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Reaction mechanism of hexavalent chromium with cellulose, hemicellulose, chitin and lignin
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Biomaterials and their degraded derivatives in nature (i.e., natural organic matter, NOM) play a critical role in reducing toxic Cr(VI) to less toxic Cr(III) in the environment. Because of the complicated compositions of these materials, the mechanism of Cr(VI) reaction with these materials have not been fully understood. Therefore, the aims of this work were to investigate the reaction mechanisms of Cr(VI) with cellulose, hemicellulose, chitin and lignin, which are the major components of NOM and biomaterials. The materials before and after Cr(VI) reaction were analyzed using FTIR and Cr K-edge XAS to identify the functional groups governing Cr(VI) reduction and the oxidation state and local structure of Cr bound to the materials, respectively. The results showed that the Cr(VI) was sorbed and reduced to Cr(III) on the surfaces of hemicellulose, chitin and lignin, while sorption and reduction of Cr(VI) on cellulose were not noticeable. The Cr K-edge XAS results indicated that Cr(III) resulting from Cr(VI) reduction is bound to the surfaces through surface complexation and precipitation. The reaction of the materials with Cr(VI) resulted in the formation of carbonyl and carboxyl groups on the surfaces of these materials, which subsequently provide binding sites for the resultant Cr(III). The results of this work will be helpful in clarifying the mechanisms of Cr(VI) reactions with NOM and biomaterials and understanding the roles of these materials in the fate of Cr(VI) in the environment.
由於Cr(VI)具有高毒性及致癌性，經由工業廢水排放後容易淋洗至深層的土壤與地下水中，對於人體與環境有極大的危害。土壤有機質與有機資材已被證實能夠使Cr(VI)還原成毒性危害較低的Cr(III)。然而其組成均相當複雜，不易釐清個別組成與Cr(VI)之間的作用機制。因此本研究利用有機資材中的主要成分─纖維素、半纖維素、木質素以及幾丁質，探討其對溶液中Cr(VI)的反應速率，並利用FTIR分析反應後的官能基之變化以推論參與反應之官能基為何，利用Cr K-edge XAS光譜分析鉻在固體上的氧化價數以及鉻與周圍原子的鍵結情形，以進一步推論纖維素、半纖維素、木質素和幾丁質對Cr(VI)反應之機制。結果顯示，半纖維素、幾丁質和木質素能夠吸附Cr(VI)，並將Cr(VI)還原成Cr(III)，而纖維素對Cr(VI)的吸附及還原能力則不顯著。利用Cr K-edge XAS分析發現還原後的Cr(III)能夠同時以錯合物及表面沉澱的方式鍵結在固體表面。由FTIR測定反應前後官能基變化可知Cr(VI)還原的同時造成吸附劑表面產生-C=O與-COOH的增加，而這些官能基進一步提供還原後的Cr(III)鍵結之位置。
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