Kx[Bi4–xMnxS6], Design of a Highly Selective Ion Exchange Material and Direct Gap 2D Semiconductor
- Ruiqi WangRuiqi WangBeijing National Laboratory for Molecular Sciences and State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. ChinaMore by Ruiqi Wang,
- Haijie ChenHaijie ChenDepartment of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United StatesMore by Haijie Chen,
- Yi XiaoYi XiaoBeijing National Laboratory for Molecular Sciences and State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. ChinaMore by Yi Xiao,
- Ido HadarIdo HadarDepartment of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United StatesMore by Ido Hadar,
- Kejun BuKejun BuCAS Key Laboratory of Materials for Energy Conversion and State Key Laboratory of High-Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, P. R. ChinaMore by Kejun Bu,
- Xian ZhangXian ZhangQian Xuesen Laboratory of Space Technology, China Academy of Space Technology, Beijing 100094, P. R. ChinaMore by Xian Zhang,
- Jie PanJie PanCAS Key Laboratory of Materials for Energy Conversion and State Key Laboratory of High-Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, P. R. ChinaMore by Jie Pan,
- Yuhao GuYuhao GuBeijing National Laboratory for Molecular Sciences and State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. ChinaMore by Yuhao Gu,
- Zhongnan GuoZhongnan GuoDepartment of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United StatesMore by Zhongnan Guo,
- Fuqiang Huang*Fuqiang Huang*[email protected]Beijing National Laboratory for Molecular Sciences and State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. ChinaCAS Key Laboratory of Materials for Energy Conversion and State Key Laboratory of High-Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, P. R. ChinaMore by Fuqiang Huang, and
- Mercouri G. Kanatzidis*Mercouri G. Kanatzidis*[email protected]Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United StatesMore by Mercouri G. Kanatzidis
Abstract
Layered sulfides with high selectivity for binding heavy metal ions and radionuclide ions are promising materials in effluent treatment and water purification. Here we present a rationally designed layered sulfide Kx[Bi4–xMnxS6] (x = 1.28) deriving from the Bi2Se3-structure type by targeted substitution to generate quintuple [Bi4–xMnxS6]x− layers and K+ cations between them. The material has dual functionality: it is an attractive semiconductor with a bandgap of 1.40 eV and also an environmental remediation ion-exchange material. The compound is paramagnetic, and optical adsorption spectroscopy and DFT electronic structure calculations reveal that it possesses a direct band gap and a work function of 5.26 eV. The K+ ions exchange readily with alkali or alkaline-earth ions (Rb+, Cs+, and Sr2+) or soft ions (Pb2+, Cd2+, Cr3+, and Zn2+). Furthermore, when the K+ ions are depleted the Mn2+ ions in the Bi2Se3-type slabs can also be replaced by soft ions, achieving large adsorption capacities. The ion exchange reactions of Kx[Bi4–xMnxS6] can be used to create new materials of the type Mx[Bi4–xMnxS6] in a low temperature kinetically controlled manner with significantly different electronic structures. The Kx[Bi4–xMnxS6] (x = 1.28) exhibits efficient capture of Cd2+ and Pb2+ ions with high distribution coefficient, Kd (107 mL/g), and exchange capacities of 221.2 and 342.4 mg/g, respectively. The material exhibits excellent capacities even in high concentration of competitive ions and over a broad pH range (2.5–11.0). The results highlight the promise of the Kx[Bi4–xMnxS6] (x = 1.28) phase to serve not only as a highly selective adsorbent for industrial and nuclear wastewater but also as a magnetic 2D semiconductor for optoelectronic applications.
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