Single crystal A1(110) was hydroxylated in UHV to give a disordered overlayer. Protolytically labile tetraneopentylzirconium did not react with hydroxylated A1(110) in UHV, which was interpreted through a mechanistic proposal for proton-transfer-based surface chemical modification. According to this proposal, a zirconium alkoxide, although less thermodynamically basic than a zirconium alkyl, could be a kinetically viable substrate for proton-transfer-based organometallic chemical vapor deposition (MOCVD) in UHV, and tetra-tert-butoxyzirconium did react with hydroxylated A1(110) to give a surface bound di-tert-butoxyzirconium species. The deposition reaction was readily studied by HREELS, XPS, and AES.