A　modified　zirconium　(Zr)-based　metal　organic　framework　(UiO-66-CTAB)　was　synthesized　by　solvothermal　method,　and　used　for　the　adsorption　and　separation　of　molybdenum　(Mo)　and　tungsten　(W).　Under　the　optimized　conditions,　UiO-66-CTAB　with　uniform　pore　size　and　containing　particles　with　tetrahedral　cage　structure　could　be　obtained.　UiO-66-CTAB　showed　BET　surface　area　and　micropore　volume　of　873.848　m2·g−1　and　0.403　cm3·g−1,　respectively,　with　the　particle　size　range　of　200–300　nm.　It　acquired　positive　charge　at　pH　＜　7,　thus　it　could　get　easily　connected　with　the　negatively　charged　Mo　species.　The　material　shows　excellent　adsorption　of　Mo　and　its　effective　separation　from　W　in　acidic　solution.　It　is　beneficial　for　separation　at　room　temperature　under　the　optimal　contact　time　of　3　h.　The　adsorption　capacity　for　Mo　(QMo)　was　355　mg·g−1　and　the　highest　separation　factor　(βMo/W)　was　51.4.　Comprehensive　analysis　of　XRD,　SEM,　FT-IR　spectroscopy,　XPS,　and　thermodynamic　results　indicate　that　the　adsorption　mechanism　involved　the　selectivity　of　the　effect　of　pore　size,　stronger　affinity　of　the　metal　point　Zr　for　Mo,　and　coordination　interaction　between　the　N　atom　of　CTAB　and　Mo　element,　which　allowed　more　Mo-homopoly　acid　ions　to　enter　the　cage　and　significantly　hindered　the　entrance　of　W-homopoly　acid　ions　into　the　UiO-66-CTAB.　The　adsorbent　UiO-66-CTAB　can　be　considered　as　a　potential　candidate　for　new　and　green　adsorbent　materials　for　the　separation　and　recovery　of　W　and　Mo　in　the　treatment　of　ores,　wastes,　and　wastewater,　which　is　beneficial　for　environmental　protection.　©　2024