Facet-dependent carrier dynamics of cuprous oxide regulating the photocatalytic hydrogen generation

Cui Ying Toe; Marlene Lamers; Thomas Dittrich; Hassan A. Tahini; Sean C. Smith; Jason Scott; Rose Amal; Roel Van De Krol; Fatwa F. Abdi; Yun Hau Ng

doi:10.1039/d1ma00934f

Facet-dependent carrier dynamics of cuprous oxide regulating the photocatalytic hydrogen generation

Cui Ying Toe, Marlene Lamers, Thomas Dittrich, Hassan A. Tahini, Sean C. Smith, Jason Scott, Rose Amal, Roel Van De Krol, Fatwa F. Abdi^*, Yun Hau Ng^*

^*Corresponding author for this work

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

20 Citations (Scopus)

Abstract

The intrinsic carrier dynamics of cuprous oxide (Cu2O) are known to have a crucial influence on photocatalytic performances. The photoactivity of rhombic dodecahedral Cu2O with dominant {110} facets (RD-Cu2O) is demonstrated to surpass that of cubic Cu2O with {100} surfaces (CB-Cu2O). Time resolved microwave conductivity (TRMC) measurements reveal the higher carrier mobility of RD-Cu2O when compared to CB-Cu2O. Additionally, modulated surface photovoltage (SPV) measurements further supported the better charge separation efficiency of RD-Cu2O. Although CB-Cu2O exhibited more pronounce SPV signals, the homogeneous distribution of electrical fields drives the majority charge inward and led to detrimental charge recombination. In contrast, the weak SPV signals for RD-Cu2O were attributed to a modulated distribution of charges towards the facets and facet boundaries, demonstrating a better charge separation. This study shows that carrier dynamics and defect density should also be regarded as facet-dependent properties that can have deciding influence on the photocatalytic activity.

Original language	English
Pages (from-to)	2200-2212
Number of pages	13
Journal	Materials Advances
Volume	3
Issue number	4
DOIs	https://doi.org/10.1039/d1ma00934f
Publication status	Published - 21 Feb 2022

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title = "Facet-dependent carrier dynamics of cuprous oxide regulating the photocatalytic hydrogen generation",

abstract = "The intrinsic carrier dynamics of cuprous oxide (Cu2O) are known to have a crucial influence on photocatalytic performances. The photoactivity of rhombic dodecahedral Cu2O with dominant {110} facets (RD-Cu2O) is demonstrated to surpass that of cubic Cu2O with {100} surfaces (CB-Cu2O). Time resolved microwave conductivity (TRMC) measurements reveal the higher carrier mobility of RD-Cu2O when compared to CB-Cu2O. Additionally, modulated surface photovoltage (SPV) measurements further supported the better charge separation efficiency of RD-Cu2O. Although CB-Cu2O exhibited more pronounce SPV signals, the homogeneous distribution of electrical fields drives the majority charge inward and led to detrimental charge recombination. In contrast, the weak SPV signals for RD-Cu2O were attributed to a modulated distribution of charges towards the facets and facet boundaries, demonstrating a better charge separation. This study shows that carrier dynamics and defect density should also be regarded as facet-dependent properties that can have deciding influence on the photocatalytic activity.",

author = "Toe, {Cui Ying} and Marlene Lamers and Thomas Dittrich and Tahini, {Hassan A.} and Smith, {Sean C.} and Jason Scott and Rose Amal and {Van De Krol}, Roel and Abdi, {Fatwa F.} and Ng, {Yun Hau}",

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doi = "10.1039/d1ma00934f",

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T1 - Facet-dependent carrier dynamics of cuprous oxide regulating the photocatalytic hydrogen generation

AU - Toe, Cui Ying

AU - Lamers, Marlene

AU - Dittrich, Thomas

AU - Tahini, Hassan A.

AU - Smith, Sean C.

AU - Scott, Jason

AU - Amal, Rose

AU - Van De Krol, Roel

AU - Abdi, Fatwa F.

AU - Ng, Yun Hau

PY - 2022/2/21

Y1 - 2022/2/21

N2 - The intrinsic carrier dynamics of cuprous oxide (Cu2O) are known to have a crucial influence on photocatalytic performances. The photoactivity of rhombic dodecahedral Cu2O with dominant {110} facets (RD-Cu2O) is demonstrated to surpass that of cubic Cu2O with {100} surfaces (CB-Cu2O). Time resolved microwave conductivity (TRMC) measurements reveal the higher carrier mobility of RD-Cu2O when compared to CB-Cu2O. Additionally, modulated surface photovoltage (SPV) measurements further supported the better charge separation efficiency of RD-Cu2O. Although CB-Cu2O exhibited more pronounce SPV signals, the homogeneous distribution of electrical fields drives the majority charge inward and led to detrimental charge recombination. In contrast, the weak SPV signals for RD-Cu2O were attributed to a modulated distribution of charges towards the facets and facet boundaries, demonstrating a better charge separation. This study shows that carrier dynamics and defect density should also be regarded as facet-dependent properties that can have deciding influence on the photocatalytic activity.

AB - The intrinsic carrier dynamics of cuprous oxide (Cu2O) are known to have a crucial influence on photocatalytic performances. The photoactivity of rhombic dodecahedral Cu2O with dominant {110} facets (RD-Cu2O) is demonstrated to surpass that of cubic Cu2O with {100} surfaces (CB-Cu2O). Time resolved microwave conductivity (TRMC) measurements reveal the higher carrier mobility of RD-Cu2O when compared to CB-Cu2O. Additionally, modulated surface photovoltage (SPV) measurements further supported the better charge separation efficiency of RD-Cu2O. Although CB-Cu2O exhibited more pronounce SPV signals, the homogeneous distribution of electrical fields drives the majority charge inward and led to detrimental charge recombination. In contrast, the weak SPV signals for RD-Cu2O were attributed to a modulated distribution of charges towards the facets and facet boundaries, demonstrating a better charge separation. This study shows that carrier dynamics and defect density should also be regarded as facet-dependent properties that can have deciding influence on the photocatalytic activity.

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DO - 10.1039/d1ma00934f

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SN - 2633-5409

VL - 3

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EP - 2212

JO - Materials Advances

JF - Materials Advances

IS - 4

ER -

Facet-dependent carrier dynamics of cuprous oxide regulating the photocatalytic hydrogen generation

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