In this study, the 3D intertwined tubular structure of carbon nanotube sponge (CNTS) was utilized to intersperse MIL-53(Fe) onto the nanofragments of CNTS. For the preparation of a novel composite catalyst, MIL-53(Fe)@CNTS, nanorestricted domain growth was combined with self-assembly regulation to realize the ordered growth of MIL-53(Fe) in the space of CNTS. The catalyst exhibited excellent activation performance for PMS within a wide pH range. The maximum removal of tetracycline (TC, 20 mg/L) was as high as 96.7 % within 90 min, and the maximum degradation rate constant (K) was as high as 0.1648 min−1. The performance of the catalyst was directly correlated with the number of domain-limited assemblies. Synchrotron radiation results and DFT theoretical calculations confirmed that the overall catalytic performance of MIL-53(Fe) was greatly improved after the nanorestricted domain assembly in CNTS. The TC degradation system involved radical–oxidative and nonradical pathways. The intermediates of the reaction system were identified by HPLC-MS, and several possible degradation pathways during the TC reaction were proposed. The toxicity degree of the intermediate monomers was analyzed in conjunction with the TEST program, and their effects on the biological environment were predicted. Combined with the toxicity prediction of the TC degradation pathways, the post-reaction degradation solution was used for practical biotoxicity assessment. The effects of the real solution before and after degradation on the ecotoxicity of different organisms were also determined. In conclusion, the composite catalyst MIL-53(Fe)@CNTS synthesized by precise assembly using the nanorestricted domain strategy has promising applications in pollutant degradation and environmental remediation.
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