Simple Setup Miniaturization with Multiple Benefits for Green Chemistry in Nanoparticle Synthesis

Mathiesen, Jette K.; Cooper, Susan; Anker, Andy S.; Kinnibrugh, Tiffany L.; Jensen, Kirsten M. Ø.; Quinson, Jonathan

doi:10.1021/acsomega.2c00030

Cited by 9 publications

(14 citation statements)

References 54 publications

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“…The NP synthesis was performed following a previously reported method. ,, A solution containing either IrCl 3 · x H 2 O (99.9%, Alfa Aesar), IrCl 4 (99.9%, Alfa Aesar), H 2 IrCl 6 ·H 2 O (99.9%, Aldrich), or Na 2 IrCl 6 ·6H 2 O (99.9% trace metals basis) as metal ion precursor in alkaline LiOH (anhydrous 98%, Alfa Aesar), NaOH (98%, Alfa Aesar), KOH (KOH . x H 2 O, ≥99.995%, Fluka), or CsOH (99.95%, Aldrich) in methanol (MeOH, ≥99.9%, HiPerSolv CHROMANORM, VWR) was obtained by mixing a stock solution of the metal ion precursor with a solution of the base of interest in MeOH.…”

Section: Methodsmentioning

confidence: 99%

“…Colloidal synthesis methods generally rely on the use of additives, such as surfactants, polymers, polyoxanions, or ionic liquids, and it is challenging to assess the effect(s) of these additives in the formation of NPs. We overcome these challenges using a surfactant-free synthesis of Ir NPs that can be performed at high metal concentration of 100 mM, which makes it compatible with in situ X-ray total scattering (TS) experiments with pair distribution function (PDF) analysis to gain new insights into the structural chemistry of Ir NP formation. We first report the formation of surfactant-free Ir NPs in alkaline methanol (MeOH) using different precursors, e.g., IrCl 3 , IrCl 4 , and H 2 IrCl 6 .…”

Section: Introductionmentioning

confidence: 99%

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Chemical Insights into the Formation of Colloidal Iridium Nanoparticles from In Situ X-ray Total Scattering: Influence of Precursors and Cations on the Reaction Pathway

et al. 2023

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Iridium nanoparticles are important catalysts for several chemical and energy conversion reactions. Studies of iridium nanoparticles have also been a key for the development of kinetic models of nanomaterial formation. However, compared to other metals such as gold or platinum, knowledge on the nature of prenucleation species and structural insights into the resultant nanoparticles are missing, especially for nanoparticles obtained from Ir x Cl y precursors investigated here. We use in situ X-ray total scattering (TS) experiments with pair distribution function (PDF) analysis to study a simple, surfactant-free synthesis of colloidal iridium nanoparticles. The reaction is performed in methanol at 50 °C with only a base and an iridium salt as precursor. From different precursor salts�IrCl 3 , IrCl 4 , H 2 IrCl 6 , or Na 2 IrCl 6 �colloidal nanoparticles as small as Ir ∼55 are obtained as the final product. The nanoparticles do not show the bulk iridium face-centered cubic (fcc) structure but show decahedral and icosahedral structures. The formation route is highly dependent on the precursor salt used. Using IrCl 3 or IrCl 4 , metallic iridium nanoparticles form rapidly from Ir x Cl y n− complexes, whereas using H 2 IrCl 6 or Na 2 IrCl 6 , the iridium nanoparticle formation follows a sudden growth after an induction period and the brief appearance of a crystalline phase. With H 2 IrCl 6 , the formation of different Ir n (n = 55, 55, 85, and 116) nanoparticles depends on the nature of the cation in the base (LiOH, NaOH, KOH, or CsOH, respectively) and larger particles are obtained with larger cations. As the particles grow, the nanoparticle structure changes from partly icosahedral to decahedral. The results show that the synthesis of iridium nanoparticles from Ir x Cl y is a valuable iridium nanoparticle model system, which can provide new compositional and structural insights into iridium nanoparticle formation and growth.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Chemical Insights into the Formation of Colloidal Iridium Nanoparticles from In Situ X-ray Total Scattering: Influence of Precursors and Cations on the Reaction Pathway

et al. 2023

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“…To comply with the requirement of the measurement, the synthesis was performed in 3 mm diameter NMR (Wildmad®, 3 mm outer diameter, 0.27 mm wall thickness, Type 1 Class A) tubes at RT. 30 The time of synthesis is expressed as the time after mixing all the chemicals and no data could be acquired for few minutes which correspond to the time needed to start the measurement.…”

Section: Chemicalsmentioning

confidence: 99%

Surfactant-free colloidal syntheses of gold-based nanomaterials in alkaline water and mono-alcohol mixtures

Quinson

Aalling‐Frederiksen

Dacayan

et al. 2023

Preprint

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Gold nanoparticles (AuNPs) and gold-based nanomaterials combine unique properties relevant for medicine, biomedical applications, imaging, optics, sensing, catalysis or energy conversion. While the Turkevich-Frens and Brust-Schiffrin methods remain the state-of-the-art colloidal syntheses of AuNPs, there is a need for more sustainable and tractable strategies. Here, a reproducible and scalable surfactant-free synthesis of stable colloidal AuNPs with multiple benefits is achieved by the simple reduction of HAuCl4 at room temperature in alkaline solutions of mono-alcohols and water. A parametric study including more than 350 experiments shows that mixing different alcohols is a simple strategy for achieving size control in the range 6-30 nm in diameter and the order of addition of the chemicals strongly affects the outcome of the synthesis. The synthesis method also applies to surfactant-free palladium (Pd) and bimetallic AuxPdy NPs, nanocomposites and multi-metallic samples, all readily active (electro)catalysts. The simple synthesis bears promising features for fundamental and applied research.

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“…252 Pt has been the most studied materials and size controlled achieved by using alcohol/water mixtures. To date, size control remains more challenging for Ir NPs 253,254 or Os NPs, 254,255 as summarized in Table 2. In the case of Ir and Os NPs, actually no base is needed to obtain NPs, 255,256 but the activity and probably the yield of the synthesis are improved using alkaline conditions.…”

Section: Ii6 Surfactant-free Mono-alcohol Synthesismentioning

confidence: 99%

“…258,259 One drawback of the synthesis is to require relatively low concentration of precursor in the case of Pt (2.5 mM) 22 but was shown to lead to small size Ir NPs even at high precursor concentration of 100 mM. 254 The related Ir NPs were shown to be up to ten time more active than the state-of-the-art for the OER. 22,259 It is expected that the high activity of the catalyst obtained will help to discriminate in more depth NP size or support effects.…”

Section: Ii6 Surfactant-free Mono-alcohol Synthesismentioning

confidence: 99%

Surfactant-free colloidal syntheses of precious metal nanoparticles for improved catalysts

Quinson

Kunz²,

Arenz

2022

Preprint

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Colloidal syntheses of nanomaterials offer multiple benefits to study, understand and optimize un-supported and supported catalysts. In particular, colloidal syntheses are relevant to synthetize (precious) metal nanoparticles. By separating the synthesis of the active phase nanoparticles from supporting steps, a deeper knowledge and a rational control on supported catalyst properties is gained. The effect of nanoparticle size, shape, composition, nature of support or metal loading on a support can be studied in more systematic ways. The fundamental knowledge gained paves the way for catalyst optimization by tuning the catalyst activity, selectivity, and stability. However, a major drawback is that most colloidal syntheses require the use of additives or surfactants, which are detrimental to most catalytic reactions since they typically block catalyst active sites. Surfactant removal typically adds complexity, can introduce a lack of reproducibility, is energy consuming, generates waste, and prevents the full exploitation of the many benefits of colloidal syntheses for catalysis. Several surfactant-free strategies to obtain stable colloidal nanoparticles are here reviewed. A focus is given to laser synthesis and processing of colloids (LSPC), solution plasma process (SPP), N,N-dimethylformamide (DMF), polyols, and recently reported mono-alcohols based syntheses. The relevance of these synthetic approaches for catalysis is detailed with a focus on heterogeneous catalysis and electro-catalysis.

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Simple Setup Miniaturization with Multiple Benefits for Green Chemistry in Nanoparticle Synthesis

Cited by 9 publications

References 54 publications

Chemical Insights into the Formation of Colloidal Iridium Nanoparticles from In Situ X-ray Total Scattering: Influence of Precursors and Cations on the Reaction Pathway

Chemical Insights into the Formation of Colloidal Iridium Nanoparticles from In Situ X-ray Total Scattering: Influence of Precursors and Cations on the Reaction Pathway

Surfactant-free colloidal syntheses of gold-based nanomaterials in alkaline water and mono-alcohol mixtures

Surfactant-free colloidal syntheses of precious metal nanoparticles for improved catalysts

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