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Natural phosphate (NP) and synthetic fluorapatite phosphate (SFAP) were proposed as stable, inexpensive, readily available and recyclable catalysts for the condensation of 1,2-diamines with 1,2-dicarbonyls in methanol to afford quinoxaline at room temperature. NP provided as high as 92–99% yield for quinoxalines in short reaction times (i.e., 1–45 min), while SFAP created quinoxalines with 87–97% yield in 60–120 min. From the chemical analyses, X-ray fluoresecency, X-ray diffraction, energy dispersive X-ray and Fourier-transform infrared spectroscopy methods, two main phases (CaO, P₂O₅) appeared in NP together with other low content phases (SiO₂, Fe₂O₃). Compared to other phases, apatite (CaO and P₂O₅ as Ca10(PO₄)₆) played a major role in the catalytic activity of NP. SFAP with similar Ca/P atomic ratio showed a relatively lower catalytic activity than NP for the condensation of 1,2-diamine with 1,2-dicarbonyl in methanol at ambient temperature. To investigate the recyclability of catalysts, the surface properties of NP and 6-recycled NP were investigated using scanning electron microscopy, energy dispersive X-ray and Brunauer–Emmett–Teller and Barrett–Joyner–Halenda methods. Some differences were observed in NP and 6-recycled NP’s particle size, surface area, the volume and size of pores, and the content of elements; nevertheless, the use–reuse process did not noticeably change the catalytic property of NP.