Cơ chế hấp phụ và sự tăng cường hóa học phổ SERS của mercaptopurine và thioguanine trên bề mặt Au6 cluster
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Abstract
The density functional theory calculations are employed to elucidate the adsorption behaviours of mercaptopurine (MP) and thioguanine (TG) drugs on the gold surface, using Au6 cluster as a model reactant. The PBE functional in combination with the effective core potential cc-pVTZ-PP basis set for gold atoms and cc-pVTZ basis set for nonmetals are used to investigated geometric structures, thermodynamic parameters and electronic properties of the obtained complexes. The IEF-PCM model with water solvent is applied to include the effect of biological environment on the interactions. The computed results show that the binding is dominated by a covelent bond Au−S and in part by electrostatic effects, namely a hydrogen bond contribution NH∙∙∙Au. In addition, the drug binding to gold clusters is a reversible process and a drug release mechanism was also clarified. Accordingly, the drugs are willing to separate from the gold surface due to either a slight change of pH in tumor cells or the presence of cysteine residues in protein matrices. In particular, the surface-enhanced Raman scattering (SERS) phenomenon of these molecules adsorbed on the Au surfaces are also elucidated.
Tóm tắt
Các phép tính DFT (lý thuyết hàm mật độ) được sử dụng để làm sáng tỏ bản chất của quá trình hấp phụ các phân tử thuốc mercaptopurine (MP) và thioguanine (TG) trên bề mặt vàng, sử dụng Au6 cluster làm mô hình phản ứng. Phiếm hàm PBE kết hợp với bộ cơ sở cc-pVDZ-PP cho Au6 và cc-pVTZ cho các phân tử thuốc được sử dụng để khảo sát cấu trúc hình học, các thông số nhiệt động và tính chất điện tử của các phức chất thu được. Mô hình IEF-PCM với dung môi nước được sử dụng để đánh giá sự ảnh hưởng của môi trường sinh học lên quá trình tương tác. Các kết quả tính toán cho thấy rằng liên kết được quyết định bởi liên kết cộng hóa trị Au−S và một phần bởi hiệu ứng tĩnh điện, cụ thể là liên kết hydro −NH∙∙∙Au. Ngoài ra, sự hấp phụ là quá trình thuận nghịch và cơ chế giải phóng thuốc khỏi bề mặt Au6 cũng được khảo sát. Theo đó, các phân tử thuốc dễ dàng tách khỏi Au6 do sự thay đổi nhỏ của pH trong tế bào khối u hoặc sự hiện diện của cysteine trong protein. Đặc biệt, hiện tượng tán xạ Raman tăng cường bề mặt (SERS) của chúng trên bề mặt kim loại Au cũng được làm sáng tỏ.
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