The critical role played by the catalytic moiety in the early-time photodynamics of hydrogen-generating bimetallic photocatalysts

Qing Pan, Francesco Mecozzi, Jeroen P. Korterik, Johannes G. Vos, Wesley R. Browne, Jannetje Maria Huijser

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Abstract

The effect of the catalytic moiety on the early-time photodynamics of Ru/M (M=Pt or Pd) bimetallic photocatalysts is studied by ultrafast transient absorption spectroscopy. In comparison to the Ru/Pd photocatalyst described earlier, the Ru/Pt analogue shows complex excited-state dynamics with three distinct kinetic components ranging from sub-ps to 102 ps, requiring a more sophisticated photophysical model than that developed earlier for the Ru/Pd complex. In the Pu/Pt photocatalyst, an additional lower-lying excited state is proposed to quench the hot higher-lying triplet metal-to-ligand chargetransfer states. Furthermore, a strong excitation wavelength dependence on the population of excited states is observed for both the Ru/Pt and Ru/Pd complexes, indicating a nonequilibrated distribution even on the 102 ps timescale. These insights shed light on the significant impact of the catalytic moiety on the fundamental early-time photophysics of Rubased photocatalysts.
Original languageEnglish
Pages (from-to)2654-2659
Number of pages6
JournalChemPhysChem
Volume17
DOIs
Publication statusPublished - 2016

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Photocatalysts
Hydrogen
Excited states
hydrogen
excitation
Absorption spectroscopy
absorption spectroscopy
Metals
analogs
Ligands
Wavelength
ligands
Kinetics
kinetics
wavelengths
metals

Keywords

  • IR-101573
  • METIS-318133

Cite this

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title = "The critical role played by the catalytic moiety in the early-time photodynamics of hydrogen-generating bimetallic photocatalysts",
abstract = "The effect of the catalytic moiety on the early-time photodynamics of Ru/M (M=Pt or Pd) bimetallic photocatalysts is studied by ultrafast transient absorption spectroscopy. In comparison to the Ru/Pd photocatalyst described earlier, the Ru/Pt analogue shows complex excited-state dynamics with three distinct kinetic components ranging from sub-ps to 102 ps, requiring a more sophisticated photophysical model than that developed earlier for the Ru/Pd complex. In the Pu/Pt photocatalyst, an additional lower-lying excited state is proposed to quench the hot higher-lying triplet metal-to-ligand chargetransfer states. Furthermore, a strong excitation wavelength dependence on the population of excited states is observed for both the Ru/Pt and Ru/Pd complexes, indicating a nonequilibrated distribution even on the 102 ps timescale. These insights shed light on the significant impact of the catalytic moiety on the fundamental early-time photophysics of Rubased photocatalysts.",
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author = "Qing Pan and Francesco Mecozzi and Korterik, {Jeroen P.} and Vos, {Johannes G.} and Browne, {Wesley R.} and Huijser, {Jannetje Maria}",
year = "2016",
doi = "10.1002/cphc.201600458",
language = "English",
volume = "17",
pages = "2654--2659",
journal = "ChemPhysChem",
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publisher = "Wiley-VCH Verlag",

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The critical role played by the catalytic moiety in the early-time photodynamics of hydrogen-generating bimetallic photocatalysts. / Pan, Qing; Mecozzi, Francesco; Korterik, Jeroen P.; Vos, Johannes G.; Browne, Wesley R.; Huijser, Jannetje Maria.

In: ChemPhysChem, Vol. 17, 2016, p. 2654-2659.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - The critical role played by the catalytic moiety in the early-time photodynamics of hydrogen-generating bimetallic photocatalysts

AU - Pan, Qing

AU - Mecozzi, Francesco

AU - Korterik, Jeroen P.

AU - Vos, Johannes G.

AU - Browne, Wesley R.

AU - Huijser, Jannetje Maria

PY - 2016

Y1 - 2016

N2 - The effect of the catalytic moiety on the early-time photodynamics of Ru/M (M=Pt or Pd) bimetallic photocatalysts is studied by ultrafast transient absorption spectroscopy. In comparison to the Ru/Pd photocatalyst described earlier, the Ru/Pt analogue shows complex excited-state dynamics with three distinct kinetic components ranging from sub-ps to 102 ps, requiring a more sophisticated photophysical model than that developed earlier for the Ru/Pd complex. In the Pu/Pt photocatalyst, an additional lower-lying excited state is proposed to quench the hot higher-lying triplet metal-to-ligand chargetransfer states. Furthermore, a strong excitation wavelength dependence on the population of excited states is observed for both the Ru/Pt and Ru/Pd complexes, indicating a nonequilibrated distribution even on the 102 ps timescale. These insights shed light on the significant impact of the catalytic moiety on the fundamental early-time photophysics of Rubased photocatalysts.

AB - The effect of the catalytic moiety on the early-time photodynamics of Ru/M (M=Pt or Pd) bimetallic photocatalysts is studied by ultrafast transient absorption spectroscopy. In comparison to the Ru/Pd photocatalyst described earlier, the Ru/Pt analogue shows complex excited-state dynamics with three distinct kinetic components ranging from sub-ps to 102 ps, requiring a more sophisticated photophysical model than that developed earlier for the Ru/Pd complex. In the Pu/Pt photocatalyst, an additional lower-lying excited state is proposed to quench the hot higher-lying triplet metal-to-ligand chargetransfer states. Furthermore, a strong excitation wavelength dependence on the population of excited states is observed for both the Ru/Pt and Ru/Pd complexes, indicating a nonequilibrated distribution even on the 102 ps timescale. These insights shed light on the significant impact of the catalytic moiety on the fundamental early-time photophysics of Rubased photocatalysts.

KW - IR-101573

KW - METIS-318133

U2 - 10.1002/cphc.201600458

DO - 10.1002/cphc.201600458

M3 - Article

VL - 17

SP - 2654

EP - 2659

JO - ChemPhysChem

JF - ChemPhysChem

SN - 1439-4235

ER -