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Studies of electronic and magnetic structure and surface reactivity are reported for R2T14B compounds where R=Y, Nd, Gd, and T=Fe, Co. The calculations employed the self-consistent, spin-polarized linear-muffin-tin orbital method. Experiments included ultraviolet, x-ray, and Auger electron spectroscopy. Comparisons are made between the calculated and measured electronic densities of states, and the reactions of the surfaces with O2, H2, and CO gases are studied. The effects of heat treatment on surface segregation are also reported. Journal of Applied Physics is copyrighted by The American Institute of Physics.