RESUMEN
Two-dimensional (2D) metal chalcogenides provide rich ground for the development of nanoscale thermoelectrics, although achieving optimal thermoelectric efficiency is still a challenge. Here, we leverage the unique chemistry of tellurium (Te), renowned for its hypervalent bonding and catenation abilities, to tackle this challenge as manifested in Al2Te3 and Al2Te5 monolayers. While the former forms a straightforward covalent Al-Te network, the latter adopts a more intricate bonding mechanism, enabled by eccentric features of Te chemistry, to maintain charge balance. In Al2Te5, a square planar chain (SPC) known as polytelluride [Te3]2- is neutralized by the covalently bonded [Al2Te2]2+ framework. The hypervalent nature of Te results in bizarre Born effective charges of 7 and -4 for adjacent Te atoms within the square planar chain, a feature that induces significant anharmonicity in Al2Te5 monolayers. Enhanced anharmonic lattice vibrations and the accordion pattern bestow glass-like, strongly anisotropic thermal conductivity to the Al2Te5 monolayer. The calculated κL values of 1.8 and 0.5 W m-1 K-1 along the a- and b-axes at 600 K are one order of magnitude lower than those of Al2Te3, and even lower than monolayers that contain heavy cations like Bi2Te3. Moreover, the tellurium chain dominates the valence band maximum and conduction band minimum of Al2Te5, leading to a high valley degeneracy of 10, and thus a high power factor and figure of merit (zT). Using rigorous first-principles calculations of electron relaxation time, the estimated hole-doped and electron-doped zT of, respectively, 1.5 and 0.5 at 600 K is achieved for Al2Te5. The pioneering zT of Al2Te5 compared to that of Al2Te3 is rooted merely in its amorphous-like lattice thermal transport and its polytelluride chain. These findings underscore the importance of aluminum telluride and polymeric-based inorganic compounds as practical and cost-effective thermoelectric materials, pending further experimental validation.
RESUMEN
Activation of human carbonic anhydrase II (hCA II) holds great promise for treating memory loss symptoms associated with Alzheimer's disease. Despite its importance, the activation mechanism of hCA II has been largely overlooked in favor of the well-studied inhibition mechanism. To address this unexplored realm, we use first-principles calculations to tease out the activation mechanism of hCA II using 2-(2-aminoethyl)-pyridine (2-2AEPy), a promising in vitro activator. We explored both stepwise and concerted mechanisms via both available nitrogen sites of 2-2AEPy: (i) aminoethyl group (Nα) and (ii) pyridine ring (Nß). Our results show that a concerted mechanism via Nα holds the key to hCA II activation. The activation process of the concerted mechanism exhibits the characteristics of an exergonic reaction, wherein the transition state resembles the reactant with a notably low imaginary frequency of 452.4i cm-1 and barrier height of 5.2 kcal mol-1. Such meager transition barriers propel the activation of hCA II at in vivo temperatures. These findings initiate future research into hCA II activation mechanisms and the development of efficient activators, which may lead to promising therapeutic interventions for Alzheimer's disease.