Boosting Photocatalytic Hydrogen Production by Modulating Recombination Modes and Proton Adsorption Energy

Yitao Dai; Qijing Bu; Rishmali Sooriyagoda; Pedram Tavadze; Olivia Pavlic; Tingbin Lim; Yanbin Shen; Aref Mamakhel; Xiaoping Wang; Yongwang Li; Hans Niemantsverdriet; Bo B. Iversen; Flemming Besenbacher; Tengfeng Xie; James P. Lewis; Alan D. Bristow; Nina Lock; Ren Su

doi:10.1021/acs.jpclett.9b01460

Boosting Photocatalytic Hydrogen Production by Modulating Recombination Modes and Proton Adsorption Energy

Yitao Dai, Qijing Bu, Rishmali Sooriyagoda, Pedram Tavadze, Olivia Pavlic, Tingbin Lim, Yanbin Shen, Aref Mamakhel, Xiaoping Wang, Yongwang Li, Hans Niemantsverdriet, Bo B. Iversen, Flemming Besenbacher, Tengfeng Xie, James P. Lewis, Alan D. Bristow, Nina Lock, Ren Su^*

^*Corresponding author for this work

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

19 Citations (Scopus)

Abstract

Solar-driven production of renewable energy (e.g., H₂) has been investigated for decades. To date, the applications are limited by low efficiency due to rapid charge recombination (both radiative and nonradiative modes) and slow reaction rates. Tremendous efforts have been focused on reducing the radiative recombination and enhancing the interfacial charge transfer by engineering the geometric and electronic structure of the photocatalysts. However, fine-tuning of nonradiative recombination processes and optimization of target reaction paths still lack effective control. Here we show that minimizing the nonradiative relaxation and the adsorption energy of photogenerated surface-adsorbed hydrogen atoms are essential to achieve a longer lifetime of the charge carriers and a faster reaction rate, respectively. Such control results in a 16-fold enhancement in photocatalytic H₂ evolution and a 15-fold increase in photocurrent of the crystalline g-C₃N₄ compared to that of the amorphous g-C₃N₄.

Original language	English
Journal	Journal of Physical Chemistry Letters
Volume	10
Issue	18
Pages (from-to)	5381-5386
Number of pages	11
ISSN	1948-7185
DOIs	https://doi.org/10.1021/acs.jpclett.9b01460
Publication status	Published - Sept 2019

Keywords

CARBON NITRIDE PHOTOCATALYST
CDS
CHARGE SEPARATION
COCATALYSTS
CRYSTALLINE G-C3N4
EFFICIENCY
ELECTRON INJECTION
GENERATION
NANOPARTICLES
QUANTUM DOTS

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Dai, Y., Bu, Q., Sooriyagoda, R., Tavadze, P., Pavlic, O., Lim, T., Shen, Y., Mamakhel, A., Wang, X., Li, Y., Niemantsverdriet, H., Iversen, B. B., Besenbacher, F., Xie, T., Lewis, J. P., Bristow, A. D., Lock, N., & Su, R. (2019). Boosting Photocatalytic Hydrogen Production by Modulating Recombination Modes and Proton Adsorption Energy. Journal of Physical Chemistry Letters, 10(18), 5381-5386. https://doi.org/10.1021/acs.jpclett.9b01460

@article{3a8bb9faa82d42df9fed973e65528201,

title = "Boosting Photocatalytic Hydrogen Production by Modulating Recombination Modes and Proton Adsorption Energy",

abstract = "Solar-driven production of renewable energy (e.g., H2) has been investigated for decades. To date, the applications are limited by low efficiency due to rapid charge recombination (both radiative and nonradiative modes) and slow reaction rates. Tremendous efforts have been focused on reducing the radiative recombination and enhancing the interfacial charge transfer by engineering the geometric and electronic structure of the photocatalysts. However, fine-tuning of nonradiative recombination processes and optimization of target reaction paths still lack effective control. Here we show that minimizing the nonradiative relaxation and the adsorption energy of photogenerated surface-adsorbed hydrogen atoms are essential to achieve a longer lifetime of the charge carriers and a faster reaction rate, respectively. Such control results in a 16-fold enhancement in photocatalytic H2 evolution and a 15-fold increase in photocurrent of the crystalline g-C3N4 compared to that of the amorphous g-C3N4.",

keywords = "CARBON NITRIDE PHOTOCATALYST, CDS, CHARGE SEPARATION, COCATALYSTS, CRYSTALLINE G-C3N4, EFFICIENCY, ELECTRON INJECTION, GENERATION, NANOPARTICLES, QUANTUM DOTS",

author = "Yitao Dai and Qijing Bu and Rishmali Sooriyagoda and Pedram Tavadze and Olivia Pavlic and Tingbin Lim and Yanbin Shen and Aref Mamakhel and Xiaoping Wang and Yongwang Li and Hans Niemantsverdriet and Iversen, {Bo B.} and Flemming Besenbacher and Tengfeng Xie and Lewis, {James P.} and Bristow, {Alan D.} and Nina Lock and Ren Su",

year = "2019",

month = sep,

doi = "10.1021/acs.jpclett.9b01460",

language = "English",

volume = "10",

pages = "5381--5386",

journal = "Journal of Physical Chemistry Letters",

issn = "1948-7185",

publisher = "American Chemical Society",

number = "18",

}

Dai, Y, Bu, Q, Sooriyagoda, R, Tavadze, P, Pavlic, O, Lim, T, Shen, Y, Mamakhel, A, Wang, X, Li, Y, Niemantsverdriet, H, Iversen, BB, Besenbacher, F, Xie, T, Lewis, JP, Bristow, AD, Lock, N & Su, R 2019, 'Boosting Photocatalytic Hydrogen Production by Modulating Recombination Modes and Proton Adsorption Energy', Journal of Physical Chemistry Letters, vol. 10, no. 18, pp. 5381-5386. https://doi.org/10.1021/acs.jpclett.9b01460

Boosting Photocatalytic Hydrogen Production by Modulating Recombination Modes and Proton Adsorption Energy. / Dai, Yitao; Bu, Qijing; Sooriyagoda, Rishmali et al.
In: Journal of Physical Chemistry Letters, Vol. 10, No. 18, 09.2019, p. 5381-5386.

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

TY - JOUR

T1 - Boosting Photocatalytic Hydrogen Production by Modulating Recombination Modes and Proton Adsorption Energy

AU - Dai, Yitao

AU - Bu, Qijing

AU - Sooriyagoda, Rishmali

AU - Tavadze, Pedram

AU - Pavlic, Olivia

AU - Lim, Tingbin

AU - Shen, Yanbin

AU - Mamakhel, Aref

AU - Wang, Xiaoping

AU - Li, Yongwang

AU - Niemantsverdriet, Hans

AU - Iversen, Bo B.

AU - Besenbacher, Flemming

AU - Xie, Tengfeng

AU - Lewis, James P.

AU - Bristow, Alan D.

AU - Lock, Nina

AU - Su, Ren

PY - 2019/9

Y1 - 2019/9

N2 - Solar-driven production of renewable energy (e.g., H2) has been investigated for decades. To date, the applications are limited by low efficiency due to rapid charge recombination (both radiative and nonradiative modes) and slow reaction rates. Tremendous efforts have been focused on reducing the radiative recombination and enhancing the interfacial charge transfer by engineering the geometric and electronic structure of the photocatalysts. However, fine-tuning of nonradiative recombination processes and optimization of target reaction paths still lack effective control. Here we show that minimizing the nonradiative relaxation and the adsorption energy of photogenerated surface-adsorbed hydrogen atoms are essential to achieve a longer lifetime of the charge carriers and a faster reaction rate, respectively. Such control results in a 16-fold enhancement in photocatalytic H2 evolution and a 15-fold increase in photocurrent of the crystalline g-C3N4 compared to that of the amorphous g-C3N4.

AB - Solar-driven production of renewable energy (e.g., H2) has been investigated for decades. To date, the applications are limited by low efficiency due to rapid charge recombination (both radiative and nonradiative modes) and slow reaction rates. Tremendous efforts have been focused on reducing the radiative recombination and enhancing the interfacial charge transfer by engineering the geometric and electronic structure of the photocatalysts. However, fine-tuning of nonradiative recombination processes and optimization of target reaction paths still lack effective control. Here we show that minimizing the nonradiative relaxation and the adsorption energy of photogenerated surface-adsorbed hydrogen atoms are essential to achieve a longer lifetime of the charge carriers and a faster reaction rate, respectively. Such control results in a 16-fold enhancement in photocatalytic H2 evolution and a 15-fold increase in photocurrent of the crystalline g-C3N4 compared to that of the amorphous g-C3N4.

KW - CARBON NITRIDE PHOTOCATALYST

KW - CDS

KW - CHARGE SEPARATION

KW - COCATALYSTS

KW - CRYSTALLINE G-C3N4

KW - EFFICIENCY

KW - ELECTRON INJECTION

KW - GENERATION

KW - NANOPARTICLES

KW - QUANTUM DOTS

UR - http://www.scopus.com/inward/record.url?scp=85072508565&partnerID=8YFLogxK

U2 - 10.1021/acs.jpclett.9b01460

DO - 10.1021/acs.jpclett.9b01460

M3 - Journal article

C2 - 31448921

AN - SCOPUS:85072508565

SN - 1948-7185

VL - 10

SP - 5381

EP - 5386

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

IS - 18

ER -

Boosting Photocatalytic Hydrogen Production by Modulating Recombination Modes and Proton Adsorption Energy

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