Fabrication of bimetallic Cu–Zn adsorbents with high dispersion by using confined space for gas adsorptive separation
Yu-Chao Wang, Tian-Tian Li, Li Huang, Xiao-Qin Liu, Lin-Bing Sun()
State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China
The number of active components and their dispersion degree are two key factors affecting the performance of adsorbents. Here, we report a simple but efficient strategy for dispersing active components by using a confined space, which is formed by mesoporous silica walls and templates in the as-prepared SBA-15 (AS). Such a confined space does not exist in the conventional support, calcined SBA-15, which does not contain a template. The Cu and Zn precursors were introduced to the confined space in the AS and were converted to CuO and ZnO during calcination, during which the template was also removed. The results show that up to 5 mmol·g–1 of CuO and ZnO can be well dispersed; however, severe aggregation of both oxides takes place in the sample derived from the calcined SBA-15 with the same loading. Confined space in the AS and the strong interactions caused by the abundant hydroxyl groups are responsible for the dispersion of CuO and ZnO. The bimetallic materials were employed for the adsorptive separation of propene and propane. The samples prepared from the as-prepared SBA-15 showed superior performance to their counterparts from the calcined SBA-15 in terms of both adsorption capacity of propene and selectivity for propene/propane.
. [J]. Frontiers of Chemical Science and Engineering, 2022, 16(11): 1623-1631.
Yu-Chao Wang, Tian-Tian Li, Li Huang, Xiao-Qin Liu, Lin-Bing Sun. Fabrication of bimetallic Cu–Zn adsorbents with high dispersion by using confined space for gas adsorptive separation. Front. Chem. Sci. Eng., 2022, 16(11): 1623-1631.
P Nugent, Y Belmabkhout, S D Burd, A J Cairns, R Luebke, K Forrest, T Pham, S Ma, B Space, L Wojtas, M Eddaoudi, M J Zaworotko. Porous materials with optimal adsorption thermodynamics and kinetics for CO2 separation. Nature, 2013, 495(7439): 80–84 https://doi.org/10.1038/nature11893
2
M Liu, L Zhang, M A Little, V Kapil, M Ceriotti, S Yang, L Ding, D L Holden, R Balderas-Xicohténcatl, D He, R Clowes, S Y Chong, G Schütz, L Chen, M Hirscher, A I Cooper. Barely porous organic cages for hydrogen isotope separation. Science, 2019, 366(6465): 613–620 https://doi.org/10.1126/science.aax7427
3
D S Sholl, R P Lively. Seven chemical separations to change the world. Nature, 2016, 532(7600): 435–437 https://doi.org/10.1038/532435a
4
A Karmakar, A V Desai, B Manna, B Joarder, S K Ghosh. An amide-functionalized dynamic metal-organic framework exhibiting visual colorimetric anion exchange and selective uptake of benzene over cyclohexane. Chemistry, 2015, 21(19): 7071–7076 https://doi.org/10.1002/chem.201406233
5
K Zhang, R P Lively, M E Dose, A J Brown, C Zhang, J Chung, S Nair, W J Koros, R R Chance. Alcohol and water adsorption in zeolitic imidazolate frameworks. Chemical Communications, 2013, 49(31): 3245–3247 https://doi.org/10.1039/c3cc39116g
6
B N Bhadra, A Vinu, C Serre, S H Jhung. MOF-derived carbonaceous materials enriched with nitrogen: preparation and applications in adsorption and catalysis. Materials Today, 2019, 25: 88–111 https://doi.org/10.1016/j.mattod.2018.10.016
7
T X Bui, H Choi. Adsorptive removal of selected pharmaceuticals by mesoporous silica SBA-15. Journal of Hazardous Materials, 2009, 168(2–3): 602–608 https://doi.org/10.1016/j.jhazmat.2009.02.072
8
P Z Li, X J Wang, S Y Tan, C Y Ang, H Chen, J Liu, R Zou, Y Zhao. Clicked isoreticular metal-organic frameworks and their high performance in the selective capture and separation of large organic molecules. Angewandte Chemie International Edition, 2015, 54(43): 12748–12752 https://doi.org/10.1002/anie.201504346
9
S Shi, Y X Li, S S Li, X Q Liu, L B Sun. Fabrication of Cu+ sites in confined spaces for adsorptive desulfurization by series connection double-solvent strategy. Green Energy & Environment, 2022, 7(2): 345–351 https://doi.org/10.1016/j.gee.2020.10.009
10
C Gu, W Weng, C Lu, P Tan, Y Jiang, Q Zhang, X Liu, L Sun. Decorating MXene with tiny ZIF-8 nanoparticles: an effective approach to construct composites for water pollutant removal. Chinese Journal of Chemical Engineering, 2022, 42: 42–48 https://doi.org/10.1016/j.cjche.2021.06.004
11
S Ma, H C Zhou. Gas storage in porous metal-organic frameworks for clean energy applications. Chemical Communications, 2010, 46(1): 44–53 https://doi.org/10.1039/B916295J
12
P Tan, Y Jiang, Q Wu, C Gu, S Qi, Q Zhang, X Liu, L Sun. Light-responsive adsorbents with tunable adsorbent-adsorbate interactions for selective CO2 capture. Chinese Journal of Chemical Engineering, 2022, 42: 104–111 https://doi.org/10.1016/j.cjche.2021.07.010
13
P Tan, Y Jiang, S C Qi, X J Gao, X Q Liu, L B Sun. Ce-doped smart adsorbents with photoresponsive molecular switches for selective adsorption and efficient desorption. Engineering (Beijing), 2020, 6(5): 569–576 https://doi.org/10.1016/j.eng.2020.03.005
14
X Zhao, Y Yuan, P Li, Z Song, C Ma, D Pan, S Wu, T Ding, Z Guo, N Wang. A polyether amine modified metal organic framework enhanced the CO2 adsorption capacity of room temperature porous liquids. Chemical Communications (Cambridge), 2019, 55(87): 13179–13182 https://doi.org/10.1039/C9CC07243H
15
A Alsbaiee, B J Smith, L Xiao, Y Ling, D E Helbling, W R Dichtel. Rapid removal of organic micropollutants from water by a porous β-cyclodextrin polymer. Nature, 2016, 529(7585): 190–194 https://doi.org/10.1038/nature16185
16
T Zhang, X Huang, T Asefa. Nanostructured polymers with high surface area using inorganic templates for the efficient extraction of anionic dyes from solutions. Chemical Communications, 2015, 51(89): 16135–16138 https://doi.org/10.1039/C5CC06816A
17
D K Yoo, T U Yoon, Y S Bae, S H Jhung. Metal-organic framework MIL-101 loaded with polymethacrylamide with or without further reduction: effective and selective CO2 adsorption with amino or amide functionality. Chemical Engineering Journal, 2020, 380: 122496 https://doi.org/10.1016/j.cej.2019.122496
18
S C Qi, D M Xue, G X Yu, R R Zhu, X Q Liu, L B Sun. An antiempirical strategy: sacrificing aromatic moieties in the polymer precursor for improving the properties of the derived N-doped porous carbons. Green Chemical Engineering, 2020, 1(1): 70–76 https://doi.org/10.1016/j.gce.2020.09.001
19
C J Yoo, P Narayanan, C W Jones. Self-supported branched poly(ethyleneimine) materials for CO2 adsorption from simulated flue gas. Journal of Materials Chemistry A: Materials for Energy and Sustainability, 2019, 7(33): 19513–19521 https://doi.org/10.1039/C9TA04662C
20
R L Siegelman, P J Milner, E J Kim, S C Weston, J R Long. Challenges and opportunities for adsorption-based CO2 capture from natural gas combined cycle emissions. Energy & Environmental Science, 2019, 12(7): 2161–2173 https://doi.org/10.1039/C9EE00505F
21
M Pardakhti, T Jafari, Z Tobin, B Dutta, E Moharreri, N S Shemshaki, S Suib, R Srivastava. Trends in solid adsorbent materials development for CO2 capture. ACS Applied Materials & Interfaces, 2019, 11(38): 34533–34559 https://doi.org/10.1021/acsami.9b08487
22
F Subhan, S Aslam, Z Yan, L Zhen, M Ikram, R Ullah, U J Etim, A Ahmad. Ammonia assisted functionalization of cuprous oxide within confined spaces of SBA-15 for adsorptive desulfurization. Chemical Engineering Journal, 2018, 339: 557–565 https://doi.org/10.1016/j.cej.2018.01.146
23
M A Alkhabbaz, P Bollini, G S Foo, C Sievers, C W Jones. Important roles of enthalpic and entropic contributions to CO2 capture from simulated flue gas and ambient air using mesoporous silica grafted amines. Journal of the American Chemical Society, 2014, 136(38): 13170–13173 https://doi.org/10.1021/ja507655x
24
J Kou, C Lu, W Sun, L Zhang, Z Xu. Facile fabrication of cuprous oxide-based adsorbents for deep desulfurization. ACS Sustainable Chemistry & Engineering, 2015, 3(12): 3053–3061 https://doi.org/10.1021/acssuschemeng.5b01051
25
Y Kuwahara, D Y Kang, J R Copeland, N A Brunelli, S A Didas, P Bollini, C Sievers, T Kamegawa, H Yamashita, C W Jones. Dramatic enhancement of CO2 uptake by poly(ethyleneimine) using zirconosilicate supports. Journal of the American Chemical Society, 2012, 134(26): 10757–10760 https://doi.org/10.1021/ja303136e
26
S Giret, M Wong Chi Man, C Carcel. Mesoporous-silica-functionalized nanoparticles for drug delivery. Chemistry, 2015, 21(40): 13850–13865 https://doi.org/10.1002/chem.201500578
27
X Zhang, Z Qu, F Yu, Y Wang. High-temperature diffusion induced high activity of SBA-15 supported Ag particles for low temperature CO oxidation at room temperature. Journal of Catalysis, 2013, 297(0): 264–271 https://doi.org/10.1016/j.jcat.2012.10.019
28
P Wang, X Zheng, X Wu, X Wei, L Zhou. Preparation and characterization of CuO nanoparticles encapsulated in mesoporous silica. Microporous and Mesoporous Materials, 2012, 149(1): 181–185 https://doi.org/10.1016/j.micromeso.2011.07.002
29
Z Wu, D Zhao. Ordered mesoporous materials as adsorbents. Chemical Communications, 2011, 47(12): 3332 https://doi.org/10.1039/c0cc04909c
30
D Y Zhao, Q S Huo, J L Feng, B F Chmelka, G D Stucky. Nonionic triblock and star diblock copolymer and oligomeric surfactant syntheses of highly ordered, hydrothermally stable, mesoporous silica structures. Journal of the American Chemical Society, 1998, 120(24): 6024–6036 https://doi.org/10.1021/ja974025i
31
D Y Zhao, J L Feng, Q S Huo, N Melosh, G H Fredrickson, B F Chmelka, G D Stucky. Triblock copolymer syntheses of mesoporous silica with periodic 50 to 300 angstrom pores. Science, 1998, 279(5350): 548–552 https://doi.org/10.1126/science.279.5350.548
32
Z Zhang, I Melián-Cabrera. Modifying the hierarchical porosity of SBA-15 via mild-detemplation followed by secondary treatments. Journal of Physical Chemistry C, 2014, 118(49): 28689–28698 https://doi.org/10.1021/jp5096213
33
Q Zheng, Y Zhu, J Xu, Z Cheng, H Li, X Li. Fluoroalcohol and fluorinated-phenol derivatives functionalized mesoporous SBA-15 hybrids: high-performance gas sensing toward nerve agent. Journal of Materials Chemistry, 2012, 22(5): 2263–2270 https://doi.org/10.1039/C1JM14779J
34
J Zhi, D Song, Z Li, X Lei, A Hu. Palladium nanoparticles in carbon thin film-lined SBA-15 nanoreactors: efficient heterogeneous catalysts for Suzuki-Miyaura cross coupling reaction in aqueous media. Chemical Communications, 2011, 47(38): 10707–10709 https://doi.org/10.1039/c1cc14169d
35
Z Wu, W Zhu, M Zhang, Y Lin, N Xu, F Chen, D Wang, Z Chen. Adsorption and synergetic fenton-like degradation of methylene blue by a novel mesoporous α-Fe2O3/SiO2 at neutral pH. Industrial & Engineering Chemistry Research, 2018, 57(16): 5539–5549 https://doi.org/10.1021/acs.iecr.8b00077
36
Z Wu, Q Lu, W H Fu, S Wang, C Liu, N Xu, D Wang, Y M Wang, Z Chen. Fabrication of mesoporous Al-SBA-15 as a methylene blue capturer via a spontaneous infiltration route. New Journal of Chemistry, 2015, 39(2): 985–993 https://doi.org/10.1039/C4NJ01473A
37
Y M Wang, Z Y Wu, H J Wang, J H Zhu. Fabrication of metal oxides occluded in ordered mesoporous hosts via a solid-state grinding route: the influence of host-guest interactions. Advanced Functional Materials, 2006, 16(18): 2374–2386 https://doi.org/10.1002/adfm.200500613
38
Y Yin, W J Jiang, X Q Liu, Y H Li, L B Sun. Dispersion of copper species in a confined space and their application in thiophene capture. Journal of Materials Chemistry, 2012, 22(35): 18514 https://doi.org/10.1039/c2jm33216g
39
L Y Shi, Y X Li, D M Xue, P Tan, Y Jiang, X Q Liu, L B Sun. Fabrication of highly dispersed nickel in nanoconfined spaces of as-made SBA-15 for dry reforming of methane with carbon dioxide. Chemical Engineering Journal, 2020, 390: 124491 https://doi.org/10.1016/j.cej.2020.124491
40
T Wang, X Li, W Dai, Y Fang, H Huang. Enhanced adsorption of dibenzothiophene with zinc/copper-based metal-organic frameworks. Journal of Materials Chemistry A: Materials for Energy and Sustainability, 2015, 3(42): 21044–21050 https://doi.org/10.1039/C5TA05204A
41
N A Khan, C M Kim, S H Jhung. Adsorptive desulfurization using Cu-Ce/metal-organic framework: improved performance based on synergy between Cu and Ce. Chemical Engineering Journal, 2017, 311: 20–27 https://doi.org/10.1016/j.cej.2016.11.067
42
G I Danmaliki, T A Saleh. Effects of bimetallic Ce/Fe nanoparticles on the desulfurization of thiophenes using activated carbon. Chemical Engineering Journal, 2017, 307: 914–927 https://doi.org/10.1016/j.cej.2016.08.143
43
Y Kou, L B Sun. Size regulation of platinum nanoparticles by using confined spaces for the low-temperature oxidation of ethylene. Inorganic Chemistry, 2018, 57(3): 1645–1650 https://doi.org/10.1021/acs.inorgchem.7b02988
44
M X Gu, Y Kou, S C Qi, M Q Shao, M B Yue, X Q Liu, L B Sun. Highly dispersive cobalt oxide constructed in confined space for oxygen evolution reaction. ACS Sustainable Chemistry & Engineering, 2019, 7(2): 2837–2843 https://doi.org/10.1021/acssuschemeng.8b06214
45
L Kong, T Zhang, R Yao, Y Zeng, L Zhang, P Jian. Adsorptive desulfurization of fuels with Cu(I)/SBA-15 via low-temperature reduction. Microporous and Mesoporous Materials, 2017, 251: 69–76 https://doi.org/10.1016/j.micromeso.2017.05.052
