安徽大学葛炳辉团队报道了通过界面工程调整液态金属纳米液滴异质结构生长。相关研究成果于2024年7月8日发表在国际顶尖学术期刊《美国化学会志》。

液态金属（LM）纳米液滴具有有趣的表面性质，因此在化学合成、催化和生物医学方面具有很好的潜力。然而，LM纳米液滴表面的反应动力学和产物生长受到所涉及的界面的显著影响，这一点尚未得到彻底的探索和理解。

该文中，研究人员提出了一种界面工程策略，以Ga⁰和AuCl₄^-离子之间的自发电流反应为代表，通过在LM和反应环境之间建立厚度可控的介电界面，成功地调节Ga基LM纳米液滴表面异质结构的生长。结合高分辨率电子能量损失谱（EELS）分析和理论模拟，发现界面处的诱导电荷分布主导了反应位点的时空分布。

采用不同厚度的氧化钨（WOx）作为LM的介电界面，Ga@WOx@Au已经实现了具有不同核壳卫星或类二聚体异质结构，并表现出不同的光探测光响应能力。

了解产品生长的动力学和介电界面的调控策略，为控制涉及LM纳米液滴的化学过程中，产品的结构和性能提供了一种实验方法。

附：英文原文

Title: Tailoring Heterostructure Growth on Liquid Metal Nanodroplets through Interface Engineering

Author: Siqi Guo, Yuan Ji, Gengcheng Liao, Jian Wang, Zhong-Hui Shen, Xiang Qi, Christian Liebscher, Ningyan Cheng, Long Ren, Binghui Ge

Issue&Volume: July 8, 2024

Abstract: Liquid metal (LM) nanodroplets possess intriguing surface properties, thus offering promising potential in chemical synthesis, catalysis, and biomedicine. However, the reaction kinetics and product growth at the surface of LM nanodroplets are significantly influenced by the interface involved, which has not been thoroughly explored and understood. Here, we propose an interface engineering strategy, taking a spontaneous galvanic reaction between Ga0 and AuCl4– ions as a representative example, to successfully modulate the growth of heterostructures on the surface of Ga-based LM nanodroplets by establishing a dielectric interface with a controllable thickness between LM and reactive surroundings. Combining high-resolution electron energy-loss spectroscopy (EELS) analysis and theoretical simulation, it was found that the induced charge distribution at the interface dominates the spatiotemporal distribution of the reaction sites. Employing tungsten oxide (WOx) with varying thicknesses as the demonstrated dielectric interface of LM, Ga@WOx@Au with distinct core–shell-satellite or dimer-like heterostructures has been achieved and exhibited different photoresponsive capabilities for photodetection. Understanding the kinetics of product growth and the regulatory strategy of the dielectric interface provides an experimental approach to controlling the structure and properties of products in LM nanodroplet-involved chemical processes.

DOI: 10.1021/jacs.4c02521

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c02521