"Of laird and tenant": a study of the social and economic geography of Shetland in the eighteenth and early nineteenth centuries, based on the Garth and Gardie estate manuscripts

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Sustainably funding a marginal welfare programme - Why does English social care for older people face a persistent funding crisis?

English social care for older people faces a funding crisis. After more than two decades of growth, public spending on residential and home care fell in the years of financial austerity that followed the Great Recession, leaving almost half a million fewer older people eligible for publicly funded care and support. Social care is a non-core welfare programme financed by a secondary area of the English state that has suffered significant reductions in spending over the past decade. Policymakers recognise that social care has a structural funding problem, and there is a broad consensus that an alternative sustainable funding approach is needed to deliver more appropriate and equitable levels of social care provision, but policymakers have consistently failed to reform how social care is funded. This thesis argues that two very different institutional poles have emerged in England that deliver sustainable welfare programme funding: legacy positive state institutions that joined the welfare state core in the golden age of welfare, and more recent non-core welfare institutions where policymakers have engineered devolved, non-taxation funding approaches. Public social care is a significant, mature and complex welfare institution that is supported by neither. Moving English social care towards the positive welfare state core has proved to be technically and politically unworkable, and less than fully engaged policymakers have been unable to agree on a bespoke, programme-specific funding solution designed to deliver greater sustainability. Elsewhere, it has been possible to enact successful sustainable funding reform in marginal policy areas, when policymakers have looked in the policy garbage can and found that an established, pre-existing institutional answer to the funding problem already exists, allowing the politics of organisational change to follow the structure. While English policymakers might express a desire for change, the existing funding approach has been undermined by a decade of austerity, and history has not left social care a clear route to an alternative de-centred funding solution

Ruthenium-catalyzed asymmetric reduction of isoxazolium salts : access to optically active Δ4-isoxazolines

A tethered MsDPEN–ruthenium catalyst reduces a series of isoxazolium salts, affording optically active Δ4-isoxazolines in moderate to good yields and enantioenrichment. The redundancy of heating or high pressures allowed for chemoselective reduction with no subsequent heterocyclic ring opening. Our results reinforce our understanding of the workings of these Noyori-class catalysts

Exploitation of differential electronic densities for the stereoselective reduction of ketones bearing a masked amino surrogate

A tethered ruthenium-TsDPEN catalyst is employed for the facile catalytic asymmetric reduction of α-phthalimyl-α′-ketoethers under mild conditions. Leveraging exclusively on the contrasting electronic densities on the heteroatoms, a series of enantioenriched phthalimyl ether alcohols can be obtained in generally good stereoselectivities from this challenging class of substrate. Subsequent transformation into highly valuable chiral β-amino alcohols is demonstrated to take place without significant losses in yield and optical purity

Applications of N′-monofunctionalised TsDPEN derivatives in asymmetric catalysis

This review contains an account of recent developments in the applications of N′-monoalkylated or N′-mono(thio)acylated(N-sulfonyl)-1,2-diphenylethylene-1,2-diamine (TsDPEN) derivatives to asymmetric catalysis. The coverage features examples of applications of derivatives as ligands in organometallic complexes for use in asymmetric reduction and oxidation reactions. The use of TsDPEN derivatives as catalysts in a diverse range of C–C and C–S bond formation reactions is also described in detail

Probing the effects of heterocyclic functionality in [(Benzene) Ru(TsDPENR) Cl] catalysts for asymmetric transfer hydrogenation

A range of TsDPEN catalysts containing heterocyclic groups on the amine nitrogen atom were prepared and evaluated in the asymmetric transfer hydrogenation of ketones. Bidentate and tridentate ligands demonstrated a mutual exclusivity directly related to their function as catalysts. A broad series of ketones were reduced with these new catalysts, permitting the ready identification of an optimal catalyst for each substrate and revealing the subtle effects that changes to nearby donor groups can exhibit

The evolution of the tetrapod humerus: morphometrics, disparity, and evolutionary rates

The present study explores the macroevolutionary dynamics of shape changes in the humeri of all major grades and clades of early tetrapods and their fish-like forerunners. Coordinate point eigenshape analysis applied to humeral outlines in extensor view reveals that fish humeri are more disparate than those of most early tetrapod groups and significantly separate from the latter. Our findings indicate sustained changes in humeral shape in the deepest portions of the tetrapod stem group and certain portions of the crown. In the first half of sampled tetrapod history, subclades show larger than expected humeral disparity, suggesting rapid diffusion into morphospace. Later in tetrapod evolution, subclades occupy smaller and non-overlapping morphospace regions. This pattern may reflect in part increasing specialisations in later tetrapod lineages. Bayesian shifts in rates of evolutionary change are distributed discontinuously across the phylogeny, and most of them occur within rather than between major groups. Most shifts with the highest Bayesian posterior probabilities are observed in lepospondyls. Similarly, maximum likelihood analyses of shifts support marked rate accelerations in lepospondyls and in various subclades within that group. In other tetrapod groups, rates either tend to slow down or experience only small increases. Somewhat surprisingly, no shifts are concurrent with structural, functional, or ecological innovations in tetrapod evolution, including the origin of digits, the water-land transition and increasing terrestrialisation. Although counterintuitive, these results are consistent with a model of continual phenotypic innovation that, although decoupled from key evolutionary changes, is possibly triggered by niche segregation in divergent clades and grades of early tetrapods.</p

Of Laird and Tenant

A study of the social and economic geography of Shetland in the eighteenth and early nineteenth centuries, based on the Garth and Gardie estate manuscripts. The thesis is based upon a major and hitherto almost unresearched historical manuscript source, the Gardie Papers; it assesses their usefulness to the historian and the historical geographer, compares the evidence from this source with that from the extensive published literature on the Shetland Islands, and analyses data from Gardie that is not available from other sources. The first (historical) part of the work (chapters 1, 2 and 3) discusses the Garth and Gardie estates in the general context of seventeenth and eighteenth century Shetland, and the role of the Mouat family in the social, economic and political affairs of the time. The second (thematic) half (chapters 4, 5 and 6) is based on statistical analyses of data from Gardie and elsewhere; it covers a range of topics under the broad headings of 'The Estate and its Produce', 'The Tenants and the Land' and 'Problems of Demography and Labour Supply'