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Distinct roles of pH and organic ligands in the dissolution of goethite by cysteine

Journal of Environmental Sciences 2022年第3期34卷 260-268页

作者： Ji Li Chenlu Shi Wenbin Zeng Yaru Wang Zebin Hong Yibing Ma Liping Fang Faculty of Material Sciences and Chemistry China University of GeosciencesWuhan 430074China Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management Institute of Eco-environmental and Soil SciencesGuangdong Academy of SciencesGuangzhou 510650China National-Regional Joint Engineering Research Center for Soil Pollution Control and Remediation in South China Guangzhou 520650China Macao Environmental Research Institute Macao University of Science and TechnologyTaipa 999078MachaoChina

Electron shuttles such cysteine play an important role in Fe cycle and its availability in soils,while the roles of pH and organic ligands in this process are poorly understood.Herein,the reductive dissolution process of goethite by cysteine were explored in the presence of organic ligands.Our results showed that cysteine exhibited a strong reactivity towards goethite-a typical iron minerals in paddy soils with a rate constant ranging from 0.01 to0.1 hr^(-1).However,a large portion of Fe(Ⅱ) appeared to be "structural species" retained on the surface.The decline of pH was favorable to generate more Fe(Ⅱ) ions and enhancing tendency of Fe(Ⅱ) release to solution.The decline of generation of Fe(Ⅱ) by increasing pH was likely to be caused by a lower redox potential and the nature of cysteine pH-dependent adsorption towards goethite.Interestingly,the co-existence of oxalate and citrate ligands also enhanced the rate constant of Fe(Ⅱ) release from 0.09 to 0.15 hr-1;nevertheless,they negligibly affected the overall generation of Fe(Ⅱ) in opposition to the pH effect.Further spectroscopic evidence demonstrated that two molecules of cysteine could form disulfide bonds(S-S) to generate cystine through oxidative dehydration,and subsequently,inducing electron transfer from cysteine to the structural Fe(Ⅲ) on goethite;meanwhile,those organic ligands act as Fe(Ⅱ) "strippers".The findings of this work provide new insights into the understanding of the different roles of pH and organic ligands on the generation and release of Fe induced by electron shuttles in soils.

关键词： Electron transfer reductive dissolution Iron cycling Organic ligands

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