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1.
Angew Chem Int Ed Engl ; 59(4): 1696-1702, 2020 Jan 20.
Artigo em Inglês | MEDLINE | ID: mdl-31638732

RESUMO

Solar radiation is a versatile source of energy, convertible to different forms of power. A direct path to exploit it is the generation of heat, for applications including passive building heating, but it can also drive secondary energy-conversion steps. We present a novel concept for a hybrid material which is both strongly photo-absorbing and with superior characteristics for the insulation of heat. The combination of that two properties is rather unique, and make this material an optical superheater. To realize such a material, we are combining plasmonic nanoheaters with alumina aerogel. The aerogel has the double function of providing structural support for plasmonic nanocrystals, which serve as nanoheaters, and reducing the diffusion rate of the heat generated by them, resulting in large local temperature increases under a relatively low radiation intensity. This work includes theoretical discussion on the physical mechanisms impacting the system's balanced thermal equilibrium.

2.
RSC Adv ; 10(4): 2277-2282, 2020 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-35494579

RESUMO

In order to enable future use of aerogels in heterogeneous solid or fluidized bed catalysis a method of production of millimeter sized monolithic Au/Al2O3 aerogel spheres by a continuous flow reactor is developed. Flow velocities and synthesis parameters are optimized to produce aerogel spheres in three different sizes. The resulting aerogel spheres exhibit a porous aluminium oxide aerogel matrix with a large specific surface area of 400 m2 g-1 on which gold nanoparticles are evenly distributed. The aerogel spheres are compared to xerogels of the same material in contrast to their surface area, pore size distribution, morphology, crystal structure and thermal properties. The presented method allows a broad access to various mixed aerogel systems of oxidic carrier material and noble metal nanoparticles and is therefore relevant for the shaping of different aerogel catalyst systems.

3.
Adv Mater ; 29(11)2017 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-28060420

RESUMO

A new class of multimetallic hierarchical aerogels composed entirely of interconnected Ni-Pdx Pty nano-building-blocks with in situ engineered morphologies and compositions is demonstrated. The underlying mechanism of the galvanic shape-engineering is elucidated in terms of nanowelding of intermediate nanoparticles. The hierarchical aerogels integrate two levels of porous structures, leading to improved electrocatalysis performance.

4.
ACS Appl Mater Interfaces ; 8(33): 21570-5, 2016 Aug 24.
Artigo em Inglês | MEDLINE | ID: mdl-27482755

RESUMO

Since the beginning of the 1980s, colloidally synthesized quantum dots (QDs) have been in the focus of interest due to their possible implementation for color conversion, luminescent light concentrators, and lasing. For all these applications, the QDs benefit from being embedded into a host matrix to ensure stability and usability. Many different host materials used for this purpose still have their individual shortcomings. Here, we present a universal, fast, and flexible approach for the direct incorporation of a wide range of QDs into inorganic ionic crystals using cold flow. The QD solution is mixed with a finely milled salt, followed by the removal of the solvent under vacuum. Under high pressure (GPa), the salt powder loaded with QDs transforms into transparent pellets. This effect is well-known for many inorganic salts (e.g., KCl, KBr, KI, NaCl, CsI, AgCl) from, e.g., sample preparation for IR spectroscopy. With this approach, we are able to obtain strongly luminescent QD-salt composites, have precise control over the loading, and provide a chemically robust matrix ensuring long-term stability of the embedded QDs. Furthermore, we show the photo-, chemical, and thermal stability of the composite materials and their use as color conversion layers for a white light-emitting diode (w-LED). The method presented can potentially be used for all kinds of nanoparticles synthesized in organic as well as in aqueous media.

5.
Angew Chem Int Ed Engl ; 55(21): 6334-8, 2016 05 17.
Artigo em Inglês | MEDLINE | ID: mdl-27100131

RESUMO

We report an efficient approach to assemble a variety of electrostatically stabilized all-inorganic semiconductor nanocrystals (NCs) by their linking with appropriate ions into multibranched gel networks. These all-inorganic non-ordered 3D assemblies benefit from strong interparticle coupling, which facilitates charge transport between the NCs with diverse morphologies, compositions, sizes, and functional capping ligands. Moreover, the resulting dry gels (aerogels) are highly porous monolithic structures, which preserve the quantum confinement of their building blocks. The inorganic semiconductor aerogel made of 4.5 nm CdSe colloidal NCs capped with I(-) ions and bridged with Cd(2+) ions had a large surface area of 146 m(2) g(-1) .

6.
Angew Chem Int Ed Engl ; 54(44): 13101-5, 2015 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-26356131

RESUMO

One plausible approach to endow aerogels with specific properties while preserving their other attributes is to fine-tune the building blocks. However, the preparation of metallic aerogels with designated properties, for example catalytically beneficial morphologies and transition-metal doping, still remains a challenge. Here, we report on the first aerogel electrocatalyst composed entirely of alloyed PdNi hollow nanospheres (HNSs) with controllable chemical composition and shell thickness. The combination of transition-metal doping, hollow building blocks, and the three-dimensional network structure make the PdNi HNS aerogels promising electrocatalysts for ethanol oxidation. The mass activity of the Pd83 Ni17 HNS aerogel is 5.6-fold higher than that of the commercial Pd/C catalyst. This work expands the exploitation of the electrocatalysis properties of aerogels through the morphology and composition control of its building blocks.

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