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Confining NaAlH4 in nanoporous carbon scaffolds is known to alter the sorption kinetics and/or pathways of the characteristic bulk hydride reactions through interaction with the framework at the interface, increased specific surface area of the resulting nanoparticles, decreased hydrogen diffusion distances, and prevention of phase segregation. Although the nanosize effects have been well studied, the influence of the carbon scaffold surface chemistry remains unclear. Here we compare the hydrogen sorption characteristics of NaAlH4 confined by melt infiltration in nitrogen-doped/undoped ordered nanoporous carbon of two different geometries. 23Na and 27Al MAS NMR, N2 sorption, and PXRD verify NaAlH4 was successfully confined and remains intact in the carbon nanopores after infiltration. Both the N-doped/undoped nanoconfined systems demonstrate improved reversibility in relation to the bulk hydride during hydrogen desorption/absorption cycling. Isothermal kinetic measurements indicate a lowering of the activ...

Complex metal hydrides are an attractive hydrogen storage option due to their high gravimetric hydrogen capacities, but the re/dehydriding reactions generally possess unfavorable thermodynamics and kinetics. Recent studies have attempted to alter these properties through confinement of complex hydrides in nanoporous substrates. For example, LiBH4 may be melt-infiltrated into a nanoporous carbon (LiBH4@NPC), where electron-withdrawing boron concomitantly incorporates into the substrate, facilitating the wetting of the pores with molten LiBH4. We present results of the surface functionality displayed by incorporation of electron-donating nitrogen into a nanoporous carbon. The presence of pyridinic nitrogen in the substrate, confirmed by XPS analysis, acts as a Lewis base. Our results indicate partial decomposition on melt-infiltration of LiBH4 may produce electron-accepting BH3 defects at the surface of the hydride forming a stabilizing capping layer. Isothermal hydrogen desorption measurements indicate an ...

We present first-principles solubility calculations of H–/[OH]− mixing in binary alkali metal hydrides MH and their corresponding hydroxides MOH, for M ={Li, Na, K, Rb, Cs}. Solid solubility in the...

The development and implementation of a scalable process for the manufacture of the Toll-like receptor (TLR7) agonist PF-4171455 (1) is described. Initial routes used to synthesise 1 in milligram quantities were unsuitable for large-scale synthesis to provide bulk material. As part of the transfer between Medicinal Chemistry and Research-API, collaboration provided a fit for purpose route for the kilo-scale synthesis of 1. Key aspects of the synthesis included (i) a safe and practical synthesis of a key nitropyridone intermediate 7 over four steps, (ii) a sequential regioselective chlorination to selectively functionalise 7 and (iii) use of a carbamate as a tethered carbonyl group, allowing an efficient regiospecific synthesis of 1.

This paper reports the synthesis and biological activity of a novel series of aryl-morpholine dopamine receptor agonists. Several compounds show high levels of functional selectivity for the D3 over the D2 dopamine receptor. Compound 26 has >1000-fold functional selectivity and has been successfully progressed in vivo using an intranasal delivery route.

Motivations to engage in retail shopping include both utilitarian and hedonic dimensions. Business to consumer e-commerce conducted via the mechanism of web-shopping provides an expanded opportunity for companies to create a cognitively and esthetically rich shopping environment in ways not readily imitable in the nonelectronic shopping world. In this article an attitudinal model is developed and empirically tested integrating constructs from technology acceptance research and constructs derived from models of web behavior. Results of two studies from two distinct categories of the interactive shopping environment support the differential importance of immersive, hedonic aspects of the new media as well as the more traditional utilitarian motivations. In addition, navigation, convenience, and the substitutability of the electronic environment to personally examining products were found to be important predictors of online shopping attitudes. Results are discussed in terms of insights for the creation of the online shopping webmosphere through more effective design of interactive retail shopping environments.

Modifications to the sugar portion of C-aryl glycoside sodium glucose transporter 2 (SGLT2) inhibitors were explored, including systematic deletion and modification of each of the glycoside hydroxyl groups. Based on results showing activity to be quite tolerant of structural change at the C-5 position, a series of novel C-5 spiro analogues was prepared. Some of these analogues exhibit low nanomolar potency versus SGLT2 and promote urinary glucose excretion (UGE) in rats. However, due to sub-optimal pharmacokinetic parameters (in particular half-life), predicted human doses did not meet criteria for further advancement.

Synthesis of a number of bicyclic five-membered ring derivatives of gabapentin led to the identification of two compounds, (−)-(11A) and (20A) which both had an excellent level of potency against α2δ and were profiled in an in vivo model of neuropathic pain.