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水热碱处理后废颗粒活性炭用于去除全氟和多氟烷基物质的再利用。

Reuse of spent granular activated carbon for PFAS removal following hydrothermal alkaline treatment.

作者信息

Soker Ori, Tajdini Bahareh, Abarca-Perez Angela, Wadia Aaditi, Bellona Christopher, Hao Shilai, Doudrick Kyle, Strathmann Timothy J

机构信息

Department of Civil and Environmental Engineering, Colorado School of Mines, Golden, CO 80401, USA.

Department of Civil and Environmental Engineering and Earth Sciences, University of Notre Dame, Notre Dame, IN 46556, USA.

出版信息

Water Res. 2025 Sep 1;283:123794. doi: 10.1016/j.watres.2025.123794. Epub 2025 May 8.

Abstract

Per- and polyfluoroalkyl substances (PFAS) pose a significant challenge for water treatment facilities facing strict regulatory standards. Granular activated carbon (GAC) adsorption is effective for PFAS removal, but media exhaustion and replacement can be costly, highlighting the need for innovative GAC regeneration methods. While thermal reactivation of GAC can eliminate adsorbed PFAS, it requires high temperatures and is mainly feasible for large-scale media users. This study investigates spent GAC regeneration by hydrothermal alkaline treatment (HALT), which applies subcritical water (e.g., 350 °C, 16.5 MPa) amended with strong base (e.g., NaOH) to destroy PFAS. Previous research indicates that HALT successfully degraded and defluorinated PFAS while maintaining GAC surface area and equilibrium adsorption capacity. This study presents data from rapid small-scale column tests (RSSCTs) demonstrating effective removal of long-chain PFAS by a HALT-treated spent GAC sample collected from a long-term PFAS treatment field pilot study (BV > 50,000 for PFOS, PFHxS, and PFNA). HALT-treated virgin GAC and untreated virgin GAC evaluated using RSSCTs exhibited similar PFAS breakthrough behavior, with comparable overall PFAS removal to the HALT-treated spent GAC. Physisorption measurements revealed that HALT recovers GAC pore surface area lost during field-use. Surface chemical characterization techniques indicated mostly similar surface composition and functional groups in virgin and HALT-treated GAC, with limited change in the carbon structure following HALT and differences between virgin and field-spent samples. Analyses of reactor liquid products, media mass loss, and NaOH neutralization by GAC also provided evidence for removal of adsorbed non-target organic matter and possible GAC surface renewal by carbon gasification reactions occurring in parallel with PFAS destruction, analogous to surface carbon burn-off that occurs during high-temperature thermal reactivation. Retention of adsorbed metal ions that accumulated on the spent GAC during field testing may be responsible for enhanced adsorption behavior observed for some PFAS following HALT regeneration. Results indicate that HALT can enable reuse of spent GAC, potentially alleviating the high demand for virgin media in PFAS treatment processes.

摘要

全氟和多氟烷基物质(PFAS)给面临严格监管标准的水处理设施带来了重大挑战。颗粒活性炭(GAC)吸附对去除PFAS有效,但介质耗尽和更换成本高昂,这凸显了创新GAC再生方法的必要性。虽然GAC的热再活化可以消除吸附的PFAS,但它需要高温,并且主要适用于大规模介质用户。本研究调查了通过水热碱处理(HALT)对废GAC进行再生,该方法使用用强碱(如NaOH)改性的亚临界水(如350°C,16.5 MPa)来破坏PFAS。先前的研究表明,HALT成功地降解了PFAS并使其脱氟,同时保持了GAC的表面积和平衡吸附容量。本研究展示了快速小规模柱试验(RSSCT)的数据,证明从长期PFAS处理现场中试研究收集的经HALT处理的废GAC样品能有效去除长链PFAS(对于全氟辛烷磺酸、全氟己烷磺酸和全氟萘酸,BV>50,000)。使用RSSCT评估的经HALT处理的原始GAC和未经处理的原始GAC表现出相似的PFAS穿透行为,总体PFAS去除效果与经HALT处理的废GAC相当。物理吸附测量表明,HALT恢复了在现场使用期间损失的GAC孔表面积。表面化学表征技术表明,原始GAC和经HALT处理的GAC的表面组成和官能团大多相似,HALT后碳结构变化有限,且原始样品和现场使用后的样品之间存在差异。对反应器液体产物、介质质量损失以及GAC对NaOH的中和作用的分析也提供了证据,证明去除了吸附的非目标有机物,并且与PFAS破坏同时发生的碳气化反应可能使GAC表面更新,类似于高温热再活化过程中发生的表面碳烧失。在现场测试期间积累在废GAC上的吸附金属离子的保留可能是导致HALT再生后某些PFAS吸附行为增强的原因。结果表明,HALT可以使废GAC得以再利用,有可能缓解PFAS处理过程中对原始介质的高需求。

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