Identifying site-dependent reactivity in oxidation reactions on single Pt particles

Dery, Shahar; Kim, Suhong; Haddad, David; Cossaro, Albano; Verdini, Alberto; Toste, F. Dean; Gross, Elad

doi:10.1039/c8sc01956h

Cited by 37 publications

(55 citation statements)

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“…The strong NHC-metal interaction enabled the formation of stable self-assembled monolayers (SAMs) of NHCs on metals [3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19][20][21] , metal-oxides 22,23 and semimetals 24 . The wide chemical-tunability of NHCs led to utilization of NHC-based SAMs as biosensors 10,25,26 , molecular probes for surface reactivity [27][28][29] , and co-catalysts 3,[30][31][32][33] .…”

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confidence: 99%

“…For example, aromatic organic layers were formed on conductive or semiconductive surfaces following electrochemical reduction of aryl diazonium salts 39,40 . However, utilization of the electrochemical deposition approach toward surface anchoring of NHCs was not previously demonstrated, Herein, 1,3-bis(2,4-dinitrophenyl)-imidazole (NO 2 -NHC) 16,17,27 was used as a model system for addressable carbenes and was ECdeposited on various metal surfaces. Quantitative analysis revealed that EC deposition induced monolayer formation of NO 2 -NHCs on Au films with higher surface density and improved chemical stability than those prepared by base-induced deprotonation.…”

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confidence: 99%

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Electrochemical deposition of N-heterocyclic carbene monolayers on metal surfaces

Amit

Dery

et al. 2020

Nat Commun

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N-heterocyclic carbenes (NHCs) have been widely utilized for the formation of self-assembled monolayers (SAMs) on various surfaces. The main methodologies for preparation of NHCs-based SAMs either requires inert atmosphere and strong base for deprotonation of imidazolium precursors or the use of specifically-synthesized precursors such as NHC(H)[HCO3] salts or NHC–CO2 adducts. Herein, we demonstrate an electrochemical approach for surface-anchoring of NHCs which overcomes the need for dry environment, addition of exogenous strong base or restricting synthetic steps. In the electrochemical deposition, water reduction reaction is used to generate high concentration of hydroxide ions in proximity to a metal electrode. Imidazolium cations were deprotonated by hydroxide ions, leading to carbenes formation that self-assembled on the electrode’s surface. SAMs of NO2-functionalized NHCs and dimethyl-benzimidazole were electrochemically deposited on Au films. SAMs of NHCs were also electrochemically deposited on Pt, Pd and Ag films, demonstrating the wide metal scope of this deposition technique.

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confidence: 99%

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confidence: 99%

Electrochemical deposition of N-heterocyclic carbene monolayers on metal surfaces

Amit

Dery

et al. 2020

Nat Commun

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“…[1][2][3] The strong NHC-metal interaction enabled the formation of stable and chemically-addressable self-assembled monolayers (SAMs) of NHCs on metals, [4][5][6][7][8][9][10][11][12][13][14][15][16] metal-oxides 17,18 and semimetals. 19 The wide chemical-tunability of NHCs led to utilization of NHC-based SAMs as biosensors, [20][21][22] molecular probes for surface reactivity [23][24][25] and co-catalysts. 2,[26][27][28][29] NHC-based SAMs have been prepared thus far by two deposition techniques; namely liquid-and vapor-phase deposition (Scheme 1a and 1b, respectively).…”

Section: Introductionmentioning

confidence: 99%

“…In this work, nitro-functionalized NHCs (NO 2 -NHCs) 10, 11,23 were utilized as a model system for addressable carbenes and were EC-deposited on Au surfaces. The ECdeposition leads to high spatial and temporal proximity between the deprotonation and surface-anchoring of NHCs, while sustaining a small and constant concentration of active carbenes in the solution.…”

Section: Introductionmentioning

confidence: 99%

Electrochemical Deposition of Addressable N-Heterocyclic Carbene Monolayers

Amit¹,

Dery²,

Kim³

et al. 2020

Preprint

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<div>Herein, we introduce an electrochemical based approach for surface-anchoring of N-heterocyclic carbene (NHC) monolayers. The deposition process is based on in-situ formation of hydroxide ions by water reduction under negative potential. The hydroxide ions function as a base for deprotonation of the imidazole cations for the formation of active carbenes that self-assemble on the electrode's surface. Therefore, the electrochemical deposition does not require dry conditions or the addition of external base for carbene activation. The high temporal and spatial proximity between the NHC's activation and surface anchoring enabled the formation of well-ordered monolayers of NHCs on Au surfaces with higher density and stability than those achieved using liquid-phase deposition.</div>

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“…Destaca-se que, embora o potencial de SINS já esteja sendo demonstrado em diversos campos do conhecimento, 9,[27][28][29][30] tal técnica ainda não está sendo usada de forma sistemática na investigação de bens culturais, ao contrário de µ-FTIR com radiação sincrotron. 31,32 Atualmente, além do Laboratório Nacional de Luz Síncrotron (LNLS), apenas 2 laboratórios no mundo realizam o experimento SINS de forma aberta à comunidade.…”

Section: Introductionunclassified

Nanoespectroscopia De Absorção De Radiação Síncrotron No Infravermelho Para Nanoespeciação De Produtos De Corrosão Metálica

et al. 2019

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SYNCHROTRON INFRARED NANO-SPECTROSCOPY FOR NANO-SPECIATION OF METAL CORROSION PRODUCTS. The understanding of chemical and physical behavior of materials, especially metals and their alloys, is of utmost importance for industrial and technological applications, development of new materials and preservation of cultural heritage. The use of complementary analytical techniques has allowed a better understanding of corrosion mechanisms, and results obtained by Raman micro-spectroscopy, for example, have been complemented by FTIR and XRD. When focusing on the development of new materials and proposition of preservation strategies, the understanding of corrosion processes and of their very initial steps (nanometric scale) is fundamental. SERS reaches such lateral resolution if TERS is used, however, it cannot be universally applied and needs to be complemented by other techniques. In this work it is presented the potentials of a recent installed technique at the Brazilian Synchrotron Light Laboratory (LNLS), which can be used for nano-speciation of corrosion products, complementing investigation carried out by, for example, Raman micro-spectroscopy and TERS. It is Synchrotron Infrared Nano-Spectroscopy (SINS), which allows the investigation of both chemical nature and physical distribution of corrosion products. The infrastructure presented at LNLS is one of the few available in the world. As a model system, thin films of Pb exposed to formic acid were used.

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Identifying site-dependent reactivity in oxidation reactions on single Pt particles

Abstract: IR nanospectroscopy measurements revealed the influence of oxidizing reaction conditions on the reactivity of different surface sites on Pt particles.

Cited by 37 publications

References 54 publications

Electrochemical deposition of N-heterocyclic carbene monolayers on metal surfaces

Electrochemical deposition of N-heterocyclic carbene monolayers on metal surfaces

Electrochemical Deposition of Addressable N-Heterocyclic Carbene Monolayers

Nanoespectroscopia De Absorção De Radiação Síncrotron No Infravermelho Para Nanoespeciação De Produtos De Corrosão Metálica

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