Efficient photocatalytic hydrogen evolution with ligand engineered all-inorganic InP and InP/ZnS colloidal quantum dots

Yu, Shan; Fan, Xiang‐Bing; Wang, Xian; Li, Jingguo; Zhang, Qian; Xia, Andong; Wei, Shiqian; Wu, Li‐Zhu; Zhou, Ying; Patzke, Greta R.

doi:10.1038/s41467-018-06294-y

Cited by 216 publications

(230 citation statements)

References 69 publications

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“…Among various kinds of photocatalysts, metal sulfides exhibit many advantages due to their suitable band structure and strong visible-light absorption. Many research works focused on sulfides such as CdS, [21][22][23][24] ZnS, 25 CuInS2 26 have been reported; meanwhile, the development of other metal sulfides is necessary. 27 In our previous work, 28 we discovered that MnS/In2S3 composite is an effective photocatalyst for hydrogen evolution from H2S in the visible light region.…”

Section: Introductionmentioning

confidence: 99%

Highly dispersed PdS preferably anchored on In2S3 of MnS/In2S3 composite for effective and stable hydrogen production from H2S

Doronkin

et al. 2019

Journal of Catalysis

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As an important byproduct during natural gas exploitation, green utilization of hydrogen sulfide (H2S) by photocatalysis has offered us the possibility for production of clean hydrogen (H2) from H2S with low energy consumption. In this work, we have successfully introduced well-dispersed palladium sulfide (PdS) which is preferably loaded on In2S3 of MnS/In2S3 composite for improved photocatalytic hydrogen evolution from H2S aqueous solution. In contrast to binary MnS/In2S3, ternary MnS/In2S3/PdS has exhibited a remarkable and stable hydrogen production rate of 22.7 mmol g-1 h-1 with an apparent quantum yield of 34 % at around 395 nm. A comprehensive structure characterization of the ternary composite including scanning transmission electron microscopy (STEM) and X-ray absorption spectroscopy (XAS) in combination with theoretical calculations confirm the good dispersion of PdS in the composite. Moreover, we discovered that PdS preferably interact with In2S3 rather than MnS in the composite through Pd-SIn bond on the interface of the two. Photoluminescence (PL) spectra, surface photovoltage (SPV) spectra together with transient photocurrent and electrochemical impedance spectra (EIS) demonstrate the advantage of PdS for promoting the charge separation. Due to the corrosion-resistant nature of PdS in H2S-rich reaction media, MnS/In2S3/PdS present good stability as well. This work sheds light on the positive effect on the enhanced activity and stability of the corresponding system resulting from the preferable anchoring of highly dispersed PdS on In2S3 in the composite by chemical Pd-SIn bond. Not only the high dispersion but also the preferable anchoring of the cocatalyst in the composite could hence inspire people for more rational designs of ternary composite in future.

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Section: Introductionmentioning

confidence: 99%

Highly dispersed PdS preferably anchored on In2S3 of MnS/In2S3 composite for effective and stable hydrogen production from H2S

Doronkin

et al. 2019

Journal of Catalysis

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“…Figure 2a shows a trace amount of InP QDs deposited onto CdS NRs. The high-resolution TEM (HR-TEM) image of the composite (Figure 2b) clearly demonstrated two lattice spacings of 0.33 nm and 0.34 nm, which were assigned to CdS, [57] and InP, [47] respectively. The elemental compositions determined through EDS mapping ( Figure S3) evidenced the distribution of InP QDs on CdS NRs.…”

Section: Resultsmentioning

confidence: 99%

Indium Phosphide Quantum Dots Integrated with Cadmium Sulfide Nanorods for Photocatalytic Carbon Dioxide Reduction

et al. 2020

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Photocatalytic conversion of CO 2 into storable fuels is an attractive way to simultaneously address worldwide energy demands and environmental problems. Semiconductor quantum dots (QDs) have gained prominence as candidates for photocatalytic applications due to their many advantages, which include tunability for advanced electronic, optical, and surface properties. Indium phosphide (InP) quantum dots are semiconducting QDs with enormous potential for solar-driven CO 2 reduction. Their advantages include a tunable bandgap, diverse surface chemistry, and nontoxicity. InP QDs and CdS nanorods were integrated using a simple and inexpensive method. CO 2 photoreduction by the CdS-InP composites was evaluated in aqueous solution using triethanolamine as a sacrificial donor. The crystal structures, surface compositions, and morphologies were investigated via X-ray diffraction analysis, X-ray photoelectron spectroscopy, and transmission electron microscopy, respectively. The UV-visible diffuse reflectance spectra of the CdS-InP composites indicated efficient visible light utilization in the 500-550 nm range. The results of photoelectrochemical and photoluminescence analyses illustrated effective charge separation in the composites. The photocatalytic activity of the as-synthesized composites was superior to that of pure CdS. The CO evolution rate of the optimized composite was 216 μmol h À 1 g À 1 during the first three hours of irradiation and increased steadily over the next 62 hours. We also studied the influences of different solvents, the hole scavenger concentration, and catalyst loading on the performance of the optimized composite.

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“…Type‐I band alignment might prevent the ability to extract the charge carriers from the core to achieve photocatalytic functionality but a thin shell may still allow this. We use Ni(NO 3 ) 2 as a co‐catalyst and L‐ascorbic acid (AA) as a hole acceptor, a system known to have high efficiency in hydrogen formation for zinc chalcogenide nanocrystals and other colloidal semiconductor nanocrystals . The NRs solution was irradiated with a 30 mW LED at 365 nm during which the amount of hydrogen gas produced was determined in situ using gas chromatography (see SI and Figure S5 for further details).…”

Section: Resultsmentioning

confidence: 99%

Shell Stabilization of Photocatalytic ZnSe Nanorods

et al. 2019

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Zinc chalcogenides nanostructures are promising newly-studied materials for photocatalytic reactions such as water reduction for hydrogen generation and photoinitiation of radical polymerization processes. Herein, we introduced a straightforward synthesis of thin ZnS shell on ZnSe nanorods and characterized the resulting core/shell ZnSe/ZnS nanorods by electron microscopy techniques and X-ray photoelectron spectroscopy. Then, the photocatalytic activities of the nanorods were studied by gas chromatography for hydrogen generation and by Fourier transform infrared spectroscopy for the photoinitiation capability. While such core/shell systems may limit charge transfer to the solution due to the type-I band alignment, we find that the photochemical stability and photocatalytic activity of this system is significantly enhanced over pristine ZnSe nanorods. ZnSe/ZnS nanorods with Ni(NO 3 ) 2 co-catalyst are used for hydrogen generation and the effects of the nanorods' surface coating, pH conditions and type of hole scavenger are examined. The best performances were observed for nanorods after ligand stripping with Meerwein's reagent using ascorbic acid as a hole acceptor at pH 4.5. All three parameters were found to affect the photocatalytic activity. Yet, the surface coating and pH dependence differ from previous reports on cadmium chalcogenides photocatalysts. The origin of their differences is discussed and attributed to the band alignment of the systems and the nature of the co-catalyst. The stable heavy-metal free ZnSe/ZnS nanorods system presented here holds promise for various photocatalytic applications.

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Efficient photocatalytic hydrogen evolution with ligand engineered all-inorganic InP and InP/ZnS colloidal quantum dots

Cited by 216 publications

References 69 publications

Highly dispersed PdS preferably anchored on In2S3 of MnS/In2S3 composite for effective and stable hydrogen production from H2S

Highly dispersed PdS preferably anchored on In2S3 of MnS/In2S3 composite for effective and stable hydrogen production from H2S

Indium Phosphide Quantum Dots Integrated with Cadmium Sulfide Nanorods for Photocatalytic Carbon Dioxide Reduction

Shell Stabilization of Photocatalytic ZnSe Nanorods

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