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首页> 外文期刊>ACS catalysis >Engineering Gold Nanoparticles with DNA Ligands for Selective Catalytic Oxidation of Chiral Substrates
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Engineering Gold Nanoparticles with DNA Ligands for Selective Catalytic Oxidation of Chiral Substrates

机译：具有DNA配体的工程金纳米颗粒用于手性基质的选择性催化氧化。

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Noble metal nanoparticles are promising materials for heterogeneous enantioselective catalysis because of their high surface-to-volume ratios, large concentrations of highly undercoordinated surface sites, and quantum confinement effects. In this work, we report on the use of DNA as an environment-responsive chiral ligand to engineer the selective catalytic behaviors of glucose oxidase-mimicking gold nanoparticles (AuNPs), with glucose enantiomers as the substrates. DNA can be stimulated externally to switch between random-coiled and multistranded structures (e.g., duplex, i-motif, or G-quadruplex). Random-coiled DNA-capped nanoparticles preferentially catalyze oxidation of l-glucose, and structured DNA-capped nanoparticles show higher activity toward d-glucose. pH-induced selectivity diminishment of DNA-treated AuNPs is also found, further demonstrating the chiral selector effect of DNA ligands. In the end, the selective catalysis of AuNPs allows control of the size enlargement of nanoparticles through self-catalytic Au-0 deposition, in ligand- and substrate chirality-dependent manners. It is found that the effect of substrate chirality on the self-growth rate can be reversed by the hybridization of the capping DNA. The structural and chemical features of DNA grooves in the multistranded structures render binding sites with higher affinity to D-glucose than L-glucose. The results suggest a simple strategy for engineering the responsive enantioselective catalysis of metallic nanoparticles and advance the understanding of chiral interactions between nucleic acids and saccharide.
机译：贵金属纳米粒子具有高的表面体积比，高浓度的高度不配位的表面位点以及量子限制效应，因此是用于多相对映选择性催化的有前途的材料。在这项工作中，我们报道了使用DNA作为对环境敏感的手性配体来设计以葡萄糖对映体为底物的模仿葡萄糖氧化酶的金纳米颗粒（AuNPs）的选择性催化行为。可以从外部刺激DNA以在随机螺旋结构和多链结构之间切换（例如，双链体，i-基序或G-四链体）。随机缠绕的DNA封端的纳米颗粒优先催化l-葡萄糖的氧化，结构化的DNA封端的纳米颗粒对d-葡萄糖具有更高的活性。还发现pH诱导的DNA处理的AuNPs的选择性降低，进一步证明了DNA配体的手性选择剂作用。最后，AuNPs的选择性催化可以通过自催化Au-0沉积以配体和底物手性依赖的方式控制纳米颗粒的尺寸增大。发现通过覆盖DNA的杂交可以逆转底物手性对自生长速率的影响。多链结构中DNA凹槽的结构和化学特征使结合位点对D-葡萄糖的亲和力高于L-葡萄糖。结果提示了一种工程化金属纳米颗粒的对映选择性催化的简单策略，并增进了对核酸和糖类之间手性相互作用的理解。

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