“Green”, gradient multi-shell CuInSe2/(CuInSexS1-x)5/CuInS2 quantum dots for photo-electrochemical hydrogen generation

Li, Faying; Zhang, Min; Benetti, Daniele; Shi, Li; Besteiro, Lucas V.; Zhang, Hui; Liu, Jiabin; Selopal, Gurpreet Singh; Sun, Shuhui; Wang, Zhiming; Wei, Qin; Rosei, Federico

doi:10.1016/j.apcatb.2020.119402

Cited by 49 publications

(55 citation statements)

References 67 publications

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“…The as-obtained QDs sensitized TiO 2 PEC photoanodes showed outstanding saturated photocurrent density as high as 3 mA cm −2 , which is about twice as high as that obtained using pure CuInSe 2 . Li et al [172] introduced a graded CuInSe x S 1-x interfacial layer into CuInSe 2 /CuInS 2 QDs, achieving an improvement of 70% in saturated photocurrent density (≈4.5 mA cm −2 ) compared to that of CuInSe 2 /CuInS 2 QDs [44e] by increasing the leakage of both electrons and holes to the QDs' surface and reducing the lattice mismatch between core and shell. The current PL and PEC conversion efficiency is still lower than values reported for heavy-metal-based QDs, mostly due to unwanted charge traps.…”

Section: Developing Heavy-metal Free Qdsmentioning

confidence: 99%

“…For example, introducing an alloyed layer CuInSe x S 1-x into the thick-shell CuInSe 2 /CuInS 2 [44e] yields CuInSe 2 /CuInSe x S 2-x /CuInS 2 QDs. [172] In addition, nontoxic unary QDs, such as carbon QDs and Si QDs, are promising and should be further pursued to optimize their structure/property relationships. Considering their narrow absorption range (mainly UV and visible), a promising future direction would consist in developing processes that can extend their absorption range.…”

Section: Conclusion and Perspectivementioning

confidence: 99%

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Quantum Dots‐Based Photoelectrochemical Hydrogen Evolution from Water Splitting

Liu

Zhao

Wang

et al. 2021

Advanced Energy Materials

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opportunity since it is by far the most abundant, sustainable, carbon-neutral, and inexpensive energy source. The theoretical potential of solar power striking the earth's surface is ≈89 300 TW (the integral of the time-and-space-averaged solar flux 342.5 W m −2 over the earth's surface area 5.11 × 10 14 m 2 , estimating that ≈30% and ≈19% are scattered and absorbed by the atmosphere and clouds), [3] which is equivalent to ≈6000 times the power used worldwide every year (estimated at 13.5 TW in 2001, with projected growth up to 27.6 TW by 2050 by the Intergovernmental Panel on Climate Change). [4] In particular, storing solar energy in the form of H 2 presents advantages such as high energy content per mass (143 MJ kg −1), ease of transportation, and cost-effectiveness, [5] thereby addressing the storage challenge which is associated with the diffuse and intermittent character of solar irradiation. Solar energy and water could be converted into H 2 [5b] indirectly by using solar-converted electricity and an electrolyzer, [6] concentrated solar thermal and an electrolyzer, [7] biological and thermochemical processes [8] or directly by photo-/photoelectrocatalysis of water. [1b,f,g] The combination of the energy conversion step with electrolyzers is always limited by the performance of the electrolyzers, whose typical commercial efficiencies are around 73%. [9] Besides, indirect technologies suffer from excessive cost, area requirements, feasibility issues, or energy loss. [10] An alternative direct route is the photo-/photoelectrocatalysis of water, including powdered photocatalysts [11] and photoelectrochemical (PEC) cells. [12] The dispersion of powdered photocatalysts in water is suitable for large-scale processes, while the system requires stirring during the reaction and product separation after the reaction. In comparison, PEC systems (Figure 1a), which combine harvesting solar energy with water reduction into a single device, possesses several advantages. [13] i) PEC reactions address the issue of gas separation by generating products at different electrodes. ii) An external bias supply or self-bias voltage in the PEC system can provide additional energy input to compensate for the potential deficiency, [14] leading to the formation of a surface space charge layer and achieving efficient charge separation and an increased number of long-living photogenerated charges. [15] iii) Moreover, PEC systems can potentially be operated using only stable and abundant materials, such as Cu-based metal oxides, [16] Fe 2 O 3 , [14b,17] and TiO 2. [18] In a typical PEC system, at least one photoelectrode is used as a working electrode to harvest solar radiation, either acting Solar-driven photoelectrochemical (PEC) hydrogen evolution is a promising and sustainable approach to convert solar energy into a fuel that can be stored. Semiconductor quantum dots (QDs) are increasingly used in PEC devices due to their broad composition/size/shape tunable absorption spectrum (from ultraviolet to near-infrared, with significant over...

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Section: Developing Heavy-metal Free Qdsmentioning

confidence: 99%

Section: Conclusion and Perspectivementioning

confidence: 99%

Quantum Dots‐Based Photoelectrochemical Hydrogen Evolution from Water Splitting

Liu

Zhao

Wang

et al. 2021

Advanced Energy Materials

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“…As shown in Figure 4d and Table S2 (Supporting Information), the R CT follows the inverse trend of the photocurrent, with the 10 Zn-MoS 2 /PbS@CdS QDs sample presenting the smallest R CT value, indicating a lower charge transfer resistance and superior charge transfert kinetics at the electrolyte/catalyst interface. [40] As the photoanodes are constructed in similar way, the improved charge transfer can be assigned to the favorable band alignment for charge separation of photoexcited charges between QDs and 10 Zn-MoS 2 , confirming that the recombination of electron/hole pairs is strongly reduced in this kind of architecture.…”

Section: Pec Performancementioning

confidence: 70%

Modulating the 0D/2D Interface of Hybrid Semiconductors for Enhanced Photoelectrochemical Performances

Benetti

Zhang

et al. 2021

Small Methods

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Despite major progress, these materials still face several significant challenges. In particular: 1) metal oxides usually possess a large bandgap that limits the sunlight absorption, 2) not all metal oxides have a favorable band alignment to realize both redox processes (water reduction and oxidation), 3) low electrical conductivity and limited hole diffusion length, 4) charge recombination can occur easily in the bulk and on the surface, limiting the efficiency of the system.Recently, extensive efforts have been made to explore non-oxide nanomaterials, such as metal chalcogenides (MoS 2 , CdS, etc.), and metal-free photocatalysts (g-C 3 N 4 , etc.) to enhance PEC activity thanks to their small bandgap, that allows to harvest a wide range of the solar spectrum. [4] On the other hand, the fabrication of heterojunction structures is considered as a promising approach to improve PEC performance [5] due to several advantages: 1) extension of the light absorption range; 2) effective separation of electron-hole pairs; 3) reduction of the recombination of photogenerated carriers.Heterostructure based on 0D/2D interfaces are particularly interesting due to the possibility of easily construct intimate interfaces. Among a wide gamut of 0D/2D heterostructure, quantum dots (QDs)/ 2D nanosheets (NSs) are promising for enhancing photoexcited electron/hole transfer due to their high charge mobility. [6] In a QDs/NSs heterostructure, a very intimate interface between the two is created, and since processes such as exciton dissociation and charge injection are critically dependent on the QD-surface distance, they will be enhanced. [7] Further, the presence of a 2D material can provide several superior features (compared to 0D and 1D nanomaterials) such as a significant increase of the material surface area, extended contact between the assembly and the electrolyte, and most remarkably, preferential electrical transport that can suppress charge carrier recombination and overall improve the functional PEC properties. [4a,8] Based on these advantages, the 0D/2D hybrid can combine the strong light harvesting capability of QDs with the catalytic performance of 2D platform.Here we describe the design and fabrication of a 0D/2D heterostructure based on a nanoflower-like hierarchical MoS 2 NSs assembly and on metal chalcogenide QDs, such as PbS, CdS, and their composite, PbS@CdS. MoS 2 is a widely studied Photoelectrochemical (PEC) solar-driven hydrogen production is a promising route to convert solar energy into chemical energy using semiconductors as active materials. However, the performance is still far from satisfactory due to a limited absorption range and rapid charge recombination. Compared to 3D semiconductors, 0D/2D nanohybrids may exhibit better PEC performance, due to the formation of an intimate interface between the two semiconductors that can inhibit carrier recombination. Herein, a photoelectrode based on a 0D/2D heterojunction is constructed by 0D metal chalcogenide quantum dots (QDs) and hierarchical 2D Zn-MoS 2 nanos...

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“…Photocatalytic technique is a compelling strategy for aquatic and environmental remediation owning to its relatively low cost and robust chemical stability with no secondary pollution [12,13]. Solar energy can stimulate catalysts to generate photoelectron holes and produce active radicals ( • OH, • O 2 − ), which can destroy or oxidate organic matters [14][15][16]. Howbeit, due to the low solar energy utilization associated with easy recombination of e − -h + pairs, the degradation efficiency of photocatalyst is limited [17][18][19].…”

Section: Introductionmentioning

confidence: 99%

High-Efficiency Wastewater Purification System Based on Coupled Photoelectric–Catalytic Action Provided by Triboelectric Nanogenerator

Shen

Jia

et al. 2021

Nano-Micro Lett.

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It is of great importance to explore a creative route to improve the degradation efficiency of organic pollutants in wastewater. Herein, we construct a unique hybrid system by combining self-powered triboelectric nanogenerator (TENG) with carbon dots-TiO2 sheets doped three-dimensional graphene oxide photocatalyst (3DGA@CDs-TNs), which can significantly enhance the degradation efficiency of brilliant green (BG) and direct blue 5B (DB) owing to the powerful interaction of TENG and 3DGA@CDs-TNs photocatalyst. The power output of TENG can be applied for wastewater purification directly, which exhibits a self-powered electrocatalytic technology. Furthermore, the results also verify that TENG can replace conventional electric catalyst to remove pollutants effectively from wastewater without any consumption. Subsequently, the unstable fragments and the plausible removal pathways of the two pollutants are proposed. Our work sheds light on the development of efficient and sustainable TENG/photocatalyst system, opening up new opportunities and possibilities for comprehensive utilization of random energy.

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“Green”, gradient multi-shell CuInSe2/(CuInSexS1-x)5/CuInS2 quantum dots for photo-electrochemical hydrogen generation

Cited by 49 publications

References 67 publications

Quantum Dots‐Based Photoelectrochemical Hydrogen Evolution from Water Splitting

Quantum Dots‐Based Photoelectrochemical Hydrogen Evolution from Water Splitting

Modulating the 0D/2D Interface of Hybrid Semiconductors for Enhanced Photoelectrochemical Performances

High-Efficiency Wastewater Purification System Based on Coupled Photoelectric–Catalytic Action Provided by Triboelectric Nanogenerator

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