Interactive impacts of organic-inorganic modifiers on surface characteristics of Cu+-doped activated carbon for stable CO-adsorptive separation from CO2

被引:2
作者
Win, May Zaw [1 ]
Park, Ji Hye [2 ]
Oo, Wathone [1 ]
San, Thu Zar [1 ]
Ugli, Lapasov Shokhjakhon Dilshod [1 ]
Son, Chaerin [3 ]
Kim, Minkyu [3 ]
Yi, Kwang Bok [2 ]
机构
[1] Chungnam Natl Univ, Grad Sch Energy Sci & Technol, 99 Daehak Ro, Daejeon 34134, South Korea
[2] Chungnam Natl Univ, Dept Chem Engn Educ, 99 Daehak Ro, Daejeon 34134, South Korea
[3] Yeungnam Univ, Sch Chem Engn, 280 Daehak Ro, Daegu 38541, Gyeongsan, South Korea
关键词
Carbon monoxide; Selectivity; Stabilization; Surface modification; MOLECULAR-DYNAMICS; BOEHMITE; TRANSFORMATION; ACETONITRILE; SELECTIVITY; DISPERSION; COMPLEXES; OXIDATION; CHEMISTRY; CATALYSTS;
D O I
10.1016/j.seppur.2024.130065
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Conventional Cu+-doped activated carbon (C) materials are problematic in carbon monoxide (CO)-selective adsorption from carbon dioxide (CO2) due to their CO2-friendly surface basicity and microporosity. In this study, boehmite (AlOOH) film modified-carbon composite (AlC) was hydrothermally synthesized to dope with 30 wt% Cu+ ions by the impregnation-calcination method. The functional hydroxyl groups of Boehmite behaved as metallic anchoring sites for better Cu+ ion dispersion, enhancing the CO adsorption uptake to 38.84 cm(3)/g at 25 degrees C and similar to 100 kPa in isotherm analysis. Additionally, the improved Lewis acidity of AlC surface interface together with pore widening impact reduced the CO2 uptake to 14 cm(3)/g, around half that of Cu+-doped activated carbon, by undergoing Lewis acid-acid repelling interaction between boehmite film and CO2. However, to address rapid oxidation of Cu+ ions in the hygroscopic AlC structure, iron (II) chloride (FeCl2) surface modification on the Cu+-doped AlC composite created a Fe3+-Cu+ bimetallic interface with high Cu+ immobilization, enriching the CO adsorption stability to 92 % even after 30 day-air exposure. Noticeably, pre-complexation of FeCl2 with thiourea (NH2CSNH2) before its dispersion over the doped Cu+ ions led to distinct Cu+ stabilization mechanisms without bimetallic redox interaction. This involves developing auto-redoxable iron (II) sulfides as barrier coatings for Cu+ species against oxidation and raising the Cu2+ reducibility via cyanide-ligands of thiourea. These combined preservation effects for Cu+ ions ensured CO adsorption stability of 91 %, underlining higher CO adsorption uptake (39.38 cm(3)/g) and CO/CO2 selectivity (67.49 at 0.2 kPa and 3.09 at similar to 100 kPa) than modification effects of boehmite and FeCl2.
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页数:19
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