2D Chiroptical Nanostructures for High‐Performance Photooxidants,Advanced Functional Materials

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2D Chiroptical Nanostructures for High‐Performance Photooxidants
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2018-03-07 , DOI: 10.1002/adfm.201707237
Liguang Xu _{1,

2} , Maozhong Sun _{1,

2} , Ping Cheng ₃ , Rui Gao ₄ , Hui Wang ₃ , Wei Ma _{1,

2} , Xinghua Shi ₃ , Chuanlai Xu _{1,

2} , Hua Kuang _{1,

2}

Affiliation

Modulation of the chirality of solid‐like nanoscale membranous structures used as selective photooxidants is an important goal of chemical and materials science. Here, the fabrication of a chiral plasmonic nanoparticle monolayer film which is a highly selective photooxidant under circularly polarized light (CPL) in the visible‐light region is reported. The chiroptical activity of the film can be controlled by altering the amount and stereochemistry of amino acids. The experiments disclose that this stable and reusable catalyst is active in the selective oxidation of glucose enantiomers and CPL of opposite polarization gives around 10.3‐fold increase in conversion rates. The results reveal that the handedness of polarized light dominates the catalytic activity of the chiral film. It is demonstrated that the specific chiral binding of the amino acid ligands and the local field enhancement in the light‐limited regime regulates the selective photocatalytic performance, as confirmed by first‐principles density functional theory and physical field simulations. With the catalyst's signature ability for chiral recognition and switching of handedness of polarized light, the discovery provides a foundation for designing and tailoring chiral inorganic photooxidants. This research also sets an example for the development of light–matter interactions and polarized optics.

中文翻译：

用于高性能光氧化剂的二维手性纳米结构

用作选择性光氧化剂的固体状纳米级膜状结构的手性的调节是化学和材料科学的重要目标。在这里，报道了一种手性等离子体纳米单层膜的制备，该膜是在可见光区域内在圆偏振光（CPL）下具有高度选择性的光氧化剂。膜的手性可以通过改变氨基酸的数量和立体化学来控制。实验表明，这种稳定且可重复使用的催化剂在葡萄糖对映异构体的选择性氧化中具有活性，而相反极性的CPL可使转化率提高约10.3倍。结果表明，偏光的手性主导了手性膜的催化活性。正如第一原理密度泛函理论和物理场模拟所证实的，事实证明，氨基酸配体的特定手性结合和光限制机制中的局部场增强调节了选择性光催化性能。该发现物具有手性识别和偏振光手性切换的签名能力，这一发现为设计和定制手性无机光氧化剂提供了基础。这项研究也为光-物质相互作用和偏振光学的发展树立了榜样。该发现具有手征性识别和偏振光手性切换的签名能力，为设计和定制手性无机光氧化剂提供了基础。这项研究也为光-物质相互作用和偏振光学的发展树立了榜样。该发现具有手征性识别和偏振光手性切换的签名能力，为设计和定制手性无机光氧化剂提供了基础。这项研究也为光-物质相互作用和偏振光学的发展树立了榜样。

更新日期：2018-03-07

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