A new family of six ionenes containing aromatic amide linkages has been synthesized from ready available starting materials at scales up to ∼50 g. These ionene-polyamides are all constitutional isomers and vary only in the regiochemistry of the amide linkages (para, meta) and xylyl linkages (ortho, meta, para) which are present in the polymer backbone. This paper details the synthesis of these ionenes and associated characterizations. Ionene-polyamides exhibit relatively low melting points (∼150 oC) allowing them to be readily processed into films and other objects. These ionene-polyamide materials are being developed for further study as polymer membranes for the separations of gases such as CO2, N2, CH4 and H2.

Carboxylated carbon nanotubes (C or cCNTs) were incorporated in polyethersulfone hollow fiber membranes (P HFMs) to improve the gas separation performance, i.e., pure gas permeability and ideal gas selectivity. The developed CP HFMs showed the remarkable improvement in thermal stability and mechanical strength as compared to that of the pristine P HFMs. The pure gas permeability of CO2, CH4, O2, and N2 gases for the HFMs were measured at 3 bar feed pressure and room temperature. It was observed that the presence of cCNTs in HFMs significantly improved the CO2 and O2 permeability for CP HFMs by 10.8-and 11.7- fold, respectively, as compared to that measured for P HFMs. Furthermore, the ideal gas selectivity for CO2/CH4, O2/N2, and CO2/N2 gas pairs for CP HFMs was also remarkably enhanced by almost 8.6-, 10.7-and 9.9-times, respectively, as compared to that measured for P HFMs. CP HFMs exhibited gas separation performance better than or comparable to that of the literature-reported CNTs-based membranes. Remarkably, the gas separation performance of CP HFMs crossed Robeson’s 2008 upper bound curve for O2/N2 gas-pair and was almost closer to the upper bound curves drawn by Robeson in 2008 for CO2/CH4 and CO2/N2 gas pairs. The improved separation performance can be attributed to the presence of cCNTs in HFMs. Thus, the results obtained in this study clearly showed that the CP HFMs can potentially be used as a membrane material for the industrially relevant gas separations.

Monolithic integrated thin film tandem solar cells consisting of a high bandgap perovskite top cell and a low bandgap thin film bottom cell are expected to reach higher power conversion efficiencies (PCEs) with lower manufacturing cost and environmental impacts than the market-dominant crystalline silicon photovoltaics. There have been several demonstrations of 4-terminal and 2-terminal perovskite tandem devices with CuInGaSe2 (CIGS) or CuInSe2 (CIS) and, similar to the other tandem structures, the optimization of this device relies on optimal choice for the perovskite bandgap and thickness. Therefore, further advancement will be enabled by tuning the perovskite absorber to maximize the photocurrent limited by the current match condition. Here, we systematically study the optical absorption and transmission of perovskite thin films with varying absorber band gap. Based on these results, we model the photocurrent generations in both perovskite and CIS subcells and estimate the performances of projected tandem devices by considering the ideally functioning perovskite and CIS device. Our results show that for perovskite layers with 500 nm thickness the optimal bandgap is around 1.6 eV. With these configurations, PCEs above 20% could be achieved by monolithically integrated perovskite/CIS tandem solar cells. Also by modelling the absorption at every layer we calculate the quantum efficiency at each subcell in addition to tracking optical losses.

Wide bandgap Cd1-xZnxTe (CZT) and Cd1-xMgxTe (CMT) have drawn attention as top cells in tandem devices. These materials allow tuning of the band gap over a wide range by controlling the Zn or Mg concentration with little alteration to the base CdTe properties. Historically, CdS has been used as a heterojunction partner for CZT or CMT devices. However, these devices show a significant lower open circuit voltage (VOC) than expected for wide bandgap absorbers. Recent modelling work suggests that poor band alignment between the CdS emitter and absorber results in a high concentration of holes at the interface, which increased recombination and limits the VOC. This recombination should be exacerbated for wider bandgap absorbers such as CZT and CMT. In this study, we use numerical simulations with SCAPS-1D software to investigate the band alignment in the front contacts for wider bandgap CdTe based absorbers. Results show that by replacing the CdS with a wide bandgap emitter layer, the VOC can be greatly improved, though under certain conditions, the fill factor remains sensitive to the location of the emitter conduction band. As a result, different transparent front contacts were also investigated to determine a device structure required to produce a high performance CZT or CMT top-cell for tandems devices.

Increasing the band gap of cadmium telluride (CdTe) from 1.48 eV to > 2 eV can be achieved by alloying CdTe with ZnTe. Like CdTe, the alloyed films are expected to allow for low cost production, suggesting that Cd1-xZnxTe could be an ideal top cell for mass produced tandem devices. However, the CdCl2 activation of the alloyed films results in a significant loss of Zn, thereby reducing the bandgap. In this study, we demonstrate a novel CdCl2 activation method that does not result in significant Zn loss. By performing the activation step in a closed, inert environment we are able to avoid oxidation of the Zn in the Cd1-xZnxTe film; furthermore, by including sacrificial Zn in the container, an overpressure of ZnCl2 forms limiting the amount of ZnCl2 formed in the film. Both x-ray diffraction, optical measurements, and Auger spectroscopy show that the CdCl2 treatment with no flowing gas minimizes the loss of Zn from the CZT alloy.

Photoluminescence (PL) spectroscopy has been used to study the defect levels in thin film copper indium diselenide (CuInSe2, CIS) which we are developing as the absorber layer for the bottom cell of a monolithically grown perovskite/CuInSe2 tandem solar cell. Temperature and laser power dependent PL measurements of thin film CIS for two different Cu/In ratios (0.66 and 0.80) have been performed. The CIS film with Cu/In = 0.80 shows a prominent donor-to-acceptor peak (DAP) involving a shallow acceptor of binding energy ∼22 meV, with phonon replica at ∼32 meV spacing. In contrast, PL measurement of CIS film for Cu/In = 0.66 taken at 20 K exhibited an asymmetric and broad PL spectrum with peaks at 0.845 eV and 0.787 eV. Laser intensity dependent PL revealed that the observed peaks 0.845 eV and 0.787 eV shift towards higher energy (aka j-shift) at ∼11.7 meV/decade and ∼ 8 meV/decade with increase in laser intensity respectively. The asymmetric and broad spectrum together with large j-shift suggests that the observed peaks at 0.845 eV and 0.787 eV were related to band-to-tail (BT) and band-to-impurity (BI) transition, respectively. Such a band-tail-related transition originates from the potential fluctuation of defect states at low temperature. The appearance of band related transition in CIS film with Cu/In = 0.66 is the indicator of the presence of large number of charged defect states.