Dual Microenvironment Modulation of Pd Nanoparticles in Covalent Organic Frameworks for Semihydrogenation of Alkynes

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(26)

Published: May 2, 2023

The chemical microenvironment modulation of metal nanoparticles (NPs) holds promise for tackling the long-lasting challenge trade-off effect between activity and selectivity in catalysis. Herein, ultrafine PdCu2 NPs incorporated into covalent organic frameworks (COFs) with diverse groups on their pore walls have been fabricated semihydrogenation alkynes. Cu species, as primary Pd active sites, greatly improves selectivity. functional secondary around effectively regulate activity, which encapsulated COF bearing -CH3 exhibit highest >99 % conversion 97 Both experimental calculation results suggest that group affects electron-donating ability COFs, successively impacts charge transfer COFs giving rise to a modulated electronic state excellent catalytic performance.

Language: Английский

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Surface functionalization of inorganic nanoparticles with ligands: a necessary step for their utility

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(8), P. 2573 - 2595

Published: Jan. 1, 2023

The importance of organic ligands in protecting inorganic nanoparticles and thus imparting the needed stabilization as colloidal dispersions was realised many years ago. Currently, rational preparation such with designed molecules/ligands resulting formation functional (FNPs) that are tuned for a specific application is an area immense research interest. FNPs desired requires clear understanding interactions at nanoparticle (NP)-ligand ligand-solvent interfaces, demands deep appreciation surface science coordination chemistry. In this tutorial review, we briefly explore evolution surface-ligand chemistry inform readers that, apart from surface, can modulate physico-chemical properties underlying NPs well. This review further presents design principles FNPs, where one or more ligand shells be added to thereby improving adaptability amenability NP exterior towards environment which they present, required application.

Language: Английский

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A Review of Bimetallic and Monometallic Nanoparticle Synthesis via Laser Ablation in Liquid

Crystals, Journal Year: 2023, Volume and Issue: 13(2), P. 253 - 253

Published: Feb. 1, 2023

Pulsed laser ablation in liquid (PLAL) is a physical and top-down approach used to fabricate nanoparticles (NPs). Herein, the research methods current trends PLAL literature are reviewed, including recent uses of for fabricating bimetallic (BNPs) composites. BNPs have gained attention owing their advanced physicochemical properties over monometallic NPs. involves irradiation solid target (usually rod, plate, or thin film) under medium. The collects ejected NPs resulting from processing, which produces colloid that can be various applications, plasmon sensing, energy harvesting, drug delivery. most fabrication techniques, use microorganisms, do not precise NP size control require separation microorganisms produced quicker at producing than bottom-up methods. drawbacks include need find required processing parameters, requires extensive experimentation, complex non-linear relationships between inputs outputs (e.g., size).

Language: Английский

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SERS as a Probe of Surface Chemistry Enabled by Surface-Accessible Plasmonic Nanomaterials

Accounts of Chemical Research, Journal Year: 2023, Volume and Issue: 56(15), P. 2072 - 2083

Published: July 12, 2023

ConspectusWhen the size of materials is reduced, their volume decreases much faster than surface area, which in most extreme case leads to 2D nanomaterials are "all surface". Since atoms at have free energies, electronic states, and mobility very different from bulk atoms, that large surface-to-volume ratios can display remarkable new properties compared counterparts. More generally, where interact with environment, turn places chemistry heart catalysis, nanotechnology, sensing applications. Understanding utilizing nanosurfaces not possible without appropriate spectroscopic microscopic characterization techniques. An emerging technique this area surface-enhanced Raman spectroscopy (SERS), utilizes interaction between plasmonic nanoparticles light enhance signals molecules near nanoparticles' surfaces. SERS has great advantage it provide detailed situ information on orientation binding nanosurface. A long-standing dilemma limited applications studies choice surface-accessibility activity. specifically, synthesis metal strong SERS-enhancing typically involves use strongly adsorbing modifier molecules, but these modifiers also passivate product material, prevents general application analysis weaker molecule-metal interactions.In Account, we discuss our efforts development modifier-free synthetic approaches synthesize surface-accessible, for SERS. We start by discussing definition "modifiers" "surface-accessibility", especially context As a rule thumb, chemical ligands surface-accessible should be easily displaceable wide range target relevant potential then introduce bottom-up colloidal nanoparticles, basic building blocks nanotechnology. Following this, interfacial self-assembly developed group allow creation multidimensional nanoparticle arrays types nanoparticle-building blocks. These further combined functional form multifunctional hybrid materials. Finally, demonstrate as substrates chemistry. Importantly, revealed removal led only significantly enhanced observation phenomena had been previously overlooked or misunderstood literature. Realizing current limitations modifier-based provides perspectives manipulating interactions nanotechnology significant implications design next generation nanomaterials.

Language: Английский

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Surfactant-Free Colloidal Syntheses of Precious Metal Nanoparticles for Improved Catalysts

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(7), P. 4903 - 4937

Published: March 27, 2023

Colloidal syntheses of nanomaterials offer multiple benefits to study, understand, and optimize unsupported supported catalysts. In particular, colloidal are relevant the synthesis (precious) metal nanoparticles. By separating active phase, i.e., nanoparticles, from supporting steps, a deeper knowledge rational control properties catalysts is gained. The effect(s) size, shape, composition nanoparticle, nature support, or loading on support can be studied in more systematic ways. fundamental gained paves way for catalyst optimization by tuning activity, selectivity, stability. However, most require use additives surfactants, which detrimental catalytic reactions because they typically block sites. Surfactant removal therefore often required, adds complexity analysis obtained results. Developing surfactant-free strategies obtain stable nanoparticles rising field research that here reviewed. A focus given laser processing colloids-, solution plasma process-, N,N-dimethylformamide-, polyol-, recently reported monoalcohol-based syntheses. relevance these synthetic approaches catalysis detailed with heterogeneous electrocatalysis.

Language: Английский

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Nanometre-resolved observation of electrochemical microenvironment formation at the nanoparticle–ligand interface

Nature Catalysis, Journal Year: 2024, Volume and Issue: 7(4), P. 422 - 431

Published: March 25, 2024

Language: Английский

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Nanoparticle proximity controls selectivity in benzaldehyde hydrogenation

Nature Catalysis, Journal Year: 2024, Volume and Issue: 7(2), P. 172 - 184

Published: Feb. 16, 2024

Language: Английский

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Mechanically driven water splitting over piezoelectric nanomaterials

Chem Catalysis, Journal Year: 2024, Volume and Issue: 4(2), P. 100901 - 100901

Published: Jan. 26, 2024

Language: Английский

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Ultra-stable and highly reactive colloidal gold nanoparticle catalysts protected using multi-dentate metal oxide nanoclusters

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Feb. 6, 2024

Abstract Owing to their remarkable properties, gold nanoparticles are applied in diverse fields, including catalysis, electronics, energy conversion and sensors. However, for catalytic applications of colloidal nanoparticles, the trade-off between reactivity stability is a significant concern. Here we report universal approach preparing stable reactive small (~3 nm) by using multi-dentate polyoxometalates as protecting agents non-polar solvents. These exhibit exceptional even under conditions high concentration, long-term storage, heating addition bases. Moreover, they display excellent performance various oxidation reactions organic substrates molecular oxygen sole oxidant. Our findings highlight ability inorganic ligands with structural robust steric electronic effects confer upon nanoparticles. This can be extended prepare metal other than gold, enabling design novel nanomaterials promising applications.

Language: Английский

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Noble Metal‐Based Multimetallic Nanoparticles for Electrocatalytic Applications

Advanced Science, Journal Year: 2021, Volume and Issue: 9(1)

Published: Nov. 17, 2021

Noble metal-based multimetallic nanoparticles (NMMNs) have attracted great attention for their multifunctional and synergistic effects, which offer numerous catalytic applications. Combined experimental theoretical studies enabled formulation of various design principles tuning the electrocatalytic performance through controlling size, composition, morphology, crystal structure nanoparticles. Despite significant advancements in field, chemical synthesis NMMNs with ideal characteristics catalysis, including high activity, stability, product-selectivity, scalability is still challenging. This review provides an overview on structure-based classification general NMMN electrocatalysts. Furthermore, postsynthetic treatments, such as removal surfactants to optimize utilization onto suitable support practical applications are highlighted. In end, future direction challenges associated electrocatalysis covered.

Language: Английский

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