{"title":"一个模块化的蛋白质-DNA多聚体模型,探索价和单体亲和力如何形成多价DNA结合。","authors":"Hyoin Park, and , Yongwon Jung*, ","doi":"10.1021/acs.analchem.5c02695","DOIUrl":null,"url":null,"abstract":"<p >Multivalent interactions enhance binding strength through the cooperative effects of multiple weak interactions. While multivalency is known to improve sensitivity, increased valency can also enhance nonspecific interactions, potentially compromising selectivity. Insights into the relationship between valency, affinity, and detection performance are needed to optimize both sensitivity and selectivity in multivalent systems. Here, we developed modular protein–DNA multimers (valency 1–4) with uniform spatial arrangement, enabling an investigation of valency-dependent interactions between DNA strands across a broad range of monomeric affinities (subnanomolar to millimolar). Using surface plasmon resonance (SPR) and enzyme-linked immunosorbent assays (ELISA), we quantitatively analyzed how multimerization affects detection sensitivity and selectivity. We found that the optimal range of DNA monomer affinities for effective detection shifted from the nanomolar to the micromolar scale with increasing valency. For example, monomers with <i>K</i><sub>D</sub> values between a few micromolar and ∼50 μM showed the greatest signal amplification upon tetramerization under our conditions. We also discovered that monomers with <i>K</i><sub>D</sub> ≥ ∼50 μM remained largely undetectable even with tetramerization, indicating the presence of an affinity threshold for valency-driven signal enhancement. We further identified a steep transition zone in ELISA signals, where small changes in <i>K</i><sub>D</sub> led to large differences in detection, highlighting a narrow affinity window with maximal selectivity. This <i>K</i><sub>D</sub> window consistently shifted toward weaker affinities as valency increased. These findings show how a modular protein–DNA multimer model can derive quantitative trends for multivalent design, while laying a foundation for future studies in more complex protein systems.</p>","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"97 40","pages":"21883–21890"},"PeriodicalIF":6.7000,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A Modular Protein–DNA Multimer Model to Explore How Valence and Monomer Affinity Shape Multivalent DNA Binding\",\"authors\":\"Hyoin Park, and , Yongwon Jung*, \",\"doi\":\"10.1021/acs.analchem.5c02695\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Multivalent interactions enhance binding strength through the cooperative effects of multiple weak interactions. While multivalency is known to improve sensitivity, increased valency can also enhance nonspecific interactions, potentially compromising selectivity. Insights into the relationship between valency, affinity, and detection performance are needed to optimize both sensitivity and selectivity in multivalent systems. Here, we developed modular protein–DNA multimers (valency 1–4) with uniform spatial arrangement, enabling an investigation of valency-dependent interactions between DNA strands across a broad range of monomeric affinities (subnanomolar to millimolar). Using surface plasmon resonance (SPR) and enzyme-linked immunosorbent assays (ELISA), we quantitatively analyzed how multimerization affects detection sensitivity and selectivity. We found that the optimal range of DNA monomer affinities for effective detection shifted from the nanomolar to the micromolar scale with increasing valency. For example, monomers with <i>K</i><sub>D</sub> values between a few micromolar and ∼50 μM showed the greatest signal amplification upon tetramerization under our conditions. We also discovered that monomers with <i>K</i><sub>D</sub> ≥ ∼50 μM remained largely undetectable even with tetramerization, indicating the presence of an affinity threshold for valency-driven signal enhancement. We further identified a steep transition zone in ELISA signals, where small changes in <i>K</i><sub>D</sub> led to large differences in detection, highlighting a narrow affinity window with maximal selectivity. This <i>K</i><sub>D</sub> window consistently shifted toward weaker affinities as valency increased. These findings show how a modular protein–DNA multimer model can derive quantitative trends for multivalent design, while laying a foundation for future studies in more complex protein systems.</p>\",\"PeriodicalId\":27,\"journal\":{\"name\":\"Analytical Chemistry\",\"volume\":\"97 40\",\"pages\":\"21883–21890\"},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2025-09-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Analytical Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.analchem.5c02695\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, ANALYTICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Analytical Chemistry","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.analchem.5c02695","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
A Modular Protein–DNA Multimer Model to Explore How Valence and Monomer Affinity Shape Multivalent DNA Binding
Multivalent interactions enhance binding strength through the cooperative effects of multiple weak interactions. While multivalency is known to improve sensitivity, increased valency can also enhance nonspecific interactions, potentially compromising selectivity. Insights into the relationship between valency, affinity, and detection performance are needed to optimize both sensitivity and selectivity in multivalent systems. Here, we developed modular protein–DNA multimers (valency 1–4) with uniform spatial arrangement, enabling an investigation of valency-dependent interactions between DNA strands across a broad range of monomeric affinities (subnanomolar to millimolar). Using surface plasmon resonance (SPR) and enzyme-linked immunosorbent assays (ELISA), we quantitatively analyzed how multimerization affects detection sensitivity and selectivity. We found that the optimal range of DNA monomer affinities for effective detection shifted from the nanomolar to the micromolar scale with increasing valency. For example, monomers with KD values between a few micromolar and ∼50 μM showed the greatest signal amplification upon tetramerization under our conditions. We also discovered that monomers with KD ≥ ∼50 μM remained largely undetectable even with tetramerization, indicating the presence of an affinity threshold for valency-driven signal enhancement. We further identified a steep transition zone in ELISA signals, where small changes in KD led to large differences in detection, highlighting a narrow affinity window with maximal selectivity. This KD window consistently shifted toward weaker affinities as valency increased. These findings show how a modular protein–DNA multimer model can derive quantitative trends for multivalent design, while laying a foundation for future studies in more complex protein systems.
期刊介绍:
Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.