Asymmetric magnetic nanosnowman loaded with AgPd nanocage toward NIR-enhanced catalytic activity†

IF 3.5 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Dalton Transactions Pub Date : 2024-10-14 DOI:10.1039/D4DT02425G
Jie Jin, Haoran Li, Hongfa Wang, Qunling Fang, Yunqi Xu, Weili Kong, Xia Chen, Ken Cham-Fai Leung, Hailong Wang and Shouhu Xuan
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Abstract

Although bimetallic noble nanostructures often possess high activity in nanocatalysis, their controllable fabrication, tunable catalytic activity, and easy separation remain significant challenges. In this study, an Fe3O4@AgPd/Polydopamine (Fe3O4@AgPd/PDA) nanosnowman loaded with an AgPd nanocage was designed by a one-step template-disposition-redox polymerization method. The AgPd nanocage endowed the product with high catalytic activity for the reduction of organic pollutants (4-NP, MO, MB). Interestingly, under near-infrared (NIR) light, the catalytic kinetics of the Fe3O4@AgPd/PDA nanosnowman on catalytic reduction of organic pollutants increased by 2.6, 1.57, and 5.45 times, respectively. The asymmetric nanostructure facilitated the separation of electron–hole pairs, promoted electron transfer, and accelerated the catalytic activity. Density functional theory (DFT) analysis indicated that the electron transfer between the AgPd alloy and the Fe3O4 nanosphere played a critical role on the high catalytic activity. Moreover, Fe3O4@AgPd/PDA also demonstrated excellent catalytic activity in the Heck carbon–carbon coupling reaction with a >95% conversion rate and >99% selectivity. Owing to the well-encapsulated PDA shell and outstanding magnetic properties, the Fe3O4@AgPd/PDA nanosnowman exhibited good cyclic catalytic activity. With its multi-mode catalysis, NIR-enhanced catalytic activity, and easy separation, the Fe3O4@AgPd/PDA nanosnowman exhibits great application potential in nanocatalysis.

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载入 AgPd 纳米笼的不对称磁性纳米雪人可提高近红外催化活性
尽管双金属惰性纳米结构在纳米催化中通常具有很高的活性,但其可控制备、可调催化活性和易分离性仍然是重大挑战。本研究采用模板-沉积-氧化还原聚合一步法设计了负载 AgPd 纳米载体的 Fe3O4@AgPd/PDA 纳米雪人。AgPd 纳米载体赋予了该产品在还原有机污染物(4-NP、MO、MB)时的高催化活性。有趣的是,在近红外光的作用下,Fe3O4@AgPd/PDA 纳米雪人催化还原有机污染物的催化动力学分别提高了 2.6 倍、1.57 倍和 5.45 倍。不对称的纳米结构有利于电子-空穴对的分离,促进了电子转移,加速了催化活性。密度泛函理论(DFT)分析表明,AgPd 合金与 Fe3O4 纳米球之间的电子转移对高催化活性起着关键作用。此外,Fe3O4@AgPd/PDA 在赫克碳-碳偶联反应中也表现出优异的催化活性,转化率达 95%,选择性达 99%。Fe3O4@AgPd/PDA纳米雪人由于其良好的PDA外壳封装和突出的磁性能,表现出良好的循环催化活性。Fe3O4@AgPd/PDA纳米雪人具有多模式催化、近红外催化活性增强、易分离等特点,在纳米催化领域具有很高的应用潜力。
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来源期刊
Dalton Transactions
Dalton Transactions 化学-无机化学与核化学
CiteScore
6.60
自引率
7.50%
发文量
1832
审稿时长
1.5 months
期刊介绍: Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.
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