利用亚临界水氨工艺和废铜催化剂选择性地提升溴化环氧树脂的循环利用率:生产高纯度甲基嘧啶/苯酚并回收铜

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2024-09-21 DOI:10.1016/j.seppur.2024.129827
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引用次数: 0

摘要

四溴双酚 A 环氧树脂(TBBPAER)是电子废物的主要非金属成分。电子废弃物的大规模生产和随之而来的 TBBPAER 废弃物处理问题为化学回收利用提供了巨大的机遇。但由于 TBBPAER 的溴含量高且热稳定性差,其化学回收利用面临巨大挑战。在这项研究中,亚临界水氨(SWA)工艺与废铜基催化剂(WCC)相结合,选择性地将 TBBPAER 高产率(300°C 15 分钟 63.46%,60 分钟 73.66%)转化为低分子量液体产品,包括高附加值的甲基嘧啶和苯酚。WCC 中所含的多价铜之间的电子转移促进了自由基 OH、O2-、NH2 和 :NH 的产生,从而实现了 TBBPAER 的高效转化,脱溴率达 99.29%。TBBPAER 分子链被 OH 和 NH2 切断,生成四溴双酚 A 基团(TAG)和三元碳基团(TCG)。TAG 的进一步降解产生了纯度为 91.8%(气相色谱峰面积%)的酚类化学物质。在 :NH 的诱导下,TCG 进一步环化生成甲基嘧啶,纯度为 91.9%(气相色谱峰面积%)。铜氨络合物的形成导致从 WCC 中浸出/回收了 86.6% 的铜。SWA-WCC 方法证明了 TBBPAER 废物如何成为生产高附加值甲基嘧啶和苯酚化学品的可行原料。这项研究提供了一种新颖的可持续战略,对 TBBPAER 和 WCC 这两种不同的废物进行同步处理/循环利用。对协同处理后的固体残渣进行的铜和锌浸出毒性测试表明,其浸出浓度远低于危险废物标准。
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Selective upcycling of brominated epoxy resin by subcritical water ammonia process with waste copper-based catalyst: Production of high purity methyl pyrimidine/phenols and copper recovery
Tetrabromobisphenol A epoxy resin (TBBPAER) is the main non-metallic component of electronic waste. The scale of electronic waste production and the accompanying TBBPAER waste disposal problems represent a great opportunity for chemical upcycling. But the chemical upcycling of TBBPAER faces great challenges due to its high bromine content and thermally stability. In this study, a subcritical water ammonia (SWA) process combined with waste copper-based catalyst (WCC) selectively converted TBBPAER in high yields (63.46 % at 300°C for 15 min and 73.66 % for 60 min) to low molecular-weight liquid products including high value-added methyl pyrimidine and phenols. The electron transfer among multivalent copper species contained in the WCC promoted the production of free radicals OH, O2, NH2, and :NH, which resulted in the efficient conversion of TBBPAER and a 99.29 % of debromination ratio. The molecular chain of TBBPAER was snipped by OH and NH2 to produce tetrabromobisphenol A groups (TAG) and ternary carbon groups (TCG). The further degradation of TAG resulted in the producing of phenol chemicals with a purity of 91.8 % (GC peak area%). The further cyclization of TCG induced by :NH produced methyl pyrimidine with a purity of 91.9 % (GC peak area%). The formation of copper ammonia complex led to the leaching/recovery of 86.6 % of copper from the WCC. The SWA-WCC approach demonstrated how TBBPAER waste could be a viable feedstock for the producing of high value-added methyl pyrimidine and phenol chemicals. This study provided a novel sustainable strategy for synchronous treatment/upcycling of the two different wastes of TBBPAER and WCC. The leaching toxicity test of Cu and Zn for the solid residue after the co-treatment showed that their leaching concentrations were much lower than the hazardous waste standard.
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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