Hydroxyl Spillover in Fe–Se Dual-Site Catalysts for Mixed Plastics Assay

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2024-12-24 DOI:10.1021/jacs.4c16655
Yu Wu, Wenxuan Jiang, Weiqing Xu, Fan Lv, Shaojia Song, Liuyong Hu, Canglong Wang, Lirong Zheng, Wenling Gu, Riguang Zhang, Shaojun Guo, Chengzhou Zhu
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Abstract

The complex composition of real plastic wastes poses a significant challenge for their large-scale disposal. A responsive on-site compositional analysis of plastics is informative in choosing downstream processing methods. Nanocatalyst-based assay kit is highly qualified for this scene; however, there remain no efficient nanocatalysts for plastics due to their highly inert chemistry. Herein, we first unveiled the hydroxyl spillover effect in an Fe–Se dual-site catalyst (FeSe/NC) and devised a prototype colorimetric assay kit for mixed plastics. Experimental and theoretical results unveiled that Fe sites acted as the main active sites for H2O2 activation to produce adsorbed hydroxyl (*OH) intermediates, which subsequently desorb as hydroxyl radicals (OH) and transfer to Se sites, supports, and even plastics for further catalysis. Specifically, OH transferred to different plastics shows varying activities, where signal outputs were hereby used as the fingerprint for plastic identification. Moreover, the remaining *OH could respond to redox interferences in the samples for enhanced accuracy. In contrast to traditional techniques involving precise apparatus and complex pretreatments, our approach enables a rapid assay (∼10 min) of raw powdery mixed plastic wastes with an ultralow cost (0.0012 $). This discovery fills a crucial gap in the plastic assay, offering new technical guidance for diverse upcycling and recycling strategies to tackle the global plastic waste crisis.

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混合塑料试验中Fe-Se二元催化剂的羟基溢出
真实塑料垃圾的复杂成分对其大规模处理提出了重大挑战。响应现场的塑料成分分析是信息选择下游加工方法。纳米催化剂为基础的分析试剂盒是高度合格的这个场景;然而,由于其高度惰性的化学性质,目前还没有高效的塑料纳米催化剂。在此,我们首次揭示了Fe-Se双位点催化剂(FeSe/NC)中的羟基溢出效应,并设计了混合塑料的原型比色测定工具。实验和理论结果表明,Fe位点是H2O2活化的主要活性位点,产生吸附的羟基(*OH)中间体,这些中间体随后解吸成为羟基自由基(•OH),并转移到Se位点、载体甚至塑料上进行进一步催化。具体来说,•OH转移到不同的塑料中表现出不同的活性,其中信号输出被用作塑料识别的指纹。此外,剩余的*OH可以响应样品中的氧化还原干扰,以提高准确性。与涉及精密仪器和复杂预处理的传统技术相比,我们的方法能够以超低成本(0.0012美元)快速测定原料粉状混合塑料废物(~ 10分钟)。这一发现填补了塑料分析的一个关键空白,为解决全球塑料废物危机的各种升级回收和回收战略提供了新的技术指导。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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