This is the first comprehensive review on methods and materials for use in optical sensing of pH values and on applications of such sensors. The Review starts with an introduction that contains subsections on the definition of the pH value, a brief look back on optical methods for sensing of pH, on the effects of ionic strength on pH values and pKa values, on the selectivity, sensitivity, precision, dynamic ranges, and temperature dependence of such sensors. Commonly used optical sensing schemes are covered in a next main chapter, with subsections on methods based on absorptiometry, reflectometry, luminescence, refractive index, surface plasmon resonance, photonic crystals, turbidity, mechanical displacement, interferometry, and solvatochromism. This is followed by sections on absorptiometric and luminescent molecular probes for use pH in sensors. Further large sections cover polymeric hosts and supports, and methods for immobilization of indicator dyes. Further and more specific sections summarize the state of the art in materials with dual functionality (indicator and host), nanomaterials, sensors based on upconversion and 2-photon absorption, multiparameter sensors, imaging, and sensors for extreme pH values. A chapter on the many sensing formats has subsections on planar, fiber optic, evanescent wave, refractive index, surface plasmon resonance and holography based sensor designs, and on distributed sensing. Another section summarizes selected applications in areas, such as medicine, biology, oceanography, bioprocess monitoring, corrosion studies, on the use of pH sensors as transducers in biosensors and chemical sensors, and their integration into flow-injection analyzers, microfluidic devices, and lab-on-a-chip systems. An extra section is devoted to current challenges, with subsections on challenges of general nature and those of specific nature. A concluding section gives an outlook on potential future trends and perspectives.

Optical Sensing and Imaging of pH Values: Spectroscopies, Materials, and Applications

Alkaline anion-exchange membrane (AAEM) fuel cells have attracted significant interest in the past decade, thanks to the recent developments in hydroxide-anion conductive membranes. In this article, we compare the performance of current state of the art AAEM fuel cells to proton-exchange membrane (PEM) fuel cells and elucidate the sources of various overpotentials. While the continued development of highly conductive and thermally stable anion-exchange membranes is unambiguously a principal requirement, we attempt to put the focus on the challenges in electrocatalysis and interfacial charge transfer at an alkaline electrode/electrolyte interface. Specifically, a critical analysis presented here details the (i) fundamental causes for higher overpotential in hydrogen oxidation reaction, (ii) mechanistic aspects of oxygen reduction reaction, (iii) carbonate anion poisoning, (iv) unique challenges arising from the specific adsorption of alkaline ionomer cation-exchange head groups on electrocatalysts surfaces, and (v) the potential of alternative small molecule fuel oxidation. This review and analysis encompasses both the precious and nonprecious group metal based electrocatalysts from the perspective of various interfacial charge-transfer phenomena and reaction mechanisms. Finally, a research roadmap for further improvement in AAEM fuel cell performance is delineated here within the purview of electrocatalysis and interfacial charge transfer.

Alkaline Anion-Exchange Membrane Fuel Cells: Challenges in Electrocatalysis and Interfacial Charge Transfer.

Understanding the competition between hydrogen evolution and CO2 reduction is of fundamental importance to increase the faradaic efficiency for electrocatalytic CO2 reduction in aqueous electrolytes. Here, by using a copper rotating disc electrode, we find that the major hydrogen evolution pathway competing with CO2 reduction is water reduction, even in a relatively acidic electrolyte (pH 2.5). The mass-transport-limited reduction of protons takes place at potentials for which there is no significant competition with CO2 reduction. This selective inhibitory effect of CO2 on water reduction, as well as the difference in onset potential even after correction for local pH changes, highlights the importance of differentiating between water reduction and proton reduction pathways for hydrogen evolution. In-situ FTIR spectroscopy indicates that the adsorbed CO formed during CO2 reduction is the primary intermediate responsible for inhibiting the water reduction process, which may be one of the main mechanisms b...

/pdf/competition-between-hydrogen-evolution-and-carbon-dioxide-2bgbbcm31s.pdf

Competition between Hydrogen Evolution and Carbon Dioxide Reduction on Copper Electrodes in Mildly Acidic Media.

https://hal.archives-ouvertes.fr/hal-01366512/document

Update and challenges in organo-mediated polymerization reactions

The direct anti-Markovnikov addition of strong Bronsted acids to alkenes remains an unsolved problem in synthetic chemistry. Here, we report an efficient organic photoredox catalyst system for the addition of HCl, HF and also phosphoric and sulfonic acids to alkenes, with complete regioselectivity. These transformations were developed using a photoredox catalyst in conjunction with a redox-active hydrogen atom donor. The nucleophile counterion plays a critical role by ensuring high reactivity, with 2,6-lutidinium salts typically furnishing the best results. The nature of the redox-active hydrogen atom donor is also consequential, with 4-methoxythiophenol providing the best reactivity when 2,6-lutidinium salts are used. A novel acridinium sensitizer provides enhanced reactivity within several of the more challenging reaction manifolds. This Article demonstrates how nucleophilic addition reactions mediated by photoredox catalysis can change the way electrophilic and homofugal precursors are constructed.

The direct anti-Markovnikov addition of mineral acids to styrenes

Acidities of strong neutral Brønsted acids in different media

Careful analysis and comparison of the available acidity data of HCl, HBr, HI, HClO4, and CF3SO3H in water, dimethyl sulfoxide (DMSO), and gas-phase has been carried out. The data include experimental and computational pKa and gas-phase acidity data from the literature, as well as high-level computations using different approaches (including the W1 theory) carried out in this work. As a result of the analysis, for every acid in every medium, a recommended acidity value is presented. In some cases, the currently accepted pKa values were revised by more than 10 orders of magnitude.

Acidity of Strong Acids in Water and Dimethyl Sulfoxide

The structures and gas-phase acidities (GA) of several CB11H12H-based carborane acid derivatives (HA) have been calculated with DFT B3LYP method using 6-311+G**, 6-311++G** basis sets In order to verify the obtained GA values, several systems were also studied at G3(MP2) level of theory Inserted substituents (CF3, F, Cl, Br, I, CN, CH3, etc) followed the “belts” of the monocarborane cage starting from the boron antipodal to the carbon In general, the predicted intrinsic gas-phase acidities of the systems varied according to the substituents in the following order of decreasing strength: CF3 > F > Cl > Br > I > CN > CH3 Nevertheless, some inconsistencies occurred F and CN derivatives with lower degree of substitution had weaker intrinsic acidities than the respective Cl derivatives, but the situation was reversed in the case of a larger number of substituents To obtain better understanding how the substituents influence the basicity of the carborane anion, three hypothetical reaction series were inv

Gas-Phase Brønsted Superacidity of Some Derivatives of Monocarba-closo-Borates: a Computational Study

The structures and intrinsic gas-phase acidities (GA) of some dodecaborane acids, the derivatives of YB12H11H (Y = PF3, NH3, NF3, NMe3), B12H12H2, and B12H12H– (HA, H2A, and HA–, respectively) have been computationally explored with DFT B3LYP method at the 6-311+G** level of theory as new possible directions of creating superstrong Bronsted acids. Depending on the nature and number of the substituents different protonation geometries were investigated. In general, the GA values of the neutral systems varied according to the substituents in the following order: CF3 < F < Cl and in case of anionic acids: CF3 < Cl < F. The dodecatrifluoromethyl derivative of H2A, B12(CF3)12H1H2, emerges as the strongest among the considered acids and is expected to be in the gas phase at least as strong as the undecatrifluoromethyl carborane, CB11(CF3)11H1H. The GA values of the respective monoanionic forms of the considered acids all, but the (CF3)11 derivative, remained higher than the widely used threshold of superacidity...

Superacidity of closo-dodecaborate-based Brønsted acids: a DFT study.

The gas-phase acidities of ca. 60 monosubstituted anilines (with acidity span of almost 50 kcal mol–1) have been calculated using density functional theory (DFT) at the B3LYP/6-311+G** level. At th...

Acidity of anilines: calculations vs experiment.

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