Proton-conducting ceramics (PCCs) are of considerable interest for use in energy conversion and storage applications, electrochemical sensors, and separation membranes. PCCs that combine performance, efficiency, stability, and an ability to operate at low temperatures are particularly attractive. This review summarizes the recent progress made in the development of low-temperature protonconducting ceramics (LT-PCCs), which are defined as operating in the temperature range of 25-400°C. The structure of these ceramic materials, the characteristics of proton transport mechanisms, and the potential applications for LT-PCCs will be summarized with an emphasis on protonic conduction occurring at interfaces. Three temperature zones are defined in the LT-PCC operating regime based on the predominant proton transfer mechanism occurring in each zone. The variation in material properties, such as crystal structure, conductivity, microstructure, fabrication methods required to achieve the requisite grain size distribution, along with typical strategies pursued to enhance the proton conduction, is addressed. Finally, a perspective regarding applications of these materials to low-temperature solid oxide fuel cells, hydrogen separation membranes, and emerging areas in the nuclear industry including off-gas capture and isotopic separations is presented.
A substantial challenge worldwide is emergent drug resistance in malaria parasites against approved drugs, such as chloroquine (CQ). To address these unsolved CQ resistance issues, only rare examples of artemisinin (ART)‐based hybrids have been reported. Moreover, protein targets of such hybrids have not been identified yet, and the reason for the superior efficacy of these hybrids is still not known. Herein, we report the synthesis of novel ART–isoquinoline and ART–quinoline hybrids showing highly improved potencies against CQ‐resistant and multidrug‐resistant P. falciparum strains (EC50 (Dd2) down to 1.0 nm; EC50 (K1) down to 0.78 nm) compared to CQ (EC50 (Dd2)=165.3 nm; EC50 (K1)=302.8 nm) and strongly suppressing parasitemia in experimental malaria. These new compounds are easily accessible by step‐economic C−H activation and copper(I)‐catalyzed azide–alkyne cycloaddition (CuAAC) click reactions. Through chemical proteomics, putatively hybrid‐binding protein targets of the ART‐quinolines were successfully identified in addition to known targets of quinoline and artemisinin alone, suggesting that the hybrids act through multiple modes of action to overcome resistance.
Understanding the mechanisms of proton
conduction at the interface
of materials enables the development of a new generation of protonic
ceramic conductors at low temperatures (<150 °C) through water
absorption and proton transport on the surface and grain boundaries.
Conductivity measurements under Ar-3% H2O and Ar-3% D2O revealed a σ(H2O)/σ(D2O) ratio of approximately 2, indicating a hopping-based mechanism
for proton conduction at the interface. In situ Raman
spectroscopy was performed on water-saturated, porous, and nanostructured
TiO2 membranes to directly observe the isotope exchange
reactions over the temperature range of 25 to 175 °C. The behavior
of the isotope exchange reactions suggested a Grotthuss-type proton
transport and faster isotope exchange reactions at 175 °C than
that at 25 °C with a corresponding activation energy of 9 kJ
mol–1. The quantitative and mechanistic kinetic
description of the isotope exchange process via in situ Raman spectroscopy represents a significant advance toward understanding
proton transport mechanisms and aids in the development of high-performance
proton conductors with rapid surface exchange coefficients of importance
to contemporary energy conversion and storage material development.
In addition, new material systems are proposed, which combine interface
and bulk effects at low temperatures (<150 °C), resulting
in enhanced proton transport through interfacial engineering at the
nanoscale.
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