Lijuan Wu, Jiayin Li, Yin Yang, Kaize Ju, Ziyao Jia, Biqiang Gao, Shiwei Jin, Qun Sun, Laiyan Wu
Cooperative Innovation Center of Unconventional Oil and Gas, Yangtze University (Ministry of Education & Hubei Province), Wuhan, Hubei 430100, China; State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization (Yangtze University), Wuhan 430100, China.
Key Laboratory of Resources Conversion and Pollution Control of the State Ethnic Affairs Commission, College of Resources and Environmental Science, South-Central Minzu University, Wuhan 430074, China.
Int J Biol Macromol. 2025 Sep;321(Pt 3):146442. doi: 10.1016/j.ijbiomac.2025.146442. Epub 2025 Jul 30.
This study investigated the interactions between pepsin (PEP) and the organophosphite antioxidant Irgafos 168 (I 168), its metabolite 2,4-di-tert-butylphenol (24DP), focusing on structural, functional, and antioxidant implications. UV-Vis absorption spectra, fluorescence lifetimes and Stern-Volmer quenching analyses show that I 168/24DP statically bursts PEP with high binding affinity. Thermodynamic parameters, molecular docking analyses and molecular dynamics simulations (e.g. RMSD, Rg) indicate that the spontaneous formation of the stable complexes is mainly driven by van der Waals forces and hydrophobic interactions. I 168 exhibited higher pepsin inhibition (6.97 %-27.51 %) than 24DP (5.04 %-19.29 %), with dose-dependent suppression linked to altered catalytic residue accessibility (e.g., Asp32/Asp215, Tyr75) and disrupted proton transfer efficiency. Structural analyses revealed I 168 increased PEP's flexibility and hydrophobic residue exposure, while 24DP enhanced rigidity and compactness. Antioxidant assays showed 24DP's superior DPPH scavenging capacity (9.45 %-47.35 %) compared to I 168 (2.28 %-8.00 %), though PEP significantly suppressed 24DP's antioxidant efficacy. These findings underscore the necessity of evaluating both parent compounds and metabolites in safety assessments, as metabolic processes retained biological impacts on enzymatic and antioxidant functions. The study provides critical insights into the molecular mechanisms of antioxidant-induced enzyme inhibition and highlights risks to digestive health and food safety.
本研究调查了胃蛋白酶(PEP)与亚磷酸酯抗氧化剂Irgafos 168(I 168)及其代谢产物2,4-二叔丁基苯酚(24DP)之间的相互作用,重点关注结构、功能和抗氧化方面的影响。紫外可见吸收光谱、荧光寿命和斯特恩-沃尔默猝灭分析表明,I 168/24DP以高结合亲和力静态猝灭PEP。热力学参数、分子对接分析和分子动力学模拟(如均方根偏差、回旋半径)表明,稳定复合物的自发形成主要由范德华力和疏水相互作用驱动。I 168对胃蛋白酶的抑制作用(6.97%-27.51%)高于24DP(5.04%-19.29%),剂量依赖性抑制与催化残基可及性改变(如Asp32/Asp215、Tyr75)和质子转移效率破坏有关。结构分析表明,I 168增加了PEP的灵活性和疏水残基暴露,而24DP增强了刚性和紧凑性。抗氧化试验表明,与I 168(2.28%-8.00%)相比,24DP具有更强的1,1-二苯基-2-三硝基苯肼清除能力(9.45%-47.35%),尽管PEP显著抑制了24DP的抗氧化功效。这些发现强调了在安全性评估中同时评估母体化合物和代谢产物的必要性,因为代谢过程对酶和抗氧化功能保留了生物学影响。该研究为抗氧化剂诱导的酶抑制的分子机制提供了关键见解,并突出了对消化健康和食品安全的风险。