Assembling Inorganic Nanocrystal Gels

Green, Allison; Ofosu, Charles K.; Kang, Jiho; Anslyn, Eric V.; Truskett, Thomas M.; Milliron, Delia J.

doi:10.1021/acs.nanolett.1c04707

Cited by 40 publications

(49 citation statements)

References 64 publications

(157 reference statements)

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“… 18 − 24 However, combining more than one type of nanoparticle component presents a further level of challenge, and selective coupling in multicomponent mixtures is rarely seen. 18 − 24 The broad structural and compositional diversity now accessible for colloidal nanoparticles suggests vast potential for tuning composite material properties if multiple types of instructable nanoscale building block can be connected with high selectivity.…”

Section: Introductionmentioning

confidence: 99%

Constitutionally Selective Dynamic Covalent Nanoparticle Assembly

et al. 2022

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The future of materials chemistry will be defined by our ability to precisely arrange components that have considerably larger dimensions and more complex compositions than conventional molecular or macromolecular building blocks. However, exerting structural and constitutional control in the assembly of nanoscale entities presents a considerable challenge. Dynamic covalent nanoparticles are emerging as an attractive category of reaction-enabled solution-processable nanosized building block through which the rational principles of molecular synthetic chemistry can be extended into the nanoscale. From a mixture of two hydrazone-based dynamic covalent nanoparticles with complementary reactivity, specific molecular instructions trigger selective assembly of intimately mixed heteromaterial (Au–Pd) aggregates or materials highly enriched in either one of the two core materials. In much the same way as complementary reactivity is exploited in synthetic molecular chemistry, chemospecific nanoparticle-bound reactions dictate building block connectivity; meanwhile, kinetic regioselectivity on the nanoscale regulates the detailed composition of the materials produced. Selectivity, and hence aggregate composition, is sensitive to several system parameters. By characterizing the nanoparticle-bound reactions in isolation, kinetic models of the multiscale assembly network can be constructed. Despite ignoring heterogeneous physical processes such as aggregation and precipitation, these simple kinetic models successfully link the underlying molecular events with the nanoscale assembly outcome, guiding rational optimization to maximize selectivity for each of the three assembly pathways. With such predictive construction strategies, we can anticipate that reaction-enabled nanoparticles can become fully incorporated in the lexicon of synthetic chemistry, ultimately establishing a synthetic science that manipulates molecular and nanoscale components with equal proficiency.

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Section: Introductionmentioning

confidence: 99%

Constitutionally Selective Dynamic Covalent Nanoparticle Assembly

et al. 2022

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“…Several approaches have been explored for linking nanoparticles through covalent or noncovalent interactions between surface-bound molecules, including a number that achieve responsive and reversible control over assembly state. [18][19][20][21][22][23][24] However, combining more than one type of nanoparticle component presents a further level of challenge, and selective coupling in multicomponent mixtures is rarely seen. The broad structural and compositional diversity now accessible for colloidal nanoparticles suggests vast potential for tuning composite material properties if multiple types of instructable nanoscale building block can be connected with high selectivity.…”

Section: Introductionmentioning

confidence: 99%

“…[30][31][32] A wider diversity of linker structures, chemical and environmental compatibility is potentially available in the form of abiotic assembly mediators. 12,24 Although many strategies can be applied to mixtures of building blocks, only a handful of pioneering examples have achieved any degree of programmable selectivity other than through rudimentary variation of building block feed ratio. Redox-switchable pseudorotaxane links between nanoparticle-bound guests and a multivalent polymeric linker have been exploited for the selective capture and release of either gold or silver nanoparticles from a binary mixture.…”

Section: Introductionmentioning

confidence: 99%

Constitutionally selective dynamic covalent nanoparticle assembly

Marro

Suo

Naden

et al. 2022

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The future of materials chemistry will be defined by our ability to precisely arrange components that have considerably larger dimensions and more complex compositions than conventional molecular or macromolecular building blocks. However, exerting structural and constitutional control in the assembly of nanoscale entities presents a considerable challenge. Dynamic covalent nanoparticles are emerging as an attractive category of reaction-enabled solution-processable nanosized building block through which the rational principles of molecular synthetic chemistry can be extended into the nanoscale. From a mixture of two hydrazone-based dynamic covalent nanoparticles with complementary reactivity, specific molecular instructions trigger selective assembly of intimately mixed heteromaterial (Au–Pd) aggregates or materials highly enriched in either one of the two core materials. In much the same way as complementary and orthogonal reactivity is exploited in synthetic molecular chemistry, chemospecific nanoparticle-bound reactions dictate building block connectivity, and kinetic regioselectivity regulates the detailed composition of the materials produced. Selectivity, and hence aggregate composition, is sensitive to several system parameters. By characterizing the nanoparticle-bound reactions in isolation, kinetic models of the multiscale assembly network can be constructed. Despite ignoring heterogeneous physical processes such as aggregation and precipitation, these simple kinetic models successfully link the underlying molecular events with the nanoscale assembly outcome, guiding rational optimization to maximize selectivity for each of three assembly pathways. With such predictive construction strategies, we can anticipate that reaction-enabled nanoparticles can become fully incorporated in the lexicon of synthetic chemistry, establishing a synthetic science that incorporates molecular and nanoscale components with equal proficiency.

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“…7,8 We assumed that the internal structure within Mg(OH) 2 gels would act as a template for ribbonshaped MgO nanoparticles hence being the opposite of MOG preparations that proceed by combining metal ions and organic ligands as aromatic acids or polymers. 9,10 Mg(OH) 2 gel was prepared from a procedure similar to the glycerol-urea route, 11,12 but exchanging urea for isopropanol, which forms a glycerol-isopropanol (GI) binary solvent. Thereby, dissolving magnesium nitrate Mg(NO 3 ) 2 Á6.H 2 O (12.8 g 0.05 mol) in 3 : 1 GI (30 mL) and further adding sodium hydroxide (4.0 g, 0.1 mol) aqueous solution (5 mL), a stiff gel comprising of Mg(OH) 2 particles was formed.…”

mentioning

confidence: 99%

“…7,8 We assumed that the internal structure within Mg(OH) 2 gels would act as a template for ribbon-shaped MgO nanoparticles hence being the opposite of MOG preparations that proceed by combining metal ions and organic ligands as aromatic acids or polymers. 9,10…”

mentioning

confidence: 99%