Activating Molybdenum Peroxide Scissors for Converting Polyamide Plastic into Low Carbon Alcohols

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-03-14 DOI:10.1002/anie.202423766
Miao Kan, Meng Tao, Weijie Zhuang, Shiqun Wu, Li Wan, Yong Wang, Jinlong Zhang
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Abstract

Direct chemical conversion of plastic waste into low-carbon oxygenates, rather than carbon dioxide, with renewable energy, is important yet challenging. Due to high C─X (X═C, H, N) bond energy, fully optimized catalysts are required to enable precise bond cleavage for boosted efficiency and selectivity. Here, adaptable and recyclable molybdenum peroxide photocatalysts that demonstrate chemical scissors for the selective conversion of polyamide to alcohols are reported. It shows that dimensionally adaptable Mo(+5.8)-(O2) is activated via a ligand-to-metal charge transfer (LMCT) process for localized catalysis to precisely cleave C─X bonds into C2 and C1 alcohols. The additional hydrogen peroxide facilitates the activation and regeneration of the catalytic scissors. These scissors ultimately cut PA6 into methanol with an efficiency of 2.55 mmol L−1 h−1 and a selectivity of 82.4 %. This work provides insights into the role of adaptable metal peroxides in precisely cutting C─X bonds, which benefits chemical conversion of plastic wastes.

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活化过氧化钼剪刀将聚酰胺塑料转化为低碳醇
利用可再生能源将塑料垃圾直接化学转化为低碳氧化物,而不是二氧化碳,这很重要,但也很有挑战性。由于高的C-X (X = C, H, N)键能,需要充分优化的催化剂来实现精确的键裂解,以提高效率和选择性。在这里,我们报告了适应性和可回收的过氧化钼光催化剂,证明了聚酰胺选择性转化为酒精的化学剪刀。我们的实验和计算表明,尺寸适应性Mo(+5.8)-(O2)通过配体到金属电荷转移(LMCT)过程被激活,在照明下进行局部催化,精确地切割C-X键,生成C2和C1醇。额外的过氧化氢提供质子和过氧化条件,促进催化剪刀的活化和再生。化学剪刀的精确结构最终为PA6的精确氧化和切割成甲醇创造了条件,效率为2.55 mmol·L−1·h−1,选择性为82.4%。这项工作提供了适应性金属过氧化物在精确切割C-X键中的作用的见解,这对于塑料废物的高效和选择性化学转化至关重要。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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