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银纳米颗粒增强的具有界面工程的金属有机基质用于高效光催化析氢。

Silver nanoparticle enhanced metal-organic matrix with interface-engineering for efficient photocatalytic hydrogen evolution.

机构信息

Énergie Matériaux et Télécommunications, Institut National de la Recherche Scientifque (INRS) 1650 Boul. Lionel-Boulet, Varennes, QC, J3X 1P7, Canada.

Center for Advancing Electronics Dresden (Cfaed), Technische Universität Dresden, 01062, Dresden, Germany.

出版信息

Nat Commun. 2023 Feb 1;14(1):541. doi: 10.1038/s41467-023-35981-8.

Abstract

Integrating plasmonic nanoparticles into the photoactive metal-organic matrix is highly desirable due to the plasmonic near field enhancement, complementary light absorption, and accelerated separation of photogenerated charge carriers at the junction interface. The construction of a well-defined, intimate interface is vital for efficient charge carrier separation, however, it remains a challenge in synthesis. Here we synthesize a junction bearing intimate interface, composed of plasmonic Ag nanoparticles and matrix with silver node via a facile one-step approach. The plasmonic effect of Ag nanoparticles on the matrix is visualized through electron energy loss mapping. Moreover, charge carrier transfer from the plasmonic nanoparticles to the matrix is verified through ultrafast transient absorption spectroscopy and in-situ photoelectron spectroscopy. The system delivers highly efficient visible-light photocatalytic H generation, surpassing most reported metal-organic framework-based photocatalytic systems. This work sheds light on effective electronic and energy bridging between plasmonic nanoparticles and organic semiconductors.

摘要

将等离子体纳米粒子集成到光活性的金属-有机骨架中是非常可取的,因为等离子体近场增强、互补光吸收以及在结界面处光生载流子的加速分离。构建明确的、紧密的界面对于有效的载流子分离至关重要,但在合成中仍然是一个挑战。在这里,我们通过简便的一步法合成了一种带有紧密界面的结,该结由等离子体 Ag 纳米粒子和具有银节点的基质组成。通过电子能量损失映射可视化了 Ag 纳米粒子对基质的等离子体效应。此外,通过超快瞬态吸收光谱和原位光电子能谱验证了载流子从等离子体纳米粒子到基质的转移。该体系实现了高效的可见光光催化 H2 生成,超过了大多数报道的基于金属-有机骨架的光催化体系。这项工作为等离子体纳米粒子和有机半导体之间有效的电子和能量桥接提供了思路。

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