Ion-Exchangeable Molybdenum Sulfide Porous Chalcogel: Gas Adsorption and Capture of Iodine and Mercury
Ion-Exchangeable Molybdenum Sulfide Porous Chalcogel: Gas Adsorption and Capture of Iodine and Mercury
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DOI：
10.1021/jacs.5b09110
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发表时间：
2015-11-04
影响因子：
15
通讯作者：
Kanatzidis, Mercouri G.
中科院分区：
文献类型：
--
作者：
Subrahmanyam, Kota S.;Malliakas, Christos D.;Kanatzidis, Mercouri G.
本文报道了以（NH_4）（2）MoS_4和碘为原料，通过氧化偶联法合成可交换硫化钼硫凝胶。超临界干燥后，MoSx无定形气凝胶显示出高达370 m2/g的大比表面积和宽范围的孔径。X射线光电子能谱和对分布函数分析表明，Mo 6+物种在网络组装过程中发生还原，产生含Mo 4+的物种，其中硫族凝胶网络由[Mo 3S 13]结构单元组成，该结构单元包含三角形Mo金属簇和S-2（2-）单元。棕黑色硫凝胶的光学带隙类似于1.36eV。存在于硫化钼硫凝胶网络中的铵位点可与K+和Cs+离子进行离子交换。硫化钼气凝胶对CO2和C2 H6的吸附选择性高于对H2和CH 4的吸附选择性。该气凝胶还具有对碘和汞的高亲和力。
We report the synthesis of ion-exchangeable molybdenum sulfide chalcogel through an oxidative coupling process, using (NH4)(2)MoS4 and iodine. After supercritical drying, the MoSx amorphous aerogel shows a large surface area up to 370 m(2)/g with a broad range of pore sizes. X-ray photoelectron spectroscopic and pair distribution function analyses reveal that Mo6+ species undergo reduction during network assembly to produce Mo4+-containing species where the chalcogel network consists of [Mo3S13] building blocks comprising triangular Mo metal clusters and S-2(2-) units. The optical band gap of the brown-black chalcogel is similar to 1.36 eV. The ammonium sites present in the molybdenum sulfide chalcogel network are ion-exchangeable with K+ and Cs+ ions. The molybdenum sulfide aerogel exhibits high adsorption selectivities for CO2 and C2H6 over H-2 and CH4. The aerogel also possesses high affinity for iodine and mercury.