Accumulation-Driven Unified Spatiotemporal Synthesis and Structuring of Immiscible Metallic Nanoalloys
Accumulation-Driven Unified Spatiotemporal Synthesis and Structuring of Immiscible Metallic Nanoalloys
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DOI：
10.1016/j.matt.2019.10.017
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发表时间：
2019-12-04
期刊：
影响因子：
18.9
通讯作者：
Zheng, Yuebing
中科院分区：
文献类型：
--
作者：
Rajeeva, Bharath Bangalore;Kunal, Pranaw;Zheng, Yuebing
积累介导的化学反应是自然界中普遍存在的现象。在这里，我们探索微泡诱导的前体离子的积累，以实现不混溶的金属纳米合金的无表面活性剂的合成，同时图案的纳米合金成目标的架构，其增强的催化应用。我们的统一时空合成和结构化（US 3）策略，即毫秒级的离子积累发生在一个高度限制的激光介导的微泡阱（MBT），驱动超快合金合成与结构化过程同步。作为一个恰当的例子，我们采用US 3战略的原位无表面活性剂的合成和图案化的传统不混溶的铑-金（RhAu）纳米合金。随机游走模拟证明毫秒级的积累过程，导致合成时间减少3阶。以NaBH 4还原对硝基苯酚为反应体系，考察了催化剂的催化活性和结构与性能的关系。我们的原位合成和结构化策略可用于高通量生产和筛选具有定制催化，光电和磁性功能的多金属系统。
Accumulation-mediated chemical reactions are a ubiquitous phenomenon in nature. Here, we explore microbubble-induced accumulation of precursor ions to achieve surfactant-free synthesis of immiscible metallic nanoalloys and simultaneously pattern the nanoalloys into targeted architectures for their enhanced catalytic applications. Our unified spatiotemporal synthesis and structuring (US3) strategy, whereby millisecond-scale accumulation of the ions takes place in a highly confined laser-mediated microbubble trap (MBT), drives ultrafast alloy synthesis in sync with the structuring process. As a case in point, we employ the US3 strategy for the in situ surfactant-free synthesis and patterning of traditionally immiscible rhodium-gold (RhAu) nanoalloys. Stochastic random walk simulations justify the millisecond-scale accumulation process, leading to a 3-order reduction in synthesis time. The catalytic activity and structure-property relationship were evaluated using the reduction of p-nitrophenol with NaBH4. Our in situ synthesis and structuring strategy can be translated for high-throughput production and screening of multimetallic systems with tailored catalytic, optoelectronic, and magnetic functions.