Characteristic examples of three types of change of form of p n relationships at 2 5 T , as the contents of elements alloying with palladium a r e gradually increased (4,37,70,74-83,95-98,~04,108,153,154), are illustrated in Figure 9. As for the palladiumhydrogen system itself (4), such relationships have been determined from direct equilibrations with hydrogen gas, as well as being derived from measurements of electrode potential. Similarly as for palladium-hydrogen, temperature dependences of the p n relationships have been used to supplement calorimetric data ( I 10) in deriving heats and cntropies of hydrogen absorption, both at initially low values (79)(80)(81)(82)95,100,108) of hydrogen content (n-to) and over (Y =p transition regionsThe sequence of relationships in Figure 9(c) (4,37,70,74-83,'04,I54,I78).shows gradual increases with increasing rhodium content in the range o f n over which (Y and / J ' phases coexist. This sequence now seems unique to the palladium-rhodium-hydrogen system (45,75, I 53,154), since some suggestions of similarities of the palladium-manganesehydrogen system (179) seem doubtful in view of possible incomplete equilibrations.'The remaining families of p n isotherms for palladium alloy-hydrogen systems would thus seem to be divisible into two groups represented by those in Figures 9(a) and 9 (b). In both cases the ranges of n over t i + p phase regions are successively shortened with increasing content of the alloying element, even in the cases of alloys with readily hydride-forming transition or inner transition elements such as vanadium Decreases, in the range of n over (r +/I regions, with increasing amounts of alloying elements, have continued to be deduced from X-ray determinations of and / 3 phase lattice constants for additional palladium alloyhydrogen systems (4,79-82,157, I 80-1 82).Apart from the probable case of the palladium-nickel-hydrogen system (so), these general trends of decreasing extents of ( Y , p coexistence with increasing contents of alloying element are similar to the effects of increasing temperature in the palladium-hydrogen system, being accompanied by decreases in the extents of hystereses of absorption and desorption relationships between hydrogen contents and other experimental parameters (4,69,(96)(97)(98) later, has importance in choices of alloy compositions as hydrogen permeation membranes. In addition to the arguments concerning the solubility of hydrogen in the palladium-silver alloys, the extents of decreases of hydrogen solubilities with increasing contents of other alloying metals have been used (95,104,108) in support of an essentially protonic nature of the hydrogen entities. However, in order to allow for proposed levels of electron donation it has seemed necessary to postulate adoptions of oxidation states by the alloying elements which can be difficult to reconcile with their relative positions in sequence of electronegaiivities.Moreover as for the palladium-hydrogen system, latterly there has been increasing emphasis on the account ...