Reactivity mapping: electrochemical gradients for monitoring reactivity at surfaces in space and time

Sven Krabbenborg, Carlo Nicosia, P. Chen, Jurriaan Huskens

Research output: Contribution to journalArticleAcademicpeer-review

25 Citations (Scopus)
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Abstract

Studying and controlling reactions at surfaces is of great fundamental and applied interest in, among others, biology, electronics and catalysis. Because reaction kinetics is different at surfaces compared with solution, frequently, solution-characterization techniques cannot be used. Here we report solution gradients, prepared by electrochemical means, for controlling and monitoring reactivity at surfaces in space and time. As a proof of principle, electrochemically derived gradients of a reaction parameter (pH) and of a catalyst (Cu(I)) have been employed to make surface gradients on the micron scale and to study the kinetics of the (surface-confined) imine hydrolysis and the copper(I)-catalysed azide-alkyne 1,3-dipolar cycloaddition, respectively. For both systems, the kinetic data were spatially visualized in a two-dimensional reactivity map. In the case of the copper(I)-catalysed azide-alkyne 1,3-dipolar cycloaddition, the reaction order (2) was deduced from it.
Original languageEnglish
Article number1667
Pages (from-to)1-7
Number of pages7
JournalNature communications
Volume4
Issue number1667
DOIs
Publication statusPublished - 2013

Fingerprint

Alkynes
Azides
reactivity
Cycloaddition Reaction
gradients
Monitoring
Copper
Cycloaddition
cycloaddition
alkynes
Imines
Catalysis
Information Systems
Hydrolysis
copper
Kinetics
kinetics
biology
Reaction kinetics
imines

Keywords

  • METIS-301574
  • IR-90124

Cite this

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title = "Reactivity mapping: electrochemical gradients for monitoring reactivity at surfaces in space and time",
abstract = "Studying and controlling reactions at surfaces is of great fundamental and applied interest in, among others, biology, electronics and catalysis. Because reaction kinetics is different at surfaces compared with solution, frequently, solution-characterization techniques cannot be used. Here we report solution gradients, prepared by electrochemical means, for controlling and monitoring reactivity at surfaces in space and time. As a proof of principle, electrochemically derived gradients of a reaction parameter (pH) and of a catalyst (Cu(I)) have been employed to make surface gradients on the micron scale and to study the kinetics of the (surface-confined) imine hydrolysis and the copper(I)-catalysed azide-alkyne 1,3-dipolar cycloaddition, respectively. For both systems, the kinetic data were spatially visualized in a two-dimensional reactivity map. In the case of the copper(I)-catalysed azide-alkyne 1,3-dipolar cycloaddition, the reaction order (2) was deduced from it.",
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Reactivity mapping: electrochemical gradients for monitoring reactivity at surfaces in space and time. / Krabbenborg, Sven; Nicosia, Carlo; Chen, P.; Huskens, Jurriaan.

In: Nature communications, Vol. 4, No. 1667, 1667, 2013, p. 1-7.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Reactivity mapping: electrochemical gradients for monitoring reactivity at surfaces in space and time

AU - Krabbenborg, Sven

AU - Nicosia, Carlo

AU - Chen, P.

AU - Huskens, Jurriaan

N1 - Open access

PY - 2013

Y1 - 2013

N2 - Studying and controlling reactions at surfaces is of great fundamental and applied interest in, among others, biology, electronics and catalysis. Because reaction kinetics is different at surfaces compared with solution, frequently, solution-characterization techniques cannot be used. Here we report solution gradients, prepared by electrochemical means, for controlling and monitoring reactivity at surfaces in space and time. As a proof of principle, electrochemically derived gradients of a reaction parameter (pH) and of a catalyst (Cu(I)) have been employed to make surface gradients on the micron scale and to study the kinetics of the (surface-confined) imine hydrolysis and the copper(I)-catalysed azide-alkyne 1,3-dipolar cycloaddition, respectively. For both systems, the kinetic data were spatially visualized in a two-dimensional reactivity map. In the case of the copper(I)-catalysed azide-alkyne 1,3-dipolar cycloaddition, the reaction order (2) was deduced from it.

AB - Studying and controlling reactions at surfaces is of great fundamental and applied interest in, among others, biology, electronics and catalysis. Because reaction kinetics is different at surfaces compared with solution, frequently, solution-characterization techniques cannot be used. Here we report solution gradients, prepared by electrochemical means, for controlling and monitoring reactivity at surfaces in space and time. As a proof of principle, electrochemically derived gradients of a reaction parameter (pH) and of a catalyst (Cu(I)) have been employed to make surface gradients on the micron scale and to study the kinetics of the (surface-confined) imine hydrolysis and the copper(I)-catalysed azide-alkyne 1,3-dipolar cycloaddition, respectively. For both systems, the kinetic data were spatially visualized in a two-dimensional reactivity map. In the case of the copper(I)-catalysed azide-alkyne 1,3-dipolar cycloaddition, the reaction order (2) was deduced from it.

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