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热解温度对生物炭还原 Cr(VI)的供电子和介导机制的影响。

Pyrolysis-temperature depended electron donating and mediating mechanisms of biochar for Cr(VI) reduction.

机构信息

School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.

School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.

出版信息

J Hazard Mater. 2020 Apr 15;388:121794. doi: 10.1016/j.jhazmat.2019.121794. Epub 2019 Nov 30.

Abstract

Biochar could be involved in environmentally relevant redox reactions, and their redox-active moieties may change with pyrolysis temperature. In this study, pyrolysis-temperature depended electron donating and mediating ability of biochar for Cr(VI) reduction were evaluated. All biochar derived from peanut shell at 400-800 °C effectively reduced Cr(VI) into Cr(III), and the reduction capability decreased as the pyrolysis temperature increased (400-600 °C), and then increased (600-800 °C). The electron donating moieties transformed from the -OH functional groups at lower pyrolysis temperature (<600 °C) to the functional groups associated with conjugated structure at higher temperature (>600 °C). Biochar could mediate the reduction of Cr(VI) by lactate, with the reduction rates of Cr(VI) increased up to 16.3 and 345 times that by either biochar or lactate alone, respectively. The redox ability of biochar was the premise, but its conductivity was the dominant factor, for the mediating reduction of Cr(VI). The mediation capability of biochar increased with elevated pyrolysis-temperature due to its increased conductivity related to the growth of conjugated clusters and carbon defects. Our results indicated that pyrolysis-temperature affects the formation of functional groups and conjugated carbon structure of biochars which have a distinguishable influence on the electron donating and mediating ability for Cr(VI) reduction.

摘要

生物炭可能参与环境相关的氧化还原反应,其氧化还原活性基团可能随热解温度而变化。在这项研究中,评估了生物炭在热解温度依赖性下对 Cr(VI)还原的供电子和介导能力。所有源自于花生壳的生物炭在 400-800°C 下均能有效将 Cr(VI)还原为 Cr(III),且还原能力随热解温度升高而降低(400-600°C),随后升高(600-800°C)。在较低的热解温度(<600°C)下,供电子基团由-OH 官能团转变为与高温(>600°C)下共轭结构相关的官能团。生物炭可以介导乳酸盐还原 Cr(VI),Cr(VI)的还原速率分别提高了 16.3 倍和 345 倍,是生物炭或乳酸盐单独作用的还原速率。生物炭的氧化还原能力是介导还原 Cr(VI)的前提,但导电性是主要因素。由于共轭簇和碳缺陷的增加与导电性相关,生物炭的热解温度升高会增加其介导还原能力。研究结果表明,热解温度会影响生物炭的官能团形成和共轭碳结构,这对 Cr(VI)还原的供电子和介导能力有明显影响。

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