Charge Carrier Dynamics of CsPbBr3/g-C3N4Nanoheterostructures in Visible-Light-Driven CO2-to-CO Conversion

Yu Hung Chen; Kai An Tsai; Tzu Wei Liu; Yao Jen Chang; Yu Chen Wei; Meng Wei Zheng; Shou Heng Liu; Mei Yi Liao; Pei Yu Sie; Jarrn Horng Lin; Shih Wen Tseng; Ying Chih Pu

doi:10.1021/acs.jpclett.2c03474

Charge Carrier Dynamics of CsPbBr₃/g-C₃N₄Nanoheterostructures in Visible-Light-Driven CO₂-to-CO Conversion

Yu Hung Chen, Kai An Tsai, Tzu Wei Liu, Yao Jen Chang, Yu Chen Wei, Meng Wei Zheng, Shou Heng Liu, Mei Yi Liao, Pei Yu Sie, Jarrn Horng Lin, Shih Wen Tseng, Ying Chih Pu

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

Abstract

The photon energy-dependent selectivity of photocatalytic CO₂-to-CO conversion by CsPbBr₃nanocrystals (NCs) and CsPbBr₃/g-C₃N₄nanoheterostructures (NHSs) was demonstrated for the first time. The surficial capping ligands of CsPbBr₃NCs would adsorb CO₂, resulting in the carboxyl intermediate to process the CO₂-to-CO conversion via carbene pathways. The type-II energy band structure at the heterojunction of CsPbBr₃/g-C₃N₄NHSs would separate the charge carriers, promoting the efficiency in photocatalytic CO₂-to-CO conversion. The electron consumption rate of CO₂-to-CO conversion for CsPbBr₃/g-C₃N₄NHSs was found to intensively depend on the rate constant of interfacial hole transfer from CsPbBr₃to g-C₃N₄. An in situ transient absorption spectroscopy investigation revealed that the half-life time of photoexcited electrons in optimized CsPbBr₃/g-C₃N₄NHS was extended two times more than that in the CsPbBr₃NCs, resulting in the higher probability of charge carriers to carry out the CO₂-to-CO conversion. The current work presents important and novel insights of semiconductor NHSs for solar energy-driven CO₂conversion.

Original language	English
Pages (from-to)	122-131
Number of pages	10
Journal	Journal of Physical Chemistry Letters
Volume	14
Issue number	1
DOIs	https://doi.org/10.1021/acs.jpclett.2c03474
Publication status	Published - 2023 Jan 12

All Science Journal Classification (ASJC) codes

Materials Science(all)
Physical and Theoretical Chemistry

Access to Document

10.1021/acs.jpclett.2c03474

Cite this

@article{a8451e997d31473e976f2fe13c15fda7,

title = "Charge Carrier Dynamics of CsPbBr3/g-C3N4Nanoheterostructures in Visible-Light-Driven CO2-to-CO Conversion",

abstract = "The photon energy-dependent selectivity of photocatalytic CO2-to-CO conversion by CsPbBr3nanocrystals (NCs) and CsPbBr3/g-C3N4nanoheterostructures (NHSs) was demonstrated for the first time. The surficial capping ligands of CsPbBr3NCs would adsorb CO2, resulting in the carboxyl intermediate to process the CO2-to-CO conversion via carbene pathways. The type-II energy band structure at the heterojunction of CsPbBr3/g-C3N4NHSs would separate the charge carriers, promoting the efficiency in photocatalytic CO2-to-CO conversion. The electron consumption rate of CO2-to-CO conversion for CsPbBr3/g-C3N4NHSs was found to intensively depend on the rate constant of interfacial hole transfer from CsPbBr3to g-C3N4. An in situ transient absorption spectroscopy investigation revealed that the half-life time of photoexcited electrons in optimized CsPbBr3/g-C3N4NHS was extended two times more than that in the CsPbBr3NCs, resulting in the higher probability of charge carriers to carry out the CO2-to-CO conversion. The current work presents important and novel insights of semiconductor NHSs for solar energy-driven CO2conversion.",

author = "Chen, {Yu Hung} and Tsai, {Kai An} and Liu, {Tzu Wei} and Chang, {Yao Jen} and Wei, {Yu Chen} and Zheng, {Meng Wei} and Liu, {Shou Heng} and Liao, {Mei Yi} and Sie, {Pei Yu} and Lin, {Jarrn Horng} and Tseng, {Shih Wen} and Pu, {Ying Chih}",

note = "Funding Information: We acknowledge the financial support from National Science and Technology Council (NSTC) of Taiwan under Grant Nos. 111-2113-M-024-002 and 111-2811-M-024-001. We gratefully acknowledge the support of soft matter–TEM and JEOL JEM-2100F Cs STEM equipment, belonging to the Instrument Center of National Cheng Kung University, and Thermo Fisher Scientific ESCALAB Xi + electron spectroscopy equipment from the Center for Advanced Instrumentation at National Yang Ming Chiao Tung University. Publisher Copyright: {\textcopyright} 2023 American Chemical Society. All rights reserved.",

year = "2023",

month = jan,

day = "12",

doi = "10.1021/acs.jpclett.2c03474",

language = "English",

volume = "14",

pages = "122--131",

journal = "Journal of Physical Chemistry Letters",

issn = "1948-7185",

publisher = "American Chemical Society",

number = "1",

}

TY - JOUR

T1 - Charge Carrier Dynamics of CsPbBr3/g-C3N4Nanoheterostructures in Visible-Light-Driven CO2-to-CO Conversion

AU - Chen, Yu Hung

AU - Tsai, Kai An

AU - Liu, Tzu Wei

AU - Chang, Yao Jen

AU - Wei, Yu Chen

AU - Zheng, Meng Wei

AU - Liu, Shou Heng

AU - Liao, Mei Yi

AU - Sie, Pei Yu

AU - Lin, Jarrn Horng

AU - Tseng, Shih Wen

AU - Pu, Ying Chih

N1 - Funding Information: We acknowledge the financial support from National Science and Technology Council (NSTC) of Taiwan under Grant Nos. 111-2113-M-024-002 and 111-2811-M-024-001. We gratefully acknowledge the support of soft matter–TEM and JEOL JEM-2100F Cs STEM equipment, belonging to the Instrument Center of National Cheng Kung University, and Thermo Fisher Scientific ESCALAB Xi + electron spectroscopy equipment from the Center for Advanced Instrumentation at National Yang Ming Chiao Tung University. Publisher Copyright: © 2023 American Chemical Society. All rights reserved.

PY - 2023/1/12

Y1 - 2023/1/12

N2 - The photon energy-dependent selectivity of photocatalytic CO2-to-CO conversion by CsPbBr3nanocrystals (NCs) and CsPbBr3/g-C3N4nanoheterostructures (NHSs) was demonstrated for the first time. The surficial capping ligands of CsPbBr3NCs would adsorb CO2, resulting in the carboxyl intermediate to process the CO2-to-CO conversion via carbene pathways. The type-II energy band structure at the heterojunction of CsPbBr3/g-C3N4NHSs would separate the charge carriers, promoting the efficiency in photocatalytic CO2-to-CO conversion. The electron consumption rate of CO2-to-CO conversion for CsPbBr3/g-C3N4NHSs was found to intensively depend on the rate constant of interfacial hole transfer from CsPbBr3to g-C3N4. An in situ transient absorption spectroscopy investigation revealed that the half-life time of photoexcited electrons in optimized CsPbBr3/g-C3N4NHS was extended two times more than that in the CsPbBr3NCs, resulting in the higher probability of charge carriers to carry out the CO2-to-CO conversion. The current work presents important and novel insights of semiconductor NHSs for solar energy-driven CO2conversion.

AB - The photon energy-dependent selectivity of photocatalytic CO2-to-CO conversion by CsPbBr3nanocrystals (NCs) and CsPbBr3/g-C3N4nanoheterostructures (NHSs) was demonstrated for the first time. The surficial capping ligands of CsPbBr3NCs would adsorb CO2, resulting in the carboxyl intermediate to process the CO2-to-CO conversion via carbene pathways. The type-II energy band structure at the heterojunction of CsPbBr3/g-C3N4NHSs would separate the charge carriers, promoting the efficiency in photocatalytic CO2-to-CO conversion. The electron consumption rate of CO2-to-CO conversion for CsPbBr3/g-C3N4NHSs was found to intensively depend on the rate constant of interfacial hole transfer from CsPbBr3to g-C3N4. An in situ transient absorption spectroscopy investigation revealed that the half-life time of photoexcited electrons in optimized CsPbBr3/g-C3N4NHS was extended two times more than that in the CsPbBr3NCs, resulting in the higher probability of charge carriers to carry out the CO2-to-CO conversion. The current work presents important and novel insights of semiconductor NHSs for solar energy-driven CO2conversion.

UR - http://www.scopus.com/inward/record.url?scp=85145303638&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85145303638&partnerID=8YFLogxK

U2 - 10.1021/acs.jpclett.2c03474

DO - 10.1021/acs.jpclett.2c03474

M3 - Article

C2 - 36574643

AN - SCOPUS:85145303638

SN - 1948-7185

VL - 14

SP - 122

EP - 131

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

IS - 1

ER -

Charge Carrier Dynamics of CsPbBr₃/g-C₃N₄Nanoheterostructures in Visible-Light-Driven CO₂-to-CO Conversion

Abstract

All Science Journal Classification (ASJC) codes

Access to Document

Other files and links

Fingerprint

Cite this