纳米团簇
脱质子化
肽
胺气处理
光致发光
荧光
半胱氨酸
配体(生物化学)
化学
组合化学
材料科学
光化学
有机化学
生物化学
离子
物理
量子力学
受体
酶
光电子学
作者
Laura Zanetti‐Polzi,Patrick Charchar,Irene Yarovsky,Stefano Corni
出处
期刊:ACS Nano
[American Chemical Society]
日期:2022-10-27
卷期号:16 (12): 20129-20140
被引量:18
标识
DOI:10.1021/acsnano.2c04335
摘要
Ultrasmall peptide-protected gold nanoclusters are a promising class of bioresponsive material exhibiting pH-sensitive photoluminescence. We present a theoretical insight into the effect peptide-ligand environment has on pH-responsive fluorescence, with the aim of enhancing the rational design of gold nanoclusters for bioapplications. Employing a hybrid quantum/classical computational methodology, we systematically calculate deprotonation free energies of N-terminal cysteine amine groups in proximity to the inherently fluorescent core of Au25(Peptide)18 nanoclusters. We find that subtle changes in hexapeptide sequence alter the electrostatic environment and significantly shift the conventional N-terminal amine pKa expected for amino acids free-in-solution. Our findings provide an insight into how the deprotonation equilibrium of N-terminal amine and side chain carboxyl groups cooperatively respond to solution pH changes, explaining the experimentally observed, yet elusive, pH-responsive fluorescence of peptide-functionalized Au25 clusters.
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