequence: 4 givenname: Pengfei surname: Gao fullname: Gao, Pengfei organization: Hefei National Laboratory for Physical Sciences at the Microscale – sequence: 5 givenname: Jin orcidid: 0000-0003-1346-5280 surname: Zhao fullname: Zhao, Jin email: zhaojin@ustc.edu.cn organization: University of Science and Technology of China – sequence: 6 givenname: Jinlong orcidid: 0000-0002-5651-5340 surname: Yang fullname: Yang, Jinlong email: jlyang@ustc.edu.cn organization: University of Science and Technology of China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/30180588$$D View this record in MEDLINE/PubMed |
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| Title | Direct Z‑Scheme Water Splitting Photocatalyst Based on Two-Dimensional Van Der Waals Heterostructures |
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