Using Ultramicroporous Carbon for the Selective Removal of Nitrate with Capacitive Deionization

被引:138
作者
Hawks, Steven A. [1 ]
Ceron, Maira R. [1 ]
Oyarzun, Diego I. [2 ]
Tuan Anh Pham [1 ]
Zhan, Cheng [1 ]
Loeb, Colin K. [1 ]
Mew, Daniel [1 ]
Deinhart, Amanda [1 ]
Wood, Brandon C. [1 ]
Santiago, Juan G. [2 ]
Stadermann, Michael [1 ]
Campbell, Patrick G. [1 ]
机构
[1] Lawrence Livermore Natl Lab, 7000 East Ave, Livermore, CA 94550 USA
[2] Stanford Univ, Dept Mech Engn, Stanford, CA 94305 USA
关键词
1ST-PRINCIPLES MOLECULAR-DYNAMICS; ELECTRICAL DOUBLE-LAYER; MICROPOROUS CARBONS; PORE-SIZE; ION SIZE; WATER DESALINATION; HYDRATED RADIUS; FREE-ENERGY; ADSORPTION; ELECTROSORPTION;
D O I
10.1021/acs.est.9b01374
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The contamination of water resources with nitrate is a growing and significant problem. Here we report the use of ultramicroporous carbon as a capacitive deionization (CDI) electrode for selectively removing nitrate from an anion mixture. Through moderate activation, we achieve a micropore-size distribution consisting almost exclusively of narrow (<1 nm) pores that are well suited for adsorbing the planar, weakly hydrated nitrate molecule. Cyclic voltammetry measurements reveal an enhanced capacitance for nitrate when compared to chloride as well as significant ion sieving effects when sulfate is the only anion present. We measure high selectivities (S) of both nitrate over sulfate (S-NO3/SO4 = 17.8 +/- 3.6 at 0.6 V) and nitrate over chloride (S-NO3/Cl = 6.1 +/- 0.4 at 0.6 V) when performing a constant voltage CDI separation on 3.33 mM/3.33 mM/1.67 mM Cl/NO3/SO4 feedwater. These results are particularly encouraging considering that a divalent interferant was present in the feed. Using molecular dynamics simulations, we examine the solvation characteristics of these ions to better understand why nitrate is preferentially electrosorbed over sulfate and chloride.
引用
收藏
页码:10863 / 10870
页数:8
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