2D Honeycomb-Kagome Polymer Tandem as Effective Metal-Free Photocatalysts for Water Splitting

Yu Jing; Zhenpei Zhou; Weixiang Geng; Xinyue Zhu; Thomas Heine

doi:10.1002/adma.202008645

2D Honeycomb-Kagome Polymer Tandem as Effective Metal-Free Photocatalysts for Water Splitting

Yu Jing, Zhenpei Zhou, Weixiang Geng, Xinyue Zhu, Thomas Heine

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

30 Citations (Scopus)

Abstract

On the basis of first-principles calculations, the potential of applying 2D honeycomb-kagome polymers made of heteroatom-centered triangulene derivatives to photocatalyze water splitting is explored. The designed 2D polymers possess indirect bandgaps in the range of 1.80–2.84 eV and show pronounced light absorption in the ultraviolet and visible region of the solar spectrum. With suitable band edge alignment, the examined N- and B-center polymers can generate sufficient photon-excited electrons and holes to activate the hydrogen and oxygen evolution reactions, respectively. The combination of lattice-inherent band features (flat bands) with chemical functionalization (potential shift due to heteroatoms) makes it possible to construct tandem cells with suppressed electron/hole recombination for effective overall water splitting. In addition, there is a potential difference between the half-electrodes that can be utlized to power auxiliary components in self-sufficient photocatalyzers.

Original language	English
Article number	2008645
Journal	Advanced Materials
Volume	33
Issue number	21
DOIs	https://doi.org/10.1002/adma.202008645
Publication status	Published - 2021 May 27

Bibliographical note

Funding Information:
The work obtained support in China by National Natural Science Foundation of China (No. 21903046) and Natural Science Foundation of Jiangsu Province (No. BK20190744). The computational resources utilized in this research were provided by Shanghai Supercomputer Center.

Funding Information:
The work obtained support in China by National Natural Science Foundation of China (No. 21903046) and Natural Science Foundation of Jiangsu Province (No. BK20190744). The computational resources utilized in this research were provided by Shanghai Supercomputer Center. Open access funding enabled and organized by Projekt DEAL.

Publisher Copyright:
© 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH

All Science Journal Classification (ASJC) codes

Materials Science(all)
Mechanics of Materials
Mechanical Engineering

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10.1002/adma.202008645

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title = "2D Honeycomb-Kagome Polymer Tandem as Effective Metal-Free Photocatalysts for Water Splitting",

abstract = "On the basis of first-principles calculations, the potential of applying 2D honeycomb-kagome polymers made of heteroatom-centered triangulene derivatives to photocatalyze water splitting is explored. The designed 2D polymers possess indirect bandgaps in the range of 1.80–2.84 eV and show pronounced light absorption in the ultraviolet and visible region of the solar spectrum. With suitable band edge alignment, the examined N- and B-center polymers can generate sufficient photon-excited electrons and holes to activate the hydrogen and oxygen evolution reactions, respectively. The combination of lattice-inherent band features (flat bands) with chemical functionalization (potential shift due to heteroatoms) makes it possible to construct tandem cells with suppressed electron/hole recombination for effective overall water splitting. In addition, there is a potential difference between the half-electrodes that can be utlized to power auxiliary components in self-sufficient photocatalyzers.",

author = "Yu Jing and Zhenpei Zhou and Weixiang Geng and Xinyue Zhu and Thomas Heine",

note = "Funding Information: The work obtained support in China by National Natural Science Foundation of China (No. 21903046) and Natural Science Foundation of Jiangsu Province (No. BK20190744). The computational resources utilized in this research were provided by Shanghai Supercomputer Center. Funding Information: The work obtained support in China by National Natural Science Foundation of China (No. 21903046) and Natural Science Foundation of Jiangsu Province (No. BK20190744). The computational resources utilized in this research were provided by Shanghai Supercomputer Center. Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: {\textcopyright} 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH",

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AU - Heine, Thomas

N1 - Funding Information: The work obtained support in China by National Natural Science Foundation of China (No. 21903046) and Natural Science Foundation of Jiangsu Province (No. BK20190744). The computational resources utilized in this research were provided by Shanghai Supercomputer Center. Funding Information: The work obtained support in China by National Natural Science Foundation of China (No. 21903046) and Natural Science Foundation of Jiangsu Province (No. BK20190744). The computational resources utilized in this research were provided by Shanghai Supercomputer Center. Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: © 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH

PY - 2021/5/27

Y1 - 2021/5/27

N2 - On the basis of first-principles calculations, the potential of applying 2D honeycomb-kagome polymers made of heteroatom-centered triangulene derivatives to photocatalyze water splitting is explored. The designed 2D polymers possess indirect bandgaps in the range of 1.80–2.84 eV and show pronounced light absorption in the ultraviolet and visible region of the solar spectrum. With suitable band edge alignment, the examined N- and B-center polymers can generate sufficient photon-excited electrons and holes to activate the hydrogen and oxygen evolution reactions, respectively. The combination of lattice-inherent band features (flat bands) with chemical functionalization (potential shift due to heteroatoms) makes it possible to construct tandem cells with suppressed electron/hole recombination for effective overall water splitting. In addition, there is a potential difference between the half-electrodes that can be utlized to power auxiliary components in self-sufficient photocatalyzers.

AB - On the basis of first-principles calculations, the potential of applying 2D honeycomb-kagome polymers made of heteroatom-centered triangulene derivatives to photocatalyze water splitting is explored. The designed 2D polymers possess indirect bandgaps in the range of 1.80–2.84 eV and show pronounced light absorption in the ultraviolet and visible region of the solar spectrum. With suitable band edge alignment, the examined N- and B-center polymers can generate sufficient photon-excited electrons and holes to activate the hydrogen and oxygen evolution reactions, respectively. The combination of lattice-inherent band features (flat bands) with chemical functionalization (potential shift due to heteroatoms) makes it possible to construct tandem cells with suppressed electron/hole recombination for effective overall water splitting. In addition, there is a potential difference between the half-electrodes that can be utlized to power auxiliary components in self-sufficient photocatalyzers.

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2D Honeycomb-Kagome Polymer Tandem as Effective Metal-Free Photocatalysts for Water Splitting

Abstract

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