2017
DOI: 10.1021/acsenergylett.7b00730
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Competitive Hole Transfer from CdSe Quantum Dots to Thiol Ligands in CdSe-Cobaloxime Sensitized NiO Films Used as Photocathodes for H2 Evolution

Abstract: Quantum dot (QD) sensitized NiO photocathodes rely on efficient photoinduced hole injection into the NiO valence band. A system of a mesoporous NiO film co-sensitized with CdSe QDs and a molecular protonreduction catalyst was studied. While successful electron transfer from the excited QDs to the catalyst is observed, most of the photogenerated holes are instead quenched very rapidly (ps) by hole trapping at the surface thiols of the capping agent used as linker molecules. We confirmed our conclusion by first … Show more

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Cited by 36 publications
(35 citation statements)
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“…[229] Most of the holes were trapped by thiol groups and/or sulfide ions from the capping agent (thioglycolic acid) of CdSe QDs as indicated from the femtosecond TA investigation. [230] Therefore, further treatment of QDs, including using thiol-free capping agents or employing core/shell QDs with short ligands, should be taken into consideration.…”
Section: Electron Transfer Engineeringmentioning
confidence: 99%
“…[229] Most of the holes were trapped by thiol groups and/or sulfide ions from the capping agent (thioglycolic acid) of CdSe QDs as indicated from the femtosecond TA investigation. [230] Therefore, further treatment of QDs, including using thiol-free capping agents or employing core/shell QDs with short ligands, should be taken into consideration.…”
Section: Electron Transfer Engineeringmentioning
confidence: 99%
“…We next considered the possibility that the thiol group could be oxidized under photocatalytic conditions, which would effectively render it an electron donor, as previously reported. 41,42 However, 1 H-NMR spectroscopy of a ZnSe | MEMI solution after 1 h of solar irradiation did not show any signals from a potential disulfide product (Figure S13).…”
Section: Photocatalytic Co2 Reductionmentioning
confidence: 99%
“…The probe and reference pulses were scattered in a spectrograph and a diode array is used to detect these pulses. The instrumental response time is approximately 100 fs, the polarization of the pump was adjusted at a magic angle of 54.7 • with respect to the probe beam [25][26][27][28]. Low temperature-specific heat and the magnetic properties of the investigated sample were measured by using the Quantum Design Physical Properties Measurement System (PPMS).…”
Section: Characterizationmentioning
confidence: 99%