废聚酰亚胺中的半导体金属有机框架同时实现太阳能驱动的界面蒸发和光-芬顿氧化作用

IF 13 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Energy & Environmental Materials Pub Date : 2024-08-01 DOI:10.1002/eem2.12812
Lijie Liu, Huajian Liu, Zifen Fan, Jie Liu, Xueying Wen, Huiyue Wang, Yan She, Guixin Hu, Ran Niu, Jiang Gong
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引用次数: 0

摘要

界面太阳能蒸汽发生和光-芬顿氧化的集成技术已成为同时缓解淡水匮乏和降解有机污染物的一种有前途的方法。然而,制造具有高水蒸发和催化能力的低成本多功能蒸发器仍是一项重大挑战。在此,我们报告了将废弃聚酰亚胺转化为半导体 Fe-BTEC 的功能性升级再循环方法,并随后构建了基于 Fe-BTEC 的复合蒸发器,用于同时生产淡水和光-芬顿降解污染物。首先,通过溶热-溶液搅拌两步法,从废聚酰亚胺中大量制备出 20-100 nm 大小的 Fe-BTEC 纳米颗粒,其带隙能为 2.2 eV。基于 Fe-BTEC 和石墨烯的复合蒸发器具有宽太阳光谱吸收能力、高光热转换能力、快速输水和低蒸发焓等特点。得益于上述优点,该复合蒸发器从四环素溶液中实现了 2.72 kg m-2 h-1 的高蒸发率,在 1 个太阳光照射下的光热转换效率高达 97%,优于许多蒸发器。此外,该蒸发器的四环素降解率高达 99.6%,且具有良好的回收稳定性,是功能最强大的异相芬顿催化剂之一。COMSOL 多物理场和密度泛函理论计算结果证明,界面太阳能蒸汽产生的聚热与 Fe-BTEC 的催化活性位点在促进 H2O2 活化形成活性氧化自由基方面具有协同效应。这项工作不仅为废旧聚酰亚胺的升级再利用提供了一种绿色策略,还为制造多功能蒸发器提出了一种新方法。
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Simultaneous Solar-Driven Interfacial Evaporation and Photo-Fenton Oxidation by Semiconducting Metal–Organic Framework From Waste Polyimide
The integrated technology of interfacial solar steam generation and photo-Fenton oxidation has emerged as a promising way to simultaneously mitigate freshwater scarcity and degrade organic pollutants. However, fabricating low-cost, multi-functional evaporators with high water evaporation and catalytic ability still presents a significant challenge. Herein, we report the functional upcycling of waste polyimide into semiconducting Fe-BTEC and subsequently construct Fe-BTEC-based composite evaporators for simultaneous freshwater production and photo-Fenton degradation of pollutants. Firstly, through a two-step solvothermal-solution stirring method, Fe-BTEC nanoparticles with the size of 20–100 nm are massively produced from waste polyimide, with a band gap energy of 2.2 eV. The composite evaporator based on Fe-BTEC and graphene possesses wide solar-spectrum absorption capacity, high photothermal conversion capacity, rapid delivery of water, and low enthalpy of evaporation. Benefiting from the merits above, the composite evaporator achieves a high evaporation rate of 2.72 kg m−2 h−1 from tetracycline solution, as well as the photothermal conversion efficiency of 97% when exposed to irradiation of 1 Sun, superior to many evaporators. What is more, the evaporator exhibits the tetracycline degradation rate of 99.6% with good recycling stability, ranking as one of the most powerful heterogeneous Fenton catalysts. COMSOL Multiphysics and density functional theory calculation results prove the synergistic effect of the concentrated heat produced by interfacial solar steam generation and catalytic active sites of Fe-BTEC on promoting H2O2 activation to form reactive oxidation radicals. This work not only provides a green strategy for upcycling waste polyimide, but also proposes a new approach to fabricate multi-functional evaporators.
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来源期刊
Energy & Environmental Materials
Energy & Environmental Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
17.60
自引率
6.00%
发文量
66
期刊介绍: Energy & Environmental Materials (EEM) is an international journal published by Zhengzhou University in collaboration with John Wiley & Sons, Inc. The journal aims to publish high quality research related to materials for energy harvesting, conversion, storage, and transport, as well as for creating a cleaner environment. EEM welcomes research work of significant general interest that has a high impact on society-relevant technological advances. The scope of the journal is intentionally broad, recognizing the complexity of issues and challenges related to energy and environmental materials. Therefore, interdisciplinary work across basic science and engineering disciplines is particularly encouraged. The areas covered by the journal include, but are not limited to, materials and composites for photovoltaics and photoelectrochemistry, bioprocessing, batteries, fuel cells, supercapacitors, clean air, and devices with multifunctionality. The readership of the journal includes chemical, physical, biological, materials, and environmental scientists and engineers from academia, industry, and policy-making.
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