抑制甲烷形成的双金属催化剂聚乙烯氢解作用

IF 4.3 3区 工程技术 Q2 ENGINEERING, CHEMICAL Frontiers of Chemical Science and Engineering Pub Date : 2024-06-24 DOI:10.1007/s11705-024-2461-x
Xiangkun Zhang, Bingyan Sun, Zhigang Zhao, Tan Li, Marc Mate, Kaige Wang
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引用次数: 0

摘要

氢解是一种很有前景的塑料化学回收方法。贵金属(如 Ru 和 Pt)被认为是塑料氢解的有效催化剂,但它们会产生大量低价值的气态产物。在这项研究中,通过在二氧化硅载体上分别浸渍 Ni 和 Ru,开发出了一种高效的双金属催化剂,在温和的反应条件下,液态产物的产率高达 83.1%,而单一贵金属催化剂的产率仅为 65.5%。与使用 Ru 催化剂相比,使用 Ni 改性催化剂进行低密度聚乙烯氢解产生的液体产物的碳分布也转向较重的部分。同时,NiRu 催化剂在抑制端链 C-C 键裂解方面表现出色,甲烷产率仅为 10.4 C%,比 Ru/SiO2 催化剂低 69%。为了揭示低密度聚乙烯在双金属催化剂上加氢分解的详细机理,还进一步进行了氢气和丙烷的温度编程还原和解吸。结果表明,Ni-Ru 合金具有更强的氢吸附性能,这表明催化剂表面的氢覆盖率提高了,从而增强了反应中间产物的解吸能力。碳数分布最终偏向于较重的液体产物。
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Polyethylene hydrogenolysis over bimetallic catalyst with suppression of methane formation

Hydrogenolysis has been explored as a promising approach for plastic chemical recycling. Noble metals, such as Ru and Pt, are considered effective catalysts for plastic hydrogenolysis, however, they result in a high yield of low-value gaseous products. In this research, an efficient bimetallic catalyst was developed by separate impregnation of Ni and Ru on SiO2 support resulting in liquid products yield of up to 83.1 C % under mild reaction conditions, compared to the 65.5 C % yield for the sole noble metal catalyst. The carbon distribution of the liquid products from low density polyethylene hydrogenolysis with Ni-modified catalyst also shifted to a heavier fraction, compared to that with Ru catalyst. Meanwhile, the NiRu catalyst exhibited excellent performance in suppressing the cleavage of the end-chain C–C bond, leading to a methane yield of only 10.4 C %, which was 69% lower than that of the Ru/SiO2 catalyst. Temperature programmed reduction and desorption of hydrogen and propane were further conducted to reveal the detailed mechanism of low density polyethylene hydrogenolysis over the bimetallic catalyst. The results suggested that the Ni-Ru alloy exhibited stronger H adsorption properties indicating improved hydrogen coverage on the catalyst surface thus enhancing the desorption of reaction intermediates. The carbon number distribution was ultimately skewed toward heavier liquid products.

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来源期刊
CiteScore
7.60
自引率
6.70%
发文量
868
审稿时长
1 months
期刊介绍: Frontiers of Chemical Science and Engineering presents the latest developments in chemical science and engineering, emphasizing emerging and multidisciplinary fields and international trends in research and development. The journal promotes communication and exchange between scientists all over the world. The contents include original reviews, research papers and short communications. Coverage includes catalysis and reaction engineering, clean energy, functional material, nanotechnology and nanoscience, biomaterials and biotechnology, particle technology and multiphase processing, separation science and technology, sustainable technologies and green processing.
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