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At least 37 records · Page 2

Lead-Free Flexible Perovskite Solar Cells with Interfacial Native Oxide Have >10% Efficiency and Simultaneously Enhanced Stability and Reliability

Here we demonstrate an innovative compositional and interfacial engineering approach to achieve Pb-free flexible perovskite solar cells (f-PSCs) with an unprecedented combination of the highest efficiency reported to date (10.43%), together with enhanced operational stability and mechanical reliability. The key to this approach is alloying of an FASnI3 metal halide perovskite (MHP) thin film with Ge2+ to stabilize the Sn2+ oxidation state in the MHP, together with the use of a NiOx hole-transport layer. We show that this results in the in situ formation of a thin amorphous GeO2 native oxide layer at the NiOx/FASn0.9Ge0.1I3 interface. This layer not only passivates that critical interface but also enhances the interfacial mechanical bonding.

efficiency↗

Bilayer Electron Transport Layers for High–Performance Rigid and Flexible Perovskite Solar Cells

While great progress is being made in achieving high power conversion efficiency (PCE), durability, and reliability in rigid and flexible n–i–p perovskite solar cells (PSCs), there is still room for improvement. Among myriad ways this can be achieved, one way is to improve the processing and quality of electron transport layers (ETLs) used in PSCs. To that end, here we explore the use of SnO 2 /TiO 2 bilayer ETLs in both rigid and flexible PSCs. In the case of rigid PSCs, chemical bath deposition (CBD) is used where the bilayer architecture affords the CBD of high-quality ETL, which results in PSCs with up to 25.13% PCE and operational stability T 80 (80% of initial PCE retained) of 2220 h under 1-sun continuous illumination with maximum power-point tracking. In the case of flexible PSCs, once again, the bilayer architecture allows us to fabricate high-quality ETL using spin coating, which results in PSCs with up to 22.54% PCE and excellent mechanical durability, withstanding 20 000 bending cycles with ≈92% of the initial PCE retained. Mechanisms underlying the enhanced performance and stability/durability of rigid and flexible PSCs that use SnO 2 /TiO 2 bilayer ETLs are elucidated. Furthermore, this approach could be extended to other ETL systems for PSCs for further improvements in PCE, durability, and reliability.

14 SOLAR ENERGY↗

Better Back Contacts for Solar Cells on Flexible Substrates

Improved low-resistance, semitransparent back contacts, and a method of fabricating them, have been developed for solar photovoltaic cells that are made from thin films of I-III-VI2 semiconductor materials on flexible, high-temperatureresistant polyimide substrates or superstrates. The innovative aspect of the present development lies in the extension, to polyimide substrates or superstrates, of a similar prior development of improved low-resistance, semitransparent back contacts for I-III-VI2 solar cells on glass substrates or superstrates. A cell incorporating this innovation can be used either as a stand-alone photovoltaic device or as part of a monolithic stack containing another photovoltaic device that utilizes light of longer wavelengths.

Woods, Lawrence M.↗

Critical Issues for Cu(InGa)Se2 Solar Cells on Flexible Polymer Web

Elemental in-line evaporation on glass substrates has been a viable process for the large-area manufacture of CuInSe2-based photovoltaics, with module efficiencies as high as 12.7% [1]. However, lightweight, flexible CuInSe2-based modules are attractive in a number of applications, such as space power sources. In addition, flexible substrates have an inherent advantage in manufacturability in that they can be deposited in a roll-to-roll configuration allowing continuous, high yield, and ultimately lower cost production. As a result, high-temperature polymers have been used as substrates in depositing CuInSe2 films [2]. Recently, efficiency of 14.1% has been reported for a Cu(InGa)Se2-based solar cell on a polyimide substrate [3]. Both metal foil and polymer webs have been used as substrates for Cu(InGa)Se2-based photovoltaics in a roll-to-roll configuration with reasonable success [4,5]. Both of these substrates do not allow, readily, the incorporation of Na into the Cu(InGa)Se2 film which is necessary for high efficiency devices [3]. In addition, polymer substrates, can not be used at temperatures that are optimum for Cu(InGa)Se2 deposition. However, unlike metal foils, they are electrically insulating, simplifying monolithically-integrated module fabrication and are not a source of impurities diffusing into the growing film. The Institute of Energy Conversion (IEC) has modified its in-line evaporation system [6] from deposition onto glass substrates to roll-to-roll deposition onto polyimide (PI) film in order to investigate key issues in the deposition of large-area Cu(InGa)Se2 films on flexible polymer substrates. This transition presented unexpected challenges that had to be resolved. In this paper, two major problems, spitting from the Cu source and the cracking of Mo back contact film, will be discussed and the solution to each will be presented.

Eser, Erten↗

Photonic Curing of Nickel Oxide Transport Layer and Perovskite Active Layer for Flexible Perovskite Solar Cells: A Path Towards High-Throughput Manufacturing

High-throughput roll-to-roll (R2R) manufacturing of perovskite solar cells (PSCs) is currently limited by thermal processes that take tens of minutes each, translating to impractically long annealing tools at high web speeds. In addition, PSCs are usually made with metal oxide transport layer materials that require high temperatures for thermal annealing. Here, we demonstrate the fabrication of PSCs using photonic curing, instead of thermal annealing, to convert NiO x directly from sol-gel precursors for hole transport layers and to crystallize methylammonium lead iodide (MAPbI 3 ) active layers on flexible Willow ® Glass substrates. Photonic curing uses short, intense pulses of light to process materials at a high speed, hence it is compatible with R2R manufacturing. We achieved power conversion efficiencies (PCEs) of 11.7% in forward-scan and 10.9% in reverse-scan for PSCs made with photonic cured NiO x and MAPbI 3 films. Furthermore, both NiO x and MAPbI 3 films could be processed with a single photonic curing pulse, with a web speed of 5.7 m/min, and still produce PCEs comparable to thermally annealed control samples. Based on the single-pulse photonic curing condition for each film, we project a web speed of 26 m/min, laying a pathway to high-throughput production of perovskite solar modules.

14 SOLAR ENERGY↗

Regulating crystallization to maintain balanced carrier mobility via ternary strategy in blade-coated flexible organic solar cells

Regulating the crystallization of donor and acceptor to maintain balanced carrier mobility is of great importance to fabricate efficient organic solar cells (OSCs). Herein, the balanced crystallinity between donor and acceptor was finely controlled in blade-coated OSCs. By adding high crystalline FOIC into PBDB-T:ITIC system, a balanced carrier mobility was achieved, resulting in the much improved fill factor. The optimized ternary device exhibits an increased current density, due to the enhanced light-harvesting efficiency with complementary absorption and the morphology change. Morphology characterization demonstrated that the ternary film exhibits a highly balanced crystallinity between the donor and acceptor on account of the formation of acceptor alloy. Moreover, the ternary film not only possesses a small domain size, but also exhibits a high domain purity as compared to both binary films. Encouragingly, a highest power conversion efficiency (PCE) of 10.68% was obtained for the blade-coated ternary OSCs. In addition, the blade-coated flexible large-area (105 mm 2 ) OSC based on PBDB-T:ITIC:FOIC ternary system also exhibits a high PCE of 9.81%, showing great potential in the high-throughput fabrication of OSCs.

14 SOLAR ENERGY↗

Higher Throughput, Lower Cost Processing of Flexible Perovskite Solar Cells by Photonic Curing

The objectives of this SETO project are to explore whether photonic curing can be used to perform annealing in perovskite solar cell (PSC) fabrication, and if so, whether it can enable high-throughput PSC manufacturing. The successful outcome of the project will reduce manufacturing cost towards realizing the SETO goal of the Levelized cost of electricity (LCOE) $0.03/kWh by 2030. The project is a collaboration between Hsu’s group at the University of Texas at Dallas (UTD) and NovaCentrix, an Austin TX based company that pioneered the PulseForge® photonic curing tools and has expertise in applying this technology to printed electronics. Thin-film synthesis typically involves a thermal annealing step to convert from precursors to final material phases, to obtain the desired crystalline phase, or to improve materials structural or electrical properties. However, thermal annealing typically requires high temperatures that are incompatible with inexpensive plastic substrates and annealing times lasting tens-to-hundreds of minutes, making it incompatible with roll-to-roll (R2R) manufacturing at a desirable web speed. Photonic curing uses a flash Xe lamp to deliver short (20 µs to 100 ms) but high intensity (up to 50 kW/cm 2 ) pulses of broadband light (200 – 1500 nm) to the sample. It has been successfully applied to sinter printed metal nanoparticle inks into conductive patterns. This project aimed to extend the applications of photonic curing to convert halide perovskite films and transparent metal oxide transport layers. Despite the interruption by COVID-19, we have achieved significant accomplishments to establish photonic curing as a viable technology for the high-throughput manufacturing of PSCs. (1) We demonstrated that photonic curing can convert both metal oxide transport layer and halide perovskite absorber in the PSCs and successfully made flexible PSCs on Corning Willow glass® (WG)/ indium tin oxide (ITO) substrates without any thermal annealing steps. These photonically cured devices achieve performance comparable to conventional thermally annealed devices but were fabricated with a total processing time reduced by six orders of magnitude. We also show that photonic curing can achieve desirable web speed (up to 26 m/min) and large-area uniformity. (2) By establishing photonic curing processing phase spaces for the perovskite, we show that the longer pulses are more forgiving in small variation in the photonic curing conditions, making it more suitable for R2R manufacturing. (3) Our results clearly illustrated the importance of improving mechanical and optical properties of transparent electrodes on flexible substrates. (4) We also performed fundamental studies that elucidate the interactions between perovskite absorber and metal oxide transport layer that can undermine the PSC stability. Five refereed journal papers in top journals (ACS Energy Letters, npj Flexible Electronics, ACS Applied Energy Materials, Materials Advances, and Frontiers in Energy Research), one conference proceeding (PVSC-47), six conference presentations (PVSC and Materials Research Society meetings), and a Ph.D. dissertation (Trey B. Daunis) were produced under this project. Energy Materials Corporation (EMC) has forecast that with a 1.5 m wide web moving at a web speed of 30 m/min, R2R processing of PSC could provide up to 4 GW/year for a single R2R assembly line. Replacing thermal annealing with photonic curing, as demonstrated by the accomplishments of this project, is necessary to realize such an energy production goal.

14 SOLAR ENERGY↗

Rapid scalable fabrication of roll-to-roll slot-die coated flexible perovskite solar cells using intense pulse light annealing

Perovskite solar cells have achieved high efficiencies at the lab scale using batch processes that often may not be scalable. Processes that can be integrated into a continuous manufacturing platform, such as roll-to-roll, where several processes can be carried out sequentially are necessary to develop a new cost-competitive solar technology. In this work, intense pulsed light thermal post-processing is coupled with scalable slot-die coating and air knife evaporation in a high-speed roll-to-roll process of up to 2 m min –1 . The optimization of IPL energy parameters, web speeds, solution flow rates, and concentration of precursor inks yielded a champion power conversion efficiency of 11.24% for a 1 cm 2 roll-to-roll coated device. The overall processing time for a single layer in this process is reduced from minutes to seconds and the overall footprint of the manufacturing process is decreased. Furthermore, this demonstrates the promising capabilities for intensed pulsed light to reduce manufacturing costs and paves a roadmap for scalable and efficient PSCs on a roll-to-roll platform.

14 SOLAR ENERGY↗

Multi-junction Thin-film Solar Cells on Flexible Substrates for Space Power

The ultimate objective of the thin-film program at NASA GRC is development of a 20 percent AM0 thin-film device technology with high power/weight ratio. Several approaches are outlined to improve overall device efficiency and power/weight ratio. One approach involves the use of very lightweight flexible substrates such as polyimides (i.e., Kapton(Trademark)) or metal foil. Also, a compound semiconductor tandem device structure that can meet this objective is proposed and simulated using Analysis of Microelectronic and Photonic Structures (AMPS). AMPS modeling of current devices in tandem format indicate that AM0 efficiencies near 20 percent can be achieved. And with improvements in materials, efficiencies approaching 25 percent are achievable. Several important technical issues need to be resolved to realize these complex devices: development of a wide bandgap material with good electronic properties, development of transparent contacts, and targeting a 2-terminal device structure (with more complicated processing and tunnel junction) or 4-terminal device. Recent progress in the NASA GRC program is outlined.

Hepp, Aloysius F.↗

Spatial‐Uniformity–Driven Bayesian Optimization for Rapid Development of Printed Perovskite Solar Cells

Printed metal halide perovskites can enable rapid, roll-to-roll manufacturing of a broad class of optoelectronics—flexible solar cells and imagers among them—while promising cost and speed advantages over incumbent silicon. However, though current methods offer high throughput and patterning capabilities, perovskite films’ spatial heterogeneity remains a challenge for large-area devices. Here, a spatial-uniformity-driven Bayesian optimization (BO) approach is leveraged to accelerate the development of printed perovskite solar cells and improve large-area device performance. Using a BO surrogate model, a 6D design space of ink chemistry and printing physics is explored via extensive iterative experimentation (≈100) informed by an objective function capturing spatial photoluminescence (PL) variance. It is discovered that optimizing for uniformity drives rapid advances in photovoltaic performance, yielding ≈20% power conversion efficiency (PCE) for small area (0.134 cm 2 ) devices and > 16% for large area (1 cm 2 ) devices. This machine-learning approach simultaneously enables rheological comparison of ink formulations that accelerate the leveling of Saffman-Taylor artifacts and improve film uniformity. Here, this showcases uniformity-driven BO as an efficient approach for uncovering the key printing physics and mitigating spatial heterogeneity to enable device scaling beyond small cell areas.

14 SOLAR ENERGY↗

IPL-Annealed Mixed-Cation Perovskites with Robust Coating Window toward Scalable Manufacturing of Commercial Perovskite Solar Cells

Perovskite solar cells (PSCs) are a promising alternative solar technology, but the technical challenges of (1) stability/durability, (2) efficiency at scale, and (3) manufacturability must be overcome to achieve widespread PSC commercialization. The challenge of balancing solution ink formulation and scalable manufacturing is often overlooked in the literature, where focus is on adopting inks from processes that will not scale. In this study, we apply a classical roll-to-roll manufacturing perspective, utilizing both compositional engineering and intense pulsed light (IPL) annealing, to develop a mixed-cation perovskite ink with a robust coating window that simultaneously solve issues of stability and manufacturability for PSCs. Our method resulted in blade-coated, flexible, mixed-cation PSCs on ITO-PET substrates with a champion power conversion efficiency (PCE) efficiency of 16.7% using IPL annealing of the absorber layer and, to our knowledge, is one of the fastest processing methods for the perovskite layer. This overall reduction in processing time with a stable ink represents an advance toward the scaled production of perovskite solar cells on flexible substrates.

flexible perovskite solar cells↗

To grind or not to grind? The influence of mechanical and thermal treatments on the $\mathrm{Cu/Zn}$ disorder in $\mathrm{Cu}$ 2 $\mathrm{ZnSn}$($\mathrm{S}$ x $\mathrm{Se}$ 1-x ) 4 monograins

We report that Kesterite-type based thin film solar cell technologies are mainly based on polycrystalline absorber layers. A promising low cost alternative technology uses Cu 2 ZnSn(S x Se 1-x ) 4 (CZTSSe) monograins (single crystals of 20–100 μm size) which are fixed in a polymer matrix to form a flexible solar cell. The Cu/Zn disorder is discussed as a possible reason for band tailing causing voltage losses limiting the efficiency of CZTSSe-based devices. The experimental determination of the order parameter Q which is a quantitative measure of Cu/Zn disorder, requires a differentiation between the isoelectronic cations Cu + and Zn 2+ . An in-depth analysis of neutron diffraction data allows the determination of type and concentration of intrinsic point defects including a distinction between Cu and Zn. Neutron diffraction requires large sample volumes, thus monograins offer the unique possibility to correlate structural disorder in CZTSSe with device performance parameters. In this study we tackle the influence of grinding the monograins on stoichiometry deviations, the Cu/Zn disorder as well as intrinsic point defects and optoelectronic properties of CZTSSe monograins. Moreover, an easy methodology based on Raman scattering spectroscopy is proposed for the assessment of Cu/Zn disorder in the CZTSSe compounds.

14 SOLAR ENERGY↗

Synthetic Pathways to gamma-Graphyne and Related Allotropes of Carbon

Graphynes, two-dimensional carbon lattices combining sp 1 and sp 2 hybridized atoms, were predicted theoretically more than three decades ago, but few structures have been realized to date. These carbons are believed to possess remarkable mechanical and electronic properties, including high charge carrier mobilities comparable to those in graphene (10 4 to 10 5 cm 2 V -1 s -1 ). Unlike graphene, certain graphynes are predicted to be intrinsic semiconductors. Among these intriguing structures, γ-graphyne stands out as the structurally simplest and most symmetric sp 1 /sp 2 lattice. γ-Graphyne was first theorized in 1987. In contrast with graphene, γ-graphyne will be a semiconductor with a small band gap suitable for fabrication of electronic devices. This solves one of the fundamental problems of carbon-based electronics, the necessity for inducing a band gap in graphene. γ-Graphyne has the potential to form the basis for the next generation of carbon-based electronics operating at speeds unattainable by traditional silicon chips. Unlike silicon, γ-graphyne is a direct band gap semiconductor, and it will feature exceptional strength comparable to that of other 2D carbon allotropes. Such combination of properties may enable a new generation of highly efficient, ultra-light and flexible solar cells. Despite being a potentially “magical” material, γ-graphyne remained synthetically elusive for over three decades. The primary goals of this project were: (1) Synthesis of bulk γ-graphyne phases through solution-phase 2D polymerizations; (2) Experimental exploration of the physical and chemical properties of γ-graphyne; and (3) Mechanistic and theoretical studies of the novel chemical transformations developed in Goal 1. Common pyrolytic and vapor-deposition methodologies used for the synthesis of graphitic allotropes are unsuitable for graphyne and other sp 1 -contaning structures, as acetylenes readily convert to graphene and amorphous carbon at high temperatures. In contrast, this proposal is based on solution-based 2D polymerization. The major advantages of this approach over the traditional high temperature techniques are the potential to adjust the structure of the material with atomic precision, and the possibility of using structurally complex and relatively fragile repeat units. The outcomes of this research can revolutionize carbon nanotechnology, expanding the field’s structural toolbox beyond primarily graphitic and benzenoid structures. Understanding the chemistry of sp 1 carbon allotropes can lead to entirely new classes of structures with unique properties, including graphyne ribbons, nanotubes, quantum dots, and heterostructures with other 2D materials. Furthermore, the development of reliable and robust synthetic pathways towards periodic covalent molecular sheets with atomically precise structures shall have a profound impact on chemistry and materials science.

2D polymerization↗