异相ceo2负载cu掺杂Ru催化剂催化氢解低气产物聚乙烯的化学回收

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL
Masazumi Tamura, Yuna Sasano, SMA Hakim Siddiki, Masato Akatsuka, Pengru Chen, Yusuke Kita
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引用次数: 0

摘要

将聚烯烃化学回收为有价值的化学品具有很大的潜力,可以缓解塑料问题,并有助于碳回收。在之前的工作中,我们报道了CeO2-和ZrO2负载的Ru (Ru/CeO2和Ru/ZrO2)催化剂对PE、PP等聚烯烃甚至废PE塑料的氢解是有效的;然而,气体产物的生成率为 ~ 10 %。开发有效的多相催化剂,通过将廉价金属结合到Ru中来抑制廉价气体产品(特别是甲烷)的形成,是实现高产量有价值的化学品(如液体和蜡)的迫切需要。,我们发现1 wt % 1铜掺杂 wt %俄文/ CeO2,铜(1)俄文(1)/ CeO2,是一种有效的非均相催化剂的甲烷形成的抑制(2.3 %,C1-C4气体:∼4%)在 祝辞99 %转换在LDPE的氢解作用5 MPa H2,提供高收益(96 %)有价值的化学物质(液体化学品(C5-C21) + 蜡(C ≥22))。即使在H2压力为2 MPa时,气体选择性仍然很低。通过XRD、TEM、TEM- edx、H2-TPR、XAS和FT-IR等催化剂表征,Cu(1)-Ru(1)/CeO2催化剂上活性金属颗粒的尺寸约为1 nm, Cu金属加入Ru/CeO2后在Ru颗粒上形成Ru-Cu表面合金。通过向Ru中添加廉价的Cu,形成小金属颗粒和Cu-Ru表面合金,降低了Ru系综尺寸,抑制了LDPE的连续C-C键解离,导致甲烷和气体产率降低。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Chemical recycling of polyethylenes with low gas products by catalytic hydrogenolysis with heterogeneous CeO2-supported Cu-doped Ru catalyst

Chemical recycling of polyethylenes with low gas products by catalytic hydrogenolysis with heterogeneous CeO2-supported Cu-doped Ru catalyst

Chemical recycling of polyethylenes with low gas products by catalytic hydrogenolysis with heterogeneous CeO2-supported Cu-doped Ru catalyst
Chemical recycling of polyolefins to valuable chemicals has a high potential to mitigate plastic problems and contributes to carbon recycling. In the previous works, we reported that CeO2- and ZrO2-supported Ru (Ru/CeO2 and Ru/ZrO2) catalysts were effective for the hydrogenolysis of polyolefins such as PE, PP, and even waste PE plastics; however, the gas products were formed in ∼10 % yield. The development of effective heterogeneous catalysts that can suppress the formation of cheap gas products, particularly methane, through the incorporation of inexpensive metals into Ru is highly required to achieve high yields of valuable chemicals such as liquid and waxes. Herein, we found that 1 wt% Cu doped 1 wt% Ru/CeO2, Cu(1)-Ru(1)/CeO2, was an effective heterogeneous catalyst for the suppression of the methane formation (2.3 %, C1–C4 gas: ∼4%) at >99 % conversion in the hydrogenolysis of LDPE at 5 MPa H2, providing the high yield (96 %) of the valuable chemicals (liquid chemicals (C5-C21) + waxes (C ≥22)). The gas selectivity remains low even at a low H2 pressure of 2 MPa. Based on the catalyst characterizations such as XRD, TEM, TEM-EDX, H2-TPR, XAS, and FT-IR analyses, the size of the active metal particles over Cu(1)-Ru(1)/CeO2 catalyst is about 1 nm, and the addition of Cu metal into Ru/CeO2 formed Ru-Cu surface alloy on the Ru particles. The formation of the small metal particles and Cu-Ru surface alloy by the addition of inexpensive Cu to Ru decreased the Ru ensemble size to suppress the consecutive C–C bond dissociation of LDPE, leading to low methane and gas yields.
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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