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可持续生物质在亚临界水热过程中作为 Cr(VI)还原的电子供体:水热炭和液体化合物作用的分子见解。

Sustainable Biomass Acts as an Electron Donor for Cr(VI) Reduction during the Subcritical Hydrothermal Process: Molecular Insights into the Role of Hydrochar and Liquid Compounds.

机构信息

Shanghai Technical Service Platform for Pollution Control and Resource Utilization of Organic Wastes, Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, Shanghai 200438, China.

State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, China.

出版信息

Environ Sci Technol. 2024 Sep 3;58(35):15855-15863. doi: 10.1021/acs.est.4c05488. Epub 2024 Aug 20.

Abstract

Heavy metal pollution is a critical environmental issue that has garnered significant attention from the international community. Subcritical hydrothermal liquefaction (HTL) as an emerging green technology has demonstrated remarkable promise in environmental remediation. However, there is limited research on the remediation of highly toxic Cr(VI) using HTL. This study reveals that the HTL reaction of biomass enables the simultaneous reduction and precipitation of Cr(VI). At 280 °C, the reduction of Cr(VI) was nearly complete, with a high reduction rate of 98.9%. The reduced Cr as Cr(OH) and CrO was primarily enriched in hydrochar, accounting for over 99.9% of the total amount. This effective enrichment resulted in the removal of Cr(VI) from the aqueous phase while simultaneously yielding clean liquid compounds like organic acids and furfural. Furthermore, the elevated temperature facilitated the formation of Cr(III) and enhanced its accumulation within hydrochar. Notably, the resulting hydrochar and small oxygenated compounds, especially aldehyde, served as electron donors for Cr(VI) reduction. Additionally, the dissolved Cr facilitated the depolymerization and deoxygenation processes of macromolecular compounds with lignin-like structures, leading to more small oxygenated compounds and subsequently influencing Cr(VI) reduction. These findings have substantial implications for green and sustainable development.

摘要

重金属污染是一个严峻的环境问题,引起了国际社会的高度关注。亚临界水热液化(HTL)作为一种新兴的绿色技术,在环境修复方面显示出了巨大的潜力。然而,利用 HTL 修复高毒性 Cr(VI)的研究还很有限。本研究表明,生物质的 HTL 反应能够实现 Cr(VI)的同时还原和沉淀。在 280°C 下,Cr(VI)的还原几乎完全,还原率高达 98.9%。还原后的 Cr 以 Cr(OH)和 CrO 的形式主要富集在水热炭中,占总量的 99.9%以上。这种有效的富集作用将 Cr(VI)从水相中去除,同时生成了清洁的液体化合物,如有机酸和糠醛。此外,高温有利于 Cr(III)的形成,并促进其在水热炭中的积累。值得注意的是,生成的水热炭和小分子含氧化合物,特别是醛,充当了 Cr(VI)还原的电子供体。此外,溶解的 Cr 促进了具有木质素样结构的大分子化合物的解聚和脱氧过程,导致更多的小分子含氧化合物生成,从而影响 Cr(VI)的还原。这些发现对绿色可持续发展具有重要意义。

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