Jin Jie, Li Haoran, Wang Hongfa, Fang Qunling, Xu Yunqi, Kong Weili, Chen Xia, Leung Ken Cham-Fai, Wang Hailong, Xuan Shouhu
School of Materials and Chemical Engineering, Anhui Jianzhu University, Hefei, 230601, PR China.
CAS Key Laboratory of Mechanical Behavior and Design of Materials, Department of Modern Mechanics, University of Science and Technology of China, Hefei, 230026, PR China.
Dalton Trans. 2024 Nov 12;53(44):17864-17879. doi: 10.1039/d4dt02425g.
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 FeO@AgPd/Polydopamine (FeO@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 FeO@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 FeO nanosphere played a critical role on the high catalytic activity. Moreover, FeO@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 FeO@AgPd/PDA nanosnowman exhibited good cyclic catalytic activity. With its multi-mode catalysis, NIR-enhanced catalytic activity, and easy separation, the FeO@AgPd/PDA nanosnowman exhibits great application potential in nanocatalysis.
尽管双金属贵金属纳米结构在纳米催化中通常具有高活性，但其可控制备、可调催化活性和易于分离仍然是重大挑战。在本研究中，通过一步模板置换-氧化还原聚合法设计了一种负载AgPd纳米笼的FeO@AgPd/聚多巴胺（FeO@AgPd/PDA）纳米雪人。AgPd纳米笼赋予产物对有机污染物（4-硝基苯酚、甲基橙、亚甲基蓝）还原反应的高催化活性。有趣的是，在近红外（NIR）光下，FeO@AgPd/PDA纳米雪人对有机污染物催化还原的动力学分别提高了2.6倍、1.57倍和5.45倍。不对称纳米结构促进了电子-空穴对的分离，促进了电子转移，并加速了催化活性。密度泛函理论（DFT）分析表明，AgPd合金与FeO纳米球之间的电子转移对高催化活性起着关键作用。此外，FeO@AgPd/PDA在Heck碳-碳偶联反应中也表现出优异的催化活性，转化率>95%，选择性>99%。由于PDA壳层封装良好且具有出色的磁性，FeO@AgPd/PDA纳米雪人表现出良好的循环催化活性。凭借其多模式催化、近红外增强催化活性和易于分离的特点，FeO@AgPd/PDA纳米雪人在纳米催化中展现出巨大的应用潜力。
