Micro-mesoporous　P-doped　γ-Al2O3　with　cluster　morphology　was　obtained　via　an　efficient　ultrasound-assisted　sol-gel　process　and　taken　as　carrier　to　construct　palladium　catalysts　for　methane　oxidation.　It　was　revealed　that　the　structure　and　properties　of　catalysts　were　significantly　influenced　by　the　phosphorus　precursors　with　diverse　valence　and　acidity.　Dissimilar　reducibility　of　surface　hydroxyl　and　oxygen　species　is　observed　in　the　catalysts　derived　from　different　phosphorus　sources,　indicating　the　difference　in　the　oxygen　mobility　and　the　capacity　of　the　catalysts　to　convert　intermediate　CO.　The　behavior　of　charge-transfer　transition　and　d-d　transition,　the　transfer　ability　of　electrons　from　palladium　particles　into　the　antibonding　2π*　orbitals　of　CO,　together　with　the　surface　acidity　and　electronic　density　of　palladium　species　was　likewise　tailored,　which　demonstrated　the　metal-support　interaction　could　be　tuned,　making　palladium　species　behave　with　diverse　status　and　electronic　structures.　The　optimized　properties　cooperatively　provided　an　enhancement　in　catalytic　performance　of　P-containing　catalysts.　©　2019　Hydrogen　Energy　Publications　LLC