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A new ternary phosphidopolysilicate (IV), KSi2P3, has been synthesized by high temperature solid state reaction. The compound crystallizes in a new structure type in the monoclinic space group C2/c with a=10.1327(5)Å, b=10.1382(5)Å, c=21.1181(10)Å, β=96.88(0)°, and Z=8. In the structure, all SiP4 tetrahedra are connected with each other by corner-sharing P atoms to form layers, which are stacked along c direction and separated by K+ cations. The two-dimensional structure of KSi2P3 contrasts with those of the two known members in the ternary A/Si/P (A=alkali metal) system, namely Na5SiP3 (zero-dimensional) and K2SiP2 (one-dimensional), which contains less amount of Si. The band gap deduced from UV–vis–IR diffuse reflectance spectrum is 1.72eV. [ABSTRACT FROM AUTHOR]