Abstract
To facilitate removing As(III) from water through an “oxidation-adsorption” process, the double-shell CuOx@MnOy hollow spheres (DCMHS) have been fabricated via a two-step co-precipitation route combined with the soft-template method. The surface characterization results showed that Mn oxides were formed without segregation and uniformly distributed on the surface of CuOx hollow spheres. DCMHS could achieve outstanding performance to remove As(III) with an As maximum adsorption capacity of 32.15 mg/g. Meanwhile, the kinetics results illustrated that the oxidative activity of DCMHS was strengthened due to its specific structure, and part of As(III) was converted to As(V) during the adsorption process. Also, air aeration could further enhance As(III) oxidation and thus improving As removal. The As(III) removal performance could be maintained under neutral and weak alkaline conditions. Phosphate, silicate, and carbonate anions could depress the removal performance, while chloride ions and sulfate anions barely influenced As removal. Moreover, DCMHS could be regenerated using NaOH and KMnO4 solutions without breaking the hollow sphere structure. Based on the spectroscopic analysis results, As(III) molecules were converted to As(V) via two pathways, including the oxidation by Mn oxides or superoxide radicals. The Cu–Mn synergistic effect could not only enhance the oxidative activity of Mn oxides but also produce superoxide radicals via the activation of surface-adsorbed oxygen molecules. Afterwards, the newly formed As(V) could be attached to the hydroxyl groups through surface complexation. Therefore, this work has provided insights into the morphology design of Mn-oxide-containing adsorbents and supplemented the interface reaction mechanisms for enhancing As(III) removal.
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This work was financially supported by the National Key Research and Development Program of China, China (Grant No. 2019YFD1100102-04), the National Natural Science Foundation of China, China (Grant No. 51578440/51808512), the Key Research and Development Project of Shaanxi Province, China (Grant No. 2019ZDLSF05-03/2021ZDLSF05-06), the Science and Technology Program Project of Jiangxi Provincial Department of Water Resources (202022YBKT17), and the New Style Think Tank of Shaanxi Universities, China.
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Kun Wu contributed to the conception and the funding of the study. Birong Miao and Yang Li performed the experiment. Kun Wu performed the data analyses and wrote the manuscript. Birong Miao, Yuyang Xiao, and Chuanqiao Zhang contributed significantly to analysis and manuscript preparation. Ting Liu, Shengjiong Yang, and Jinfu Liu helped perform the analysis with constructive discussions.
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Wu, K., Miao, B., Xiao, Y. et al. The enhanced removal of arsenite from water by double-shell CuOx@MnOy hollow spheres (DCMHS): behavior and mechanisms. Environ Sci Pollut Res 29, 76417–76431 (2022). https://doi.org/10.1007/s11356-022-20702-3
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DOI: https://doi.org/10.1007/s11356-022-20702-3