Calix[4]resorcinarenes as Stable, Metal-Free Unexplored and Unfathomed Material for Iodine Capture: Experimental and Theoretical Insights

IF 2.9 Q2 PUBLIC, ENVIRONMENTAL & OCCUPATIONAL HEALTH ACS Chemical Health & Safety Pub Date : 2024-09-11 DOI:10.1021/acs.chas.4c00037
Gopika Jagannivasan, Jayasree G Elambalassery, Suja Haridas
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Abstract

While nuclear power offers a viable solution to the ever-growing energy demands, the piling up of nuclear waste remains a looming threat, endangering life on Earth. Safe disposal of radionuclides, especially highly volatile ones such as iodine, is a grave concern to be addressed for operational safety. Even though porous adsorbents for iodine capture have been widely investigated, less focus has been directed toward nonporous materials. Herein, we describe the synthesis of nonporous, macrocyclic Calix[4]resorcinarenes (C4Rs) via a near solventless green protocol mediated by Keggin-type phosphovanadotungstic acid and avoiding the use of mineral acids. The applicability of the synthesized C4Rs for iodine absorption at elevated temperatures has been explored. Facile synthesis strategy and metal-free nature coupled with moisture and temperature stability endorse our interest in C4Rs as highly attractive substrates for iodine sorption, with the substituent functionalities playing an important role in adsorption efficiency. We hereby report a novel C4R, DEAS, with an exceptional iodine sorption capability. The retention of iodine in the macrocyclic framework, mainly in the form of polyiodides, could be ascertained through a detailed characterization. The adsorption was found to follow pseudo-second-order kinetics. The adsorption of iodine from an aqueous solution was also subjected to investigation. Furthermore, theoretical investigation into the guest–host interactions between C4Rs and I2 has been attempted for better insights.

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钙并[4]间苯二酚作为稳定的、不含金属的、未探索和未知的碘俘获材料:实验和理论启示
虽然核能为日益增长的能源需求提供了可行的解决方案,但核废料的堆积仍然是一个迫在眉睫的威胁,危及地球上的生命。安全处置放射性核素,尤其是碘等高挥发性放射性核素,是确保运行安全的一个严重问题。尽管用于碘捕获的多孔吸附剂已被广泛研究,但对无孔材料的关注却较少。在本文中,我们介绍了通过一种近乎无溶剂的绿色方案,在凯金型磷钒钨酸的介导下,避免使用矿物酸,合成无孔大环钙[4]间苯二酚(C4Rs)的过程。研究人员探索了合成的 C4Rs 在高温下吸收碘的适用性。简便的合成策略和无金属特性以及湿度和温度稳定性使我们对 C4Rs 作为极具吸引力的碘吸附基质产生了浓厚的兴趣,而取代基的官能度在吸附效率方面起着重要作用。我们在此报告一种新型 C4R--DEAS,它具有卓越的碘吸附能力。碘在大环框架中的保留主要以聚碘化物的形式存在,这一点可以通过详细的表征来确定。研究发现,吸附过程遵循伪二阶动力学。此外,还对水溶液中碘的吸附进行了研究。此外,还尝试对 C4Rs 和 I2 之间的客体-主体相互作用进行理论研究,以获得更好的见解。
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ACS Chemical Health & Safety
ACS Chemical Health & Safety PUBLIC, ENVIRONMENTAL & OCCUPATIONAL HEALTH-
CiteScore
3.10
自引率
20.00%
发文量
63
期刊介绍: The Journal of Chemical Health and Safety focuses on news, information, and ideas relating to issues and advances in chemical health and safety. The Journal of Chemical Health and Safety covers up-to-the minute, in-depth views of safety issues ranging from OSHA and EPA regulations to the safe handling of hazardous waste, from the latest innovations in effective chemical hygiene practices to the courts'' most recent rulings on safety-related lawsuits. The Journal of Chemical Health and Safety presents real-world information that health, safety and environmental professionals and others responsible for the safety of their workplaces can put to use right away, identifying potential and developing safety concerns before they do real harm.
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