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Enhancing Photocatalytic Attributes of Perovskite Nanocrystals in Aqueous Media via Ligand Engineering
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-12-19 , DOI: 10.1021/acsami.3c14321
Monika Ahlawat 1 , Neelakshi 1 , Ramesh Ramapanicker 1 , Vishal Govind Rao 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-12-19 , DOI: 10.1021/acsami.3c14321
Monika Ahlawat 1 , Neelakshi 1 , Ramesh Ramapanicker 1 , Vishal Govind Rao 1
Affiliation
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The remarkable catalytic potential of perovskite nanocrystals (NCs) remains underutilized due to their limited stability in polar media, resulting from the vulnerability of their structure to disruption by polar solvents. In this study, we address this challenge by employing the bolaamphiphilic NKE-12 ligand, which features multiple denticities to effectively shield the surface of CsPbBr3 NCs from polar solvent interactions without compromising their light-harvesting properties. Our research, utilizing electrochemical impedance and photocurrent response measurements, highlights efficient charge separation and charge transfer enabled by NKE-12 ligands, which feature multiple ionic groups and peptide bonds, compared to conventional oleylamine/oleic acid ligands on CsPbBr3 NCs. Through the utilization of purely ligand-derived water-dispersed CsPbBr3/NKE-12 NCs, we successfully showcased their photocatalytic activity for acrylamide polymerization. A series of control experiments unveil a radical-based reaction pathway and suggest the synergistic involvement of photogenerated electrons and holes in producing the O2·– and OH· free radicals, respectively. Our findings emphasize the crucial role of ligand engineering in stabilizing perovskites in water and harnessing their exceptional photocatalytic attributes. This study opens new avenues for applying perovskite NCs in various catalytic processes in polar media.
中文翻译:
通过配体工程增强钙钛矿纳米晶体在水介质中的光催化属性
钙钛矿纳米晶体(NC)的显着催化潜力仍未得到充分利用,因为它们在极性介质中的稳定性有限,这是由于其结构容易被极性溶剂破坏。在本研究中,我们通过采用双亲性NKE-12配体来解决这一挑战,该配体具有多种齿数,可以有效保护CsPbBr 3 NCs表面免受极性溶剂相互作用的影响,同时又不影响其光捕获特性。我们的研究利用电化学阻抗和光电流响应测量,强调了NKE-12配体实现了高效的电荷分离和电荷转移,与CsPbBr 3 NC上的传统油胺/油酸配体相比,NKE-12配体具有多个离子基团和肽键。通过利用纯配体衍生的水分散CsPbBr 3 /NKE-12 NC,我们成功展示了它们对丙烯酰胺聚合的光催化活性。一系列对照实验揭示了基于自由基的反应途径,并表明光生电子和空穴分别协同参与产生 O 2 ·–和 OH ·自由基。我们的研究结果强调了配体工程在稳定水中钙钛矿和利用其卓越的光催化特性方面的关键作用。这项研究为钙钛矿纳米颗粒在极性介质中各种催化过程中的应用开辟了新途径。
更新日期:2023-12-19
中文翻译:
![](https://scdn.x-mol.com/jcss/images/paperTranslation.png)
通过配体工程增强钙钛矿纳米晶体在水介质中的光催化属性
钙钛矿纳米晶体(NC)的显着催化潜力仍未得到充分利用,因为它们在极性介质中的稳定性有限,这是由于其结构容易被极性溶剂破坏。在本研究中,我们通过采用双亲性NKE-12配体来解决这一挑战,该配体具有多种齿数,可以有效保护CsPbBr 3 NCs表面免受极性溶剂相互作用的影响,同时又不影响其光捕获特性。我们的研究利用电化学阻抗和光电流响应测量,强调了NKE-12配体实现了高效的电荷分离和电荷转移,与CsPbBr 3 NC上的传统油胺/油酸配体相比,NKE-12配体具有多个离子基团和肽键。通过利用纯配体衍生的水分散CsPbBr 3 /NKE-12 NC,我们成功展示了它们对丙烯酰胺聚合的光催化活性。一系列对照实验揭示了基于自由基的反应途径,并表明光生电子和空穴分别协同参与产生 O 2 ·–和 OH ·自由基。我们的研究结果强调了配体工程在稳定水中钙钛矿和利用其卓越的光催化特性方面的关键作用。这项研究为钙钛矿纳米颗粒在极性介质中各种催化过程中的应用开辟了新途径。