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Click catalysis and DNA conjugation using a nanoscale DNA/silver cluster pair
Nanoscale ( IF 5.8 ) Pub Date : 2024-09-11 , DOI: 10.1039/d4nr02938k Caleb J Setzler 1 , Jeffrey T Petty 1
Nanoscale ( IF 5.8 ) Pub Date : 2024-09-11 , DOI: 10.1039/d4nr02938k Caleb J Setzler 1 , Jeffrey T Petty 1
Affiliation
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DNA-bound silver clusters are most readily recognized by their strong fluorescence that spans the visible and near-infrared regions. From this suite of chromophores, we chose a green-emitting Ag106+ bound to C4AC4TC3GT4 and describe how this DNA/cluster pair is also a catalyst. A DNA-tethered alkyne conjugates with an azide via cycloaddition, an inherently slow reaction that is facilitated through the joint efforts of the cluster and DNA. The Ag106+ structure is the catalytic core in this complex, and it has three distinguishing characteristics. It facilitates cycloaddition while preserving its stoichiometry, charge, and spectra. It also acidifies its nearby alkyne to promote H/D exchange, suggesting a silver–alkyne complex. Finally, it is markedly more efficient when compared with related multinuclear DNA–silver complexes. The Ag106+ is trapped within its C4AC4TC3GT4 host, which governs the catalytic activity in two ways. The DNA has orthogonal functional groups for both the alkyne and cluster, and these can be systematically separated to quench the click reaction. It is also a polydentate ligand that imprints an elongated shape on its cluster adduct. This extended structure suggests that DNA may pry apart the cluster to open coordination sites for the alkyne and azide reactants. These studies indicate that this DNA/silver cluster pair work together with catalysis directly driven by the silver cluster and indirectly guided by the DNA host.
中文翻译：
使用纳米级 DNA/银簇对的点击催化和 DNA 偶联
DNA 结合的银簇最容易通过其跨越可见光和近红外区域的强荧光来识别。从这组发色团中，我们选择了与 C4AC4TC3GT4 结合的绿色发光 Ag106+，并描述了该 DNA/簇对如何成为催化剂。DNA 栓系炔烃通过环加成与叠氮化物偶联，这是一种固有的缓慢反应，通过簇和 DNA 的共同努力而促进。Ag106+ 结构是该复合物中的催化核心，它具有三个显着特性。它促进了环加成反应，同时保留了其化学计量、电荷和光谱。它还酸化了附近的炔烃以促进 H/D 交换，表明银-炔烃络合物。最后，与相关的多核 DNA-银复合物相比，它的效率明显更高。Ag106+ 被困在其 C4AC4TC3GT4 宿主中，该宿主以两种方式控制催化活性。DNA 具有炔烃和簇的正交官能团，这些官能团可以系统地分离以淬灭点击反应。它也是一种多齿配体，在其簇加合物上印记细长的形状。这种扩展的结构表明 DNA 可能会撬开簇以打开炔烃和叠氮化物反应物的配位位点。 这些研究表明，这种 DNA/银簇对与银簇直接驱动并间接由 DNA 宿主引导的催化一起工作。
更新日期：2024-09-11
中文翻译：
使用纳米级 DNA/银簇对的点击催化和 DNA 偶联
DNA 结合的银簇最容易通过其跨越可见光和近红外区域的强荧光来识别。从这组发色团中，我们选择了与 C4AC4TC3GT4 结合的绿色发光 Ag106+，并描述了该 DNA/簇对如何成为催化剂。DNA 栓系炔烃通过环加成与叠氮化物偶联，这是一种固有的缓慢反应，通过簇和 DNA 的共同努力而促进。Ag106+ 结构是该复合物中的催化核心，它具有三个显着特性。它促进了环加成反应，同时保留了其化学计量、电荷和光谱。它还酸化了附近的炔烃以促进 H/D 交换，表明银-炔烃络合物。最后，与相关的多核 DNA-银复合物相比，它的效率明显更高。Ag106+ 被困在其 C4AC4TC3GT4 宿主中，该宿主以两种方式控制催化活性。DNA 具有炔烃和簇的正交官能团，这些官能团可以系统地分离以淬灭点击反应。它也是一种多齿配体，在其簇加合物上印记细长的形状。这种扩展的结构表明 DNA 可能会撬开簇以打开炔烃和叠氮化物反应物的配位位点。 这些研究表明，这种 DNA/银簇对与银簇直接驱动并间接由 DNA 宿主引导的催化一起工作。
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