Assessing supported nickel catalysts for the upcycling of real WEEE plastics through low-pressure hydropyrolysis and dehalogenation†

IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Green Chemistry Pub Date : 2025-04-29 DOI:10.1039/D4GC06546H
Lidia Amodio, Jennifer Cueto, Julio López, Héctor Hernando, Patricia Pizarro and David P. Serrano
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Abstract

Electrical and electronic equipment waste (WEEE) is among the fastest-growing waste streams, posing recycling challenges due to its high heterogeneity and the presence of organo-halogenated compounds. Hydropyrolysis offers a promising way to convert WEEE plastics into valuable, dehalogenated organic liquids, facilitating their upcycling. This study examines catalytic hydropyrolysis at mild pressure of real WEEE plastics containing both chlorine and bromine. Nickel-based catalysts on various supports (Al2O3, n-ZSM-5 zeolite, SiO2, and activated carbon (AC)) were tested in batch and continuous systems. In the thermal reaction, over 70 wt% oil was obtained, decreasing slightly with catalyst use. Char played a key role in removing halogens, retaining up to 95%, which was reinforced by the dehalogenation activity of the catalysts. While all catalysts were highly efficient for oil dehalogenation, the best performance was shown by Ni/AC. The AC support alone contributed significantly to halogen trapping, while Ni incorporation into the catalyst further enhanced the oil dehalogenation degree, allowing total Br removal and reducing its Cl content to just 9 ppm, as well as enhancing the production of valuable monoaromatic hydrocarbons. The Ni/AC catalyst exhibited high stability over time on stream when using a continuous oil feeding reaction system and could be fully regenerated by water/dioxane washing, restoring its dehalogenation capability to the level of the fresh one. This work highlights the potential of catalytic hydropyrolysis to address the environmental challenges posed by WEEE plastics, offering a sustainable alternative for their dehalogenation and upcycling into valuable chemical products.

负载型镍催化剂对废旧电子电气设备塑料低压加氢热解脱卤升级回收的影响
电气和电子设备废物(WEEE)是增长最快的废物流之一,由于其高度异质性和有机卤化化合物的存在,构成了回收挑战。加氢热解为将报废电子电气设备塑料转化为有价值的脱卤有机液体提供了一种很有前途的方法,促进了它们的升级回收。本研究考察了含氯和溴的真实WEEE塑料在温和压力下的催化加氢热解。不同载体(Al2O3、n-ZSM-5沸石、SiO2和活性炭)上的镍基催化剂在间歇和连续系统中进行了测试。在热反应中,得到的油大于70 wt%,随着催化剂的使用略有下降。炭在去除卤素方面起着关键作用,保留率高达95%,催化剂的脱卤活性增强了这一点。所有催化剂均具有较好的脱卤效果,其中Ni/AC催化剂的脱卤效果最好。AC载体本身对卤素捕获有显著的贡献,而Ni加入催化剂进一步提高了石油的脱卤程度,允许总Br去除,并将其Cl含量降低到仅9 ppm,同时提高了有价值的单芳烃的产量。在连续进油反应系统中,Ni/AC催化剂表现出高的稳定性,并且可以通过水/二氧六环洗涤完全再生,使其脱卤能力恢复到新鲜的水平。这项工作强调了催化加氢热解解决WEEE塑料带来的环境挑战的潜力,为其脱卤和升级回收为有价值的化学产品提供了可持续的替代方案。
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来源期刊
Green Chemistry
Green Chemistry 化学-化学综合
CiteScore
16.10
自引率
7.10%
发文量
677
审稿时长
1.4 months
期刊介绍: Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.
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