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The binary Ag3PO4/MIL-125-NH2 (AMN-X) composites were synthesized through ion exchange-solution method, and the ternary Ag/Ag3PO4/MIL-125-NH2 (AAMN-X) Z-scheme heterojunctions were prepared via the photo chemical reduction deposition strategy. The photocatalytic hexavalent chromium (Cr(VI)) sequestration over AMN-X and AAMN-X were investigated under visible light. AAMN-120 accomplished superior reduction performance due to that Ag nanoparticles (NPs) act as electrons transfer bridge to enhance the separation efficiency of photogenerated e--h+pairs, in which the reaction rates (k value) were 2.77 and 124.2 fold higher than those of individual MIL-125-NH2 and Ag3PO4, respectively. The influences of different pH values, small organic acids and coexisting ions on the photocatalytic performance of AAMN-120 were also investigated. In addition, the AAMN-120 heterojunction expressed great reusability and stability in cycling experiments. The mechanism of photocatalytic Cr(VI) was investigated and verified through photoluminescence (PL), electrochemistry, electron spin resonance (ESR), active species capture, and Pt element deposition experiments.