Bioaccessibility of polypropylene microfiber-associated tetracycline and ciprofloxacin in simulated human gastrointestinal fluids

Abstract

Microplastics residues in natural waters can adsorb organic contaminants owing to their rough surface morphology and high specific surface area, potentially harming human health when ingested. Although humans inevitably ingest microplastics, the bioaccessibility of microplastic-associated chemicals in the human gastric and intestinal fluids remains unresolved. This study investigated the mechanism and primary factor controlling the bioaccessibility of polypropylene (PP) microplastic fiber-associated tetracycline (TC) and ciprofloxacin (CIP) in simulated human gastrointestinal fluids. After mixing 0.1 g of PP microfiber with 10 mg/L of TC (or CIP) for 96 h and exposure to simulated human gastrointestinal fluids, the TC concentrations were 0.440, 0.678, and 1.840 mg/L and the CIP concentrations were 0.700, 1.367, and 3.281 mg/L CIP in the simulated human saliva, gastric, and intestinal fluids after incubation for 60 s, 4 h, and 8 h, respectively. This indicated that the antibiotics TC and CIP adsorbed onto microfiber surface are readily released into human gastrointestinal fluids upon ingestion. Gastric and intestinal fluids showed enhanced bioaccessibility to TC/CIP adhered to PP microfiber. The primary factors affecting the bioaccessibility to TC/CIP adhered to PP microfiber surfaces were found to be pepsin in human gastric fluid and trypsin in human intestinal fluid. Molecular docking and simulated molecular dynamic analyses results showed that pepsin and trypsin stablish connections with TC via hydrogen bonds (reaction sites: pepsin TC: T₁₃₉, T₁₃₆, S₉₇, D₉₄, D₂₇₇ and Y₂₅₁; trypsin TC: S₂₅₇, H₁₂₀, K₂₃₅, G₂₇₄, and G₂₇₆) and CIP via hydrophobic interactions (reaction sites: pepsin CIP: Y₁₃₇, T₁₃₆, T₁₃₉, F₁₇₃, I₃₆₂, V₃₅₃, and I₂₇₅; trypsin CIP: W₂₇₃, I₁₆₁, C₂₅₃, and C₂₇₇). Our findings highlight that microplastic ingestion increases the risk of microplastics and the co-contaminants adsorbed to human health; thus, these findings are helpful to assess the risk of microplastics and co-contaminants to human health.

Keywords: Adsorption/resolution; Gastrointestinal tract; Microfiber; Pepsin/trypsin; Tetracycline and ciprofloxacin.