A series of AlPO 4 -11 molecular sieves with Si content ranging from zero to 0.24 Si molar fraction were crystallized from reaction gels prepared using different sources of Al and Si. It was found that the lower the crystallinity of the starting alumina the higher its reactivity and the higher the crystallinity and purity of the resulting molecular sieves. Factors affecting the initial pH of the departing gel strongly influence both the crystallinity and purity of the resulting solid. Thus, starting from the same source of alumina, it can be observed that the higher the pH within the acid region the higher the crystallinity and purity of the product. There seems to be an upper limit for the amount of Si incorporated in the AlPO 4 -11 framework, above which isolated silica patches (silica domain) are formed and subsequently dislodged from the structure when calcination is carried out at 773 K, yielding α-quartz. At this limiting value the population of both Lewis and Br nsted acid sites passes through a maximum. Unreacted pseudoboehmite coexisting with SAPO-11, was transformed upon calcination at 773 K into γ-alumina. These species seem to act as Lewis centres which would interact with Br nsted sites to increase surface acidity.