A Heterostructure Photoelectrode Based on Two-Dimensional Covalent Organic Framework Film Decorated TiO<sub>2</sub> Nanotube Arrays for Enhanced Photoelectrochemical Hydrogen Generation
The well-defined heterostructure of the photocathode is desirable for photoelectrochemically producing hydrogen from aqueous solutions. Herein, enhanced heterostructures were fabricated based on typical stable covalent organic framework (TpPa-1) films and TiO<sub>2</sub> nanotube arrays...
| Main Authors: | , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
MDPI AG
2023-01-01
|
| Series: | Molecules |
| Subjects: | |
| Online Access: | https://www.mdpi.com/1420-3049/28/2/822 |
| _version_ | 1797438268289056768 |
|---|---|
| author | Yue Zhang Yujie Li Jing Yu Bing Sun Hong Shang |
| author_facet | Yue Zhang Yujie Li Jing Yu Bing Sun Hong Shang |
| author_sort | Yue Zhang |
| collection | DOAJ |
| description | The well-defined heterostructure of the photocathode is desirable for photoelectrochemically producing hydrogen from aqueous solutions. Herein, enhanced heterostructures were fabricated based on typical stable covalent organic framework (TpPa-1) films and TiO<sub>2</sub> nanotube arrays (NTAs) as a proof-of-concept model to tune the photoelectrochemical (PEC) hydrogen generation by tailoring the photoelectrode microstructure and interfacial charge transport. Ultrathin TpPa-1 films were uniformly grown on the surface of TiO<sub>2</sub> NTAs via a solvothermal condensation of building blocks by tuning the monomer concentration. The Pt<sub>1</sub>@TpPa-1/TiO<sub>2</sub>-NTAs photoelectrode with single-atom Pt<sub>1</sub> as a co-catalyst demonstrated improved visible-light response, enhanced photoconductance, lower onset potential, and decreased Tafel slope value for hydrogen evolution. The hydrogen evolution rate of the Pt<sub>1</sub>@TpPa-1/TiO<sub>2</sub>-NTAs photoelectrode was five times that of Pt<sub>1</sub>@TpPa-1 under AM 1.5 simulated sunlight irradiation and the bias voltage of 0 V. A lower overpotential was recorded as 77 mV@10 mA cm<sup>−2</sup> and a higher photocurrent density as 1.63 mA cm<sup>−2</sup>. The hydrogen evolution performance of Pt<sub>1</sub>@TpPa-1/TiO<sub>2</sub>-NTAs photoelectrodes may benefit from the well-matched band structures, effective charge separation, lower interfacial resistance, abundant interfacial microstructural sites, and surficial hydrophilicity. This work may raise a promising way to design an efficient PEC system for hydrogen evolution by tuning well-defined heterojunctions and interfacial microstructures. |
| first_indexed | 2024-03-09T11:35:14Z |
| format | Article |
| id | doaj.art-ada543e38b984b8f9c466bddf8805329 |
| institution | Directory Open Access Journal |
| issn | 1420-3049 |
| language | English |
| last_indexed | 2024-03-09T11:35:14Z |
| publishDate | 2023-01-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Molecules |
| spelling | doaj.art-ada543e38b984b8f9c466bddf88053292023-11-30T23:45:25ZengMDPI AGMolecules1420-30492023-01-0128282210.3390/molecules28020822A Heterostructure Photoelectrode Based on Two-Dimensional Covalent Organic Framework Film Decorated TiO<sub>2</sub> Nanotube Arrays for Enhanced Photoelectrochemical Hydrogen GenerationYue Zhang0Yujie Li1Jing Yu2Bing Sun3Hong Shang4School of Science, China University of Geosciences (Beijing), Beijing 100083, ChinaSchool of Science, China University of Geosciences (Beijing), Beijing 100083, ChinaSchool of Science, China University of Geosciences (Beijing), Beijing 100083, ChinaSchool of Science, China University of Geosciences (Beijing), Beijing 100083, ChinaSchool of Science, China University of Geosciences (Beijing), Beijing 100083, ChinaThe well-defined heterostructure of the photocathode is desirable for photoelectrochemically producing hydrogen from aqueous solutions. Herein, enhanced heterostructures were fabricated based on typical stable covalent organic framework (TpPa-1) films and TiO<sub>2</sub> nanotube arrays (NTAs) as a proof-of-concept model to tune the photoelectrochemical (PEC) hydrogen generation by tailoring the photoelectrode microstructure and interfacial charge transport. Ultrathin TpPa-1 films were uniformly grown on the surface of TiO<sub>2</sub> NTAs via a solvothermal condensation of building blocks by tuning the monomer concentration. The Pt<sub>1</sub>@TpPa-1/TiO<sub>2</sub>-NTAs photoelectrode with single-atom Pt<sub>1</sub> as a co-catalyst demonstrated improved visible-light response, enhanced photoconductance, lower onset potential, and decreased Tafel slope value for hydrogen evolution. The hydrogen evolution rate of the Pt<sub>1</sub>@TpPa-1/TiO<sub>2</sub>-NTAs photoelectrode was five times that of Pt<sub>1</sub>@TpPa-1 under AM 1.5 simulated sunlight irradiation and the bias voltage of 0 V. A lower overpotential was recorded as 77 mV@10 mA cm<sup>−2</sup> and a higher photocurrent density as 1.63 mA cm<sup>−2</sup>. The hydrogen evolution performance of Pt<sub>1</sub>@TpPa-1/TiO<sub>2</sub>-NTAs photoelectrodes may benefit from the well-matched band structures, effective charge separation, lower interfacial resistance, abundant interfacial microstructural sites, and surficial hydrophilicity. This work may raise a promising way to design an efficient PEC system for hydrogen evolution by tuning well-defined heterojunctions and interfacial microstructures.https://www.mdpi.com/1420-3049/28/2/822two-dimensional materialscovalent organic frameworksurface modificationheterostructurephotocatalytic hydrogen generation |
| spellingShingle | Yue Zhang Yujie Li Jing Yu Bing Sun Hong Shang A Heterostructure Photoelectrode Based on Two-Dimensional Covalent Organic Framework Film Decorated TiO<sub>2</sub> Nanotube Arrays for Enhanced Photoelectrochemical Hydrogen Generation Molecules two-dimensional materials covalent organic framework surface modification heterostructure photocatalytic hydrogen generation |
| title | A Heterostructure Photoelectrode Based on Two-Dimensional Covalent Organic Framework Film Decorated TiO<sub>2</sub> Nanotube Arrays for Enhanced Photoelectrochemical Hydrogen Generation |
| title_full | A Heterostructure Photoelectrode Based on Two-Dimensional Covalent Organic Framework Film Decorated TiO<sub>2</sub> Nanotube Arrays for Enhanced Photoelectrochemical Hydrogen Generation |
| title_fullStr | A Heterostructure Photoelectrode Based on Two-Dimensional Covalent Organic Framework Film Decorated TiO<sub>2</sub> Nanotube Arrays for Enhanced Photoelectrochemical Hydrogen Generation |
| title_full_unstemmed | A Heterostructure Photoelectrode Based on Two-Dimensional Covalent Organic Framework Film Decorated TiO<sub>2</sub> Nanotube Arrays for Enhanced Photoelectrochemical Hydrogen Generation |
| title_short | A Heterostructure Photoelectrode Based on Two-Dimensional Covalent Organic Framework Film Decorated TiO<sub>2</sub> Nanotube Arrays for Enhanced Photoelectrochemical Hydrogen Generation |
| title_sort | heterostructure photoelectrode based on two dimensional covalent organic framework film decorated tio sub 2 sub nanotube arrays for enhanced photoelectrochemical hydrogen generation |
| topic | two-dimensional materials covalent organic framework surface modification heterostructure photocatalytic hydrogen generation |
| url | https://www.mdpi.com/1420-3049/28/2/822 |
| work_keys_str_mv | AT yuezhang aheterostructurephotoelectrodebasedontwodimensionalcovalentorganicframeworkfilmdecoratedtiosub2subnanotubearraysforenhancedphotoelectrochemicalhydrogengeneration AT yujieli aheterostructurephotoelectrodebasedontwodimensionalcovalentorganicframeworkfilmdecoratedtiosub2subnanotubearraysforenhancedphotoelectrochemicalhydrogengeneration AT jingyu aheterostructurephotoelectrodebasedontwodimensionalcovalentorganicframeworkfilmdecoratedtiosub2subnanotubearraysforenhancedphotoelectrochemicalhydrogengeneration AT bingsun aheterostructurephotoelectrodebasedontwodimensionalcovalentorganicframeworkfilmdecoratedtiosub2subnanotubearraysforenhancedphotoelectrochemicalhydrogengeneration AT hongshang aheterostructurephotoelectrodebasedontwodimensionalcovalentorganicframeworkfilmdecoratedtiosub2subnanotubearraysforenhancedphotoelectrochemicalhydrogengeneration AT yuezhang heterostructurephotoelectrodebasedontwodimensionalcovalentorganicframeworkfilmdecoratedtiosub2subnanotubearraysforenhancedphotoelectrochemicalhydrogengeneration AT yujieli heterostructurephotoelectrodebasedontwodimensionalcovalentorganicframeworkfilmdecoratedtiosub2subnanotubearraysforenhancedphotoelectrochemicalhydrogengeneration AT jingyu heterostructurephotoelectrodebasedontwodimensionalcovalentorganicframeworkfilmdecoratedtiosub2subnanotubearraysforenhancedphotoelectrochemicalhydrogengeneration AT bingsun heterostructurephotoelectrodebasedontwodimensionalcovalentorganicframeworkfilmdecoratedtiosub2subnanotubearraysforenhancedphotoelectrochemicalhydrogengeneration AT hongshang heterostructurephotoelectrodebasedontwodimensionalcovalentorganicframeworkfilmdecoratedtiosub2subnanotubearraysforenhancedphotoelectrochemicalhydrogengeneration |