CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, 230026, China; School of Energy and Environment, City University of Hong Kong, Kowloon, Hong Kong Special Administrative Region, 999077, China.
School of Metallurgy and Environment, Central South University, Changsha, 410083, China.
Water Res. 2023 Sep 1;243:120424. doi: 10.1016/j.watres.2023.120424. Epub 2023 Jul 27.
Proteins are important constituents of dissolved organic matter (DOM) in aqueous environments, and their interaction with humic acid (HA), another key component of DOM, substantially affects the environmental behaviors of DOM. In this work, the interaction mechanisms between tryptophan-containing proteins and HA were systematically investigated using multiple molecular spectroscopic approaches. The fluorescence quenching tests indicate that bovine serum albumin (BSA) was more readily quenched by HA and the coexisting phenolic, carboxyl, and quinone groups in HA contributed to this process significantly. By comparison, the fluorescence of L-tryptophan (L-Trp) was more stable under the same conditions. Furthermore, with multiple groups in HA, static quenching with the binding constants and the number of sites were calculated in the protein-HA and L-Trp-HA mixtures. In addition, the differential fluorescence spectra, UV‒Vis spectra, and two-dimensional correlation spectroscopy results confirmed that L-tryptophan amino acid could indeed form a complex with HA, while did not lead to fluorescence quenching. Finally, the molecular docking and density functional theory (DFT) simulations highlighted the contribution of multiple residues surrounding the HA groups to their interactions. The direct interaction between the tryptophan residue and HA might not be the prerequisite for the fluorescence response. Therefore, our work provides further insights into protein-HA interactions and implies other reasonable elucidations for further explanation.
蛋白质是水相环境中溶解有机物质(DOM)的重要组成部分,它们与腐殖酸(HA)的相互作用,DOM 的另一个关键组成部分,极大地影响了 DOM 的环境行为。在这项工作中,我们采用多种分子光谱方法系统地研究了含色氨酸蛋白质与 HA 之间的相互作用机制。荧光猝灭试验表明,牛血清白蛋白(BSA)更容易被 HA 猝灭,而 HA 中共存的酚、羧基和醌基团对这一过程有显著贡献。相比之下,在相同条件下,L-色氨酸(L-Trp)的荧光更稳定。此外,在 HA 存在多个基团的情况下,通过计算蛋白质-HA 和 L-Trp-HA 混合物中的结合常数和结合位点数,得出了静态猝灭的结果。此外,差示荧光光谱、紫外-可见光谱和二维相关光谱结果证实,L-色氨酸氨基酸确实可以与 HA 形成复合物,而不会导致荧光猝灭。最后,分子对接和密度泛函理论(DFT)模拟强调了 HA 基团周围多个残基对它们相互作用的贡献。色氨酸残基与 HA 的直接相互作用可能不是荧光响应的前提条件。因此,我们的工作为蛋白质-HA 相互作用提供了进一步的见解,并为进一步解释提供了其他合理的阐述。