The objective of the work presented here is to develop a nanoporous solid adsorbent which can serve as a "molecular basket" for CO 2 in the condensed form. Polyethylenimine (PEI)-modified mesoporous molecular sieve of MCM-41 type (MCM-41-PEI) has been prepared and tested as a CO 2 adsorbent. The physical properties of the adsorbents were characterized by X-ray powder diffraction (XRD), N 2 adsorption/desorption, and thermogravimetric analysis (TGA). The characterizations indicated that the structure of the MCM-41 was preserved after loading the PEI, and the PEI was uniformly dispersed into the channels of the molecular sieve. The CO 2 adsorption/desorption performance was tested in a flow system using a microbalance to track the weight change. The mesoporous molecular sieve had a synergetic effect on the adsorption of CO 2 by PEI. A CO 2 adsorption capacity as high as 215 mg-CO 2 /g-PEI was obtained with MCM-41-PEI-50 at 75 °C, which is 24 times higher than that of the MCM-41 and is even 2 times that of the pure PEI. With an increase in the CO 2 concentration in the CO 2 /N 2 gas mixture, the CO 2 adsorption capacity increased. The cyclic adsorption/desorption operation indicated that the performance of the adsorbent was stable.
An infrared study has been conducted on CO 2 sorption into nanoporous CO 2 "molecular basket" sorbents prepared by loading polyethylenimine (PEI) into mesoporous molecular sieve SBA-15. IR results from DRIFTS showed that a part of loaded PEI is anchored on the surface of SBA-15 through the interaction between amine groups and isolated surface silanol groups. Raising the temperature from 25 to 75 °C increased the molecular flexibility of PEI loaded in the mesopore channels, which may partly contribute to the increase of CO 2 sorption capacity at higher temperatures. CO 2 sorption/desorption behavior studied by in situ transmission FTIR showed that CO 2 is sorbed on amine sites through the formation of alkylammonium carbamates and absorbed into the multiple layers of PEI located in mesopores of SBA-15. A new observation by in situ IR is that two broad IR bands emerged at 2450 and 2160 cm -1 with CO 2 flowing over PEI(50)/SBA-15, which could be attributed to chemically sorbed CO 2 species on PEI molecules inside the mesopores of SBA-15. The intensities of these two bands also increased with increasing CO 2 exposure time and with raising CO 2 sorption temperature. By comparison of the CO 2 sorption rate at 25 and 75 °C in terms of differential IR intensities, it was found that CO 2 sorption over molecular basket sorbent includes two rate regimes which suggest two distinct steps: rapid sorption on exposed outer surface layers of PEI (controlled by sorption affinity or thermodynamics) and the diffusion and sorption inside the bulk of multiple layers of PEI (controlled by diffusion). The sorption of CO 2 is reversible at 75 °C. Comparative IR examination of the CO 2 sorption/ desorption spectra on dry and prewetted PEI/SBA-15 sorbent revealed that presorbed water does not significantly affect the CO 2 -amine interaction patterns.
Adsorption separation of CO2 from simulated flue gas containing CO2, O2, and N2 with and
without moisture was investigated using a novel nanoporous adsorbent based on polyethylenimine (PEI)-modified mesoporous molecular sieve MCM-41 in a flow system. The CO2 adsorption
capacity and CO2 separation selectivity of MCM-41 were greatly improved by loading PEI into
its nanosized pore channels, which made the resulting adsorbent operating like a “molecular
basket” for CO2. CO2 adsorption capacity of the MCM-41-PEI adsorbent for the simulated moist
flue gas was higher than that for the simulated dry flue gas. CO2 separation selectivity of the
MCM-41-PEI adsorbent was also improved in the presence of moisture when compared with
those in the dry gas condition. The influence of moisture concentrations in the simulated flue
gas on the CO2 adsorption separation performance was also examined. The results of adsorption/desorption separation cycles showed that the MCM-41-PEI adsorbent was stable over 10 cycles
of adsorption/desorption operations. The hydrothermal stability of the “molecular basket”
adsorbent was better than that of the MCM-41 support alone.
Efficient hole-conductor-free organic lead iodide thin film solar cells have been fabricated with a sequential deposition method, and a highest efficiency of 10.49% has been achieved. Meanwhile, the ideal current-voltage model for a single heterojunction solar cell is applied to clarify the junction property of the cell. The model confirms that the TiO 2 /CH 3 NH 3 PbI 3 /Au cell is a typical heterojunction cell and the intrinsic parameters of the cell are comparable to that of the high-efficiency thin-film solar cells. V
suffer from safety problems arising from lithium anode and fast capacity fading due to the insulating nature of sulfur, the dissolution-induced polysulfide shuttle reaction, and large volume changes. [4][5][6] To address these issues, carbonaceous material [7,8] and conducting polymers [9] have been used to trap the high-order polysulfides in the cathodes; protective layers and electrolyte additives are employed for protection of metallic-lithium anodes from reactions with polysulfide. [10,11] However, the shuttle reaction still exists, and the safety issue induced by lithium dendrite is still a great challenge.All-solid-state Li-S batteries can completely inhibit the dissolution of polysulfide, eliminate the polysulfide shuttle, and avoid lithium dendrite formation. [12][13][14][15][16][17][18][19] However, the use of rigid solid electrolytes in all-solid-state Li-S batteries also increases the stress/strain and interface resistance and reduce the reaction kinetics. [20][21][22] The key challenge is to minimize stress/strain and to construct a robust electronic and ionic pathway in the sulfur cathode, due to the electronic/ionic insulting nature of sulfur. For enhancing the electronic conductivity and reducing the electronic contact resistance, Kobayashi et al. synthesized a sulfur and acetylene black (AB) nanocomposite cathode using a gas-phase mixing method, and reported a reversible capacity of 900 mA h g −1 at a current density of 0.013 mA cm −2 in all-solid-state batteries. [23] The sulfur and carbon-nanofibers composite cathode also shows a high capacity in the all-solid-state Li-S batteries. [24] To ensure high ionic conduction in the sulfur cathode, Lin et al. synthesized core-shell structured lithium-sulfide nanoparticles with an Li 3 PS 4 electrolyte as shell, showing six orders of magnitude higher in ionic conductivity than that of bulk lithiumsulfide. Excellent cyclic performance was demonstrated for allsolid-state Li-S batteries at 60 °C. [13] By incorporation of five sulfur atoms in the Li 3 PS 4 electrolyte, the Li 3 PS 4+5 cathode with loading density of 0.25-0.6 mg cm −2 exhibits excellent cycling stability for all-solid-state Li-S batteries. [14] These studies demonstrate that a close contact of the nanosulfur, either to carbon or to electrolytes, and uniformly distributing these composites into an ionic/electronic conducting matrix, can significantly improve the electrochemical performances of solid-state Li-S cell because the nano-sulfur contacts both the highly ionic and Safety and the polysulfide shuttle reaction are two major challenges for liquid electrolyte lithium-sulfur (Li-S) batteries. Although use of solid-state electrolytes can overcome these two challenges, it also brings new challenges by increasing the interface resistance and stress/strain. In this work, the interface resistance and stress/strain of sulfur cathodes are significantly reduced by conformal coating ≈2 nm sulfur (S) onto reduced graphene oxide (rGO). An Li-S full cell consisting of an rGO@S-Li 10 GeP 2 S 12 -acetyle...
The interfacial atomic and electronic structures, charge transfer processes, and interface engineering in perovskite solar cells are discussed in this review. An effective heterojunction is found to exist at the window/perovskite absorber interface, contributing to the relatively fast extraction of free electrons. Moreover, the high photovoltage in this cell can be attributed to slow interfacial charge recombination due to the outstanding material and interfacial electronic properties. However, some fundamental questions including the interfacial atomic and electronic structures and the interface stability need to be further clarified. Designing and engineering the interfaces are also important for the next-stage development of this cell.
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