Revealing the Correlation of the Electrochemical Properties and the Hydration of Inkjet-Printed CdSe/CdS Semiconductor Gels

Miethe, Jan F.; Luebkemann, Franziska; Schlosser, Anja; Dorfs, Dirk; Bigall, Nadja C.

doi:10.1021/acs.langmuir.9b03708

Cited by 10 publications

(21 citation statements)

References 51 publications

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“…The elongation results when electrons from further distances reach the electrode, which is observed at lower frequencies due to the larger timescale of the electron transport through the network. [21,42,43] Thus, the elongation suggests electron mobility within the semiconductor network, and consequently indicates larger metal-to-metal domain distances in the interconnected tipped structure. These tipped structures possess only one Au domain on each semiconductor NR which leads as well to semiconductor-semiconductor contacts that enable the electron delocalization and transport within larger parts of the network.…”

Section: Mechanism Of the Charge Carrier Dynamicsmentioning

confidence: 99%

Revealing the Effect of Nanoscopic Design on the Charge Carrier Separation Processes in Semiconductor‐Metal Nanoparticle Gel Networks

Schlenkrich

Zámbó

Schlosser

et al. 2021

Advanced Optical Materials

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Section: Mechanism Of the Charge Carrier Dynamicsmentioning

confidence: 99%

Revealing the Effect of Nanoscopic Design on the Charge Carrier Separation Processes in Semiconductor‐Metal Nanoparticle Gel Networks

Schlenkrich

Zámbó

Schlosser

et al. 2021

Advanced Optical Materials

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“…As we have shown through numerous different gelation techniques recently, the assembly of these NCs provides a platform toward novel fluorescent superstructures with exceptionally high specific surface area, low density and promising (electro) catalytic performance. [7][8][9][10][11][12] Conduction band offset in CdSe/CdS heterojunction indicates the formation of quasi-type II structure, in which the hole is confined in the core and the electron can delocalize in the shell. [13] While this is valid for nanorods, core/ crown nanoplatelets (NPLs) show type I band alignment despite the same heterojunction.…”

Section: Introductionmentioning

confidence: 99%

One‐Step Formation of Hybrid Nanocrystal Gels: Deposition of Metal Domains on CdSe/CdS Nanorod and Nanoplatelet Networks

Zámbó

Schlosser

Graf

et al. 2021

Advanced Optical Materials

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Hybrid semiconductor‐based nanocrystals (NCs) are generally synthesized in organic media prior to their assembly into catalytically promising nanostructures via multistep methods. Here, a tunable, easy‐to‐adapt and versatile approach for the preparation of hybrid nanoparticle networks from aqueous nanocrystal solutions is demonstrated. The networks consist of interconnected semiconductor NC backbones (made of CdSe/CdS dot‐in‐rods or core/crown nanoplatelets) decorated with noble metal (Au and Pt) or with metal‐based domains (Co2+ and Ni2+) demonstrating a powerful synthetic control over a variety of hybrid nanostructures. The deposition of the domains and the formation of the network take place simultaneously (one‐step method) at room temperature in dark conditions without any external trigger. Beside the in‐depth structural characterization of the gel‐like hybrid networks, the wavelength‐dependent optical features are studied to reveal an efficient charge carrier separation in the systems and a controllable extent of fluorescence quenching through the domain sizes. Photoluminescence quantum yields and decay dynamics highlight the importance of fine‐tuning the conduction band/Fermi level offset between the semiconductors and the various deposited metals playing central role in the electron–hole separation processes. This procedure provides a novel platform toward the preparation of photo(electro)catalytically promising hybrid nanostructures (acetogels and xerogels) without the need of presynthetic hybrid particle design.

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Section: Nanostructuring I: Tailoring the Composition And Shape Of Thmentioning

confidence: 99%

“… 64 , 65 In our works, we first applied similar techniques for electrode production based on doctor blade casting of a NC solution and rapid freezing 32 or the gelation of NC solutions within molds. 66 …”

Section: Macrostructuring: Shaping the Monolith By Molding And Printimentioning

confidence: 99%

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Control over Structure and Properties in Nanocrystal Aerogels at the Nano-, Micro-, and Macroscale

2020

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Conspectus The assembly of individual colloidal nanocrystals into macroscopic solvogels and aerogels introduced a new exciting type of material into the class of porous architectures. In these so-called nanocrystal gels, the structure and properties can be controlled and fine-tuned to the smallest details. Recently it was shown that by employing nanocrystal building blocks for such gel materials, the interesting nanoscopic properties can be conserved or even expanded to properties that are available neither in the nanocrystals nor in their respective bulk materials. In general, the production of these materials features the wet-chemical synthesis of stable nanocrystal colloids followed by their carefully controlled destabilization to facilitate arrangement of the nanocrystals into highly porous, interconnected networks. By isolation of the synthesis of the discrete building blocks from the assembly process, the electronic structure, optical properties, and structural morphology can be tailored by the myriad of procedures developed in colloidal nanocrystal chemistry. Furthermore, knowledge and control over the structure–property correlation in the resulting gel structures opens up numerous new ways for extended and advanced applications. Consequently, the amount of different materials converted to nanocrystal-based gel structures is rising steadily. Meanwhile the number of methods for assembly initiation is likewise increasing, offering control over the overall network structure and porosity as well as the individual nanocrystal building block connection. The resulting networks can be dried by different methods to obtain highly porous air-filled networks (aerogels) or applied in their wet form (solvogels). By now a number of different applications profiting from the unique advantages of nanocrystal-based gel materials have been realized and exploited in the areas of photocatalysis, electrocatalysis, and sensing. In this Account, we aim to summarize the efforts undertaken in the structuring of nanocrystal-based network materials on different scales, fine-tuning of the individual building blocks on the nanoscale, the network connections on the microscale, and the macroscale structure and shape of the final construct. It is exemplarily demonstrated how cation exchange reactions (at the nanoscale), postgelation modifications on the nanocrystal networks (microscale), and the structuring of the gels via printing techniques (macroscale) endow the resulting nanocrystal gel networks with novel physicochemical, mechanical, and electrocatalytic properties. The methods applied in the more traditional sol–gel chemistry targeting micro- and macroscale structuring are also reviewed, showing their future potential promoting the field of nanocrystal-based aerogels and their applications.

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Revealing the Correlation of the Electrochemical Properties and the Hydration of Inkjet-Printed CdSe/CdS Semiconductor Gels

Cited by 10 publications

References 51 publications

Revealing the Effect of Nanoscopic Design on the Charge Carrier Separation Processes in Semiconductor‐Metal Nanoparticle Gel Networks

Revealing the Effect of Nanoscopic Design on the Charge Carrier Separation Processes in Semiconductor‐Metal Nanoparticle Gel Networks

One‐Step Formation of Hybrid Nanocrystal Gels: Deposition of Metal Domains on CdSe/CdS Nanorod and Nanoplatelet Networks

Control over Structure and Properties in Nanocrystal Aerogels at the Nano-, Micro-, and Macroscale

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