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Reactivity mapping with 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.

SUBMITTER: Krabbenborg SO

PROVIDER: S-EPMC3644076 | biostudies-literature | 2013

REPOSITORIES: biostudies-literature

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

Krabbenborg Sven O SO Nicosia Carlo C Chen Pengkun P Huskens Jurriaan J

Nature communications 20130101

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 react ...[more]

PMID: 23575671

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Project description:BackgroundSensorimotor communication is frequently observed in complex joint actions and social interactions. However, it remains challenging to explore the cognitive foundations behind sensorimotor communication.MethodsThe present study extends previous research by introducing a single-person baseline condition and formulates two distinct categories of asymmetric joint action tasks: distance tasks and orientation tasks. This research investigates the action performance of 65 participants under various experimental conditions utilizing a 2 (cooperative intention: Coop, No-coop) × 2 (task characteristic: distance, orientation) × 4 (target: T1, T2, T3, T4) repeated-measures experimental design to investigate the cognitive mechanisms underlying sensorimotor communication between individuals.ResultsThe results showed that (1) target key dwell time, motion time, total motion time, and maximum motion height in the Coop condition are more than in the No-coop condition. (2) In the distance task without cooperative intention, the dwell time of T4 is smaller than T1, T2, T3, and its variability of T1, T2, T3, and T4 were no different. In the distance task with cooperative intention, the dwell time and its variability of T1, T2, T3, and T4 displayed an increasing trend. (3) In the orientation task without cooperative intention, the dwell time of T1 is smaller than T2, T3, T4, and variability of the target keys T1, T2, T3, and T4 had no difference. In the orientation task with cooperative intention, the dwell time and variability of the target keys T1, T2, T3, and T4 had increasing trends.ConclusionsThose findings underscore the importance of cooperative intention for sensorimotor communication. In the distance task with cooperative intention, message senders establish a mapping relationship characterized by "near-small, far-large" between the task distance and the individual's action characteristics through sensorimotor experience. In the orientation task with cooperative intention, message senders combined sensorimotor experience and verbal metaphors to establish a mapping relationship between task orientation and action characteristics, following the sequence of "left-up, right-up, left-down, right-down" to transmit the message to others.

Project description:OBJECTIVE:Cerebrovascular reactivity (CR) is a mechanism that maintains stable blood flow supply to the brain. Pressure reactivity index (PRx), the correlation coefficient between slow waves of invasive arterial blood pressure (ABP) and intracranial pressure (ICP) has been validated for CR assessment. However, in clinical ward, not every subarachnoid hemorrhage (SAH) patient has invasive ABP monitoring. Pulse transit time (PTT), the propagation time of a pulse wave travelling from the heart to peripheral arteries, has been suggested as a surrogate measure of ABP. In this study, we proposed to use PTT instead of invasive ABP to monitor CR. APPROACH:Forty-five SAH patients with simultaneous recordings of invasive ABP, ICP, oxygen saturation level (SpO2) and electrocardiograph (ECG) were included. PTT was calculated as the time from the ECG R-wave peak to the onset of SpO2. PTT based pressure reactivity index (tPRx) was calculated as the correlation coefficient between slow waves of PTT and ICP. Wavelet tPRx (wtRx) was calculated as the cosine of wavelet phase shift between PTT and ICP. Meanwhile, PRx and wPRx were also calculated using invasive ABP and ICP as input. MAIN RESULTS:The result showed a negative relationship between PTT and ABP (r??=??-0.58, p???<??0.001). tPRx negatively correlated with PRx (r??=??-0.51, p???=??0.003). Wavelet method correlated well with correlation method demonstrated through positive relationship between wPRx and PRx (r??=??0.82, p???<??0.001) as well as wtPRx and tPRx (r??=??0.84, p???<??0.001). SIGNIFICANCE:PTT demonstrates great potential as a useful tool for CR assessment when invasive ABP is unavailable. Key points • Pulse transit time (PTT), defined as the propagation time of a pulse wave travelling from the heart to the peripheral arteries, has been proposed as a surrogate measure of ABP. The relationship between PTT and ABP in SAH patients remains unknown. • Cerebrovascular reactivity (CR) assessment through PTT has advantages over invasive ABP, as it avoids bleeding and infection risk, and can be used outside of the ICU. • We introduced a new method to assess CR using PTT and ICP through correlation based method and wavelet based method. • We found that beat-to-beat PTT was negatively related with invasive ABP in SAH patients. A significant linear relationship exists between PTT-based CR parameter and a well validated method, PRx. PTT demonstrates great potential as a useful tool for CR assessment when invasive ABP is unavailable in SAH patients.

Dataset Information

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

Publications

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

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