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1.
J Environ Sci (China) ; 140: 292-305, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38331509

RESUMEN

Integrated CO2 capture and utilization (ICCU) technology requires dual functional materials (DFMs) to carry out the process in a single reaction system. The influence of the calcination atmosphere on efficiency of 4% Ru-8% Na2CO3-8% CaO/γ-Al2O3 DFM is studied. The adsorbent precursors are first co-impregnated onto alumina and calcined in air. Then, Ru precursor is impregnated and four aliquotes are subjected to different calcination protocols: static air in muffle or under different mixtures (10% H2/N2, 50% H2/N2 and N2) streams. Samples are characterized by XRD, N2 adsorption-desorption, H2 chemisorption, TEM, XPS, H2-TPD, H2-TPR, CO2-TPD and TPSR. The catalytic behavior is evaluated, in cycles of CO2 adsorption and hydrogenation to CH4, and temporal evolution of reactants and products concentrations is analyzed. The calcination atmosphere influences the physicochemical properties and, ultimately, activity of DFMs. Characterization data and catalytic performance discover the acccomodation of Ru nanoparticles disposition and basic sites is mostly influencing the catalytic activity. DFM calcined under N2 flow (RuNaCa-N2) shows the highest CH4 production (449 µmol/g at 370°C), because a well-controlled decomposition of precursors which favors the better accomodation of adsorbent and Ru phases, maximizing the specific surface area, the Ru-basic sites interface and the participation of different basic sites in the CO2 methanation reaction. Thus, the calcination in a N2 flow is revealed as the optimal calcination protocol to achieve highly efficient DFM for integrated CO2 adsorption and hydrogenation applications.


Asunto(s)
Óxido de Aluminio , Dióxido de Carbono , Adsorción , Hidrogenación , Atmósfera , Iones
2.
J Phys Chem Lett ; 8(15): 3473-3477, 2017 Aug 03.
Artículo en Inglés | MEDLINE | ID: mdl-28696704

RESUMEN

Polymer-rich composite electrolytes with lithium bis(fluorosulfonyl)imide/poly(ethylene oxide) (LiFSI/PEO) containing either Li-ion conducting glass ceramic (LICGC) or inorganic Al2O3 fillers are investigated in all-solid-state Li-S cells. In the presence of the fillers, the ionic conductivity of the composite polymer electrolytes (CPEs) does not increase compared to the plain LiFSI/PEO electrolyte at various tested temperatures. The CPE with Al2O3 fillers improves the stability of the Li/electrolyte interface, while the Li-S cell with a LICGC-based CPE delivers high sulfur utilization of 1111 mAh g-1 and areal capacity of 1.14 mAh cm-2. In particular, the cell performance gets further enhanced when combining these two CPEs (Li | Al2O3-CPE/LICGC-CPE | S), reaching a capacity of 518 mAh g-1 and 0.53 mAh cm-2 with Coulombic efficiency higher than 99% at the end of 50 cycles at 70 °C. This study shows that the CPEs can be promising electrolyte candidates to develop safe and high-performance all-solid-state Li-S batteries.

3.
J Phys Chem Lett ; 8(9): 1956-1960, 2017 May 04.
Artículo en Inglés | MEDLINE | ID: mdl-28407471

RESUMEN

Solid polymer electrolytes (SPEs) comprising lithium bis(fluorosulfonyl)imide (Li[N(SO2F)2], LiFSI) and poly(ethylene oxide) (PEO) have been studied as electrolyte material and binder for the Li-S polymer cell. The LiFSI-based Li-S all solid polymer cell can deliver high specific discharge capacity of 800 mAh gsulfur-1 (i.e., 320 mAh gcathode-1), high areal capacity of 0.5 mAh cm-2, and relatively good rate capability. The cycling performances of Li-S polymer cell with LiFSI are significantly improved compared with those with conventional LiTFSI (Li[N(SO2CF3)2]) salt in the polymer membrane due to the improved stability of the Li anode/electrolyte interphases formed in the LiFSI-based SPEs. These results suggest that the LiFSI-based SPEs are attractive electrolyte materials for solid-state Li-S batteries.

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