Despite its widespread use, the composition and structure of gamma-alumina
have been the subject of controversy for decades. In this article we review
the historical attempts to resolve two principal questions that have each
been extensively debated, but in independent communities: (1) What is the d
istribution of vacancies over the two cation sublattices in the nominal spi
nel structure, and (2) what is the hydrogen content of gamma-alumina, if an
y? We then review how recent investigations have shown that these two quest
ions are, in fact, related, and have a single resolution. The experimental
study of gamma-alumina surfaces has long been dominated by IR spectroscopy
of the hydroxylated surfaces, and Al-27 NMR. Both techniques have produced
perplexing results. Here we review the development of these surface studies
and parallel computational studies. Finally, we review recent computationa
l results that explain the puzzling experimental findings.