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Highly Efficient Large-area Perovskite Solar Cells

Periodic Reporting for period 1 - LrgPSCs (Highly Efficient Large-area Perovskite Solar Cells)

Période du rapport: 2021-09-01 au 2023-08-31

The Action “Highly Efficient Large-area Perovskite Solar Cells (LrgPSCs)” aims to address the scaling challenges in emerging perovskite photovoltaics. While solar energy is crucial for a sustainable energy future, the high-temperature processing of silicon photovoltaics raises sustainability concerns. Perovskite solar cells (PSCs), with their excellent performance, low costs, and solution processability, emerge as a promising alternative. However, their commercialization is stalled by the absence of efficient large-scale solar modules. This issue stems from the increasing complexity in controlling perovskite crystallization for larger film areas, leading to non-uniform film formation and reduced crystalline quality. Additionally, the scalability of essential interface engineering strategies is challenged by strict requirements on interlayer thicknesses.

The large-scale deployment of efficient perovskite solar cells (PSCs) holds significant societal implications. Economically, 20% PCE PSCs could potentially lower the levelized cost of electricity to below 3 ¢/kWh, offering a competitive advantage over the 3.5–5 ¢/kWh of commercial silicon solar cells and promoting a shift from fossil fuels. This aids efforts in climate change mitigation. PSCs' adaptable thin-film architectures enable diverse applications in wearable electronics and the Internet of Things. Their lightweight, semitransparent modules can be integrated into building facades, windows, and vehicles, easing land-use conflicts for photovoltaic installations in populated European regions. Furthermore, PSCs have a significantly lower carbon footprint than commercial silicon, reducing the energy payback time to just four months and offering more sustainable end-of-life recycling options, avoiding landfill disposal.

This Marie Skłodowska Curie Action (MSCA) aimed to address research gaps in developing perovskite solar modules (PSMs) by focusing on four key areas: controlling perovskite crystallization, overcoming conductivity issues in 2D/3D heterostructures, integrating materials strategies for over 20% PCE in large-area PSMs, and employing advanced characterization techniques for fundamental understandings. A significant aspect was also to support the career development of the experienced researcher (ER).

In conclusion, this MSCA introduced innovative methods in perovskite formation and interface engineering, utilizing new dye molecule-based additives and scalable surface passivation with non-invasive ammonium ligands. It emphasized the role of systematic surface-sensitive characterizations in accelerating materials development. These efforts resulted in PSMs with PCEs of 20.8% and 20.5% in normal and inverted device architectures, respectively, documented in publications in Science and Advanced Materials. This work, aligning with Horizon 2020's goals, has laid a foundation for the commercialization of PSCs by demonstrating efficient large-area devices.
This 24-month MSCA, organized into six Work Packages (WPs), balanced technical (WP1-3) and non-technical aspects (WP4-6).

In WP1, studies on modifying perovskite film crystallization with molecular additives resulted in a journal publication and conference presentation. Characterization techniques such as X-ray diffraction and microscopic characterizations assessed film quality and homogeneity, contributing to centimeter-scale solar cell fabrication.

WP2 focused on developing interface engineering with structure-tailored ammonium ligands, yielding a conference presentation, a Science publication, and an accepted Nature manuscript. Over 10 ammonium ligands were investigated for their interactions with perovskite films, using various spectroscopy and X-ray scattering methods, leading to both small and large-area perovskite solar cell fabrication.

WP3 combined WP1 and WP2 discoveries to demonstrate efficient perovskite solar modules, achieving 20.5% and 20.8% PCE for inverted and normal-structure perovskite solar cells, respectively. The ER also tested the device stability, achieving long-term (>1000 hour) operating stability under ISOS-L-2 and ISOS-L-3 levels.

The project was managed under WP4. In WPs 5 and 6, the ER attended 3 conferences and 5 workshops on teaching, leadership, and diversity. He gave 2 seminars at top universities and two lectures on next-generation photovoltaics. Demonstrating leadership in publication and research, he mentored two early career researchers and joined the young editorial boards of Nanoenergy Advances and EcoEnergy. He is now organizing a special issue on perovskite solar cell stability. During the grant period, the ER was interviewed by MIT Technology Review (China) and honored with a Forbes 30 under 30 (Europe) award for his contributions to renewable energy research.

As an overview, the results of this MSCA are reported in: (1) one paper in Advanced Materials on the impact of dye molecule additive to modulate perovskite formation and establish buried interface passivation in a self-assembled fashion; (2) one paper in Science on the reactivity of ammonium ligands with perovskite films, and how minimized ligand interaction benefits large-area device demonstration; (3) a forthcoming paper in Nature on improving hole-selective contact for efficient and stable perovskite solar cells. These results, already disseminated at international conferences, will make an impact within the photovoltaic community. Some of these findings have been utilized as supporting data for H2020 funding applications.
This MSCA has propelled next-generation photovoltaics by:

(1) Publishing a paper in Advanced Materials that reported the first large-area perovskite solar cells that passed accelerated aging tests under ISOS-L-2I standards, introducing an effective dye additive engineering approach for enhanced stability and performance.

(2) A paper in Science highlighted the first efficient (>20% PCE) perovskite solar cells operating at 85°C and 50% relative humidity with a lifetime over 1000 hours, introducing non-reactive ammonium ligands for interface stabilization.

(3) A forthcoming Nature paper reported a PCE record (24.8%) for inverted perovskite solar cells, presenting an innovative efficiency improvement approach and offering new insights into SAM formation for solar cell applications.

Additionally, the MSCA enhanced methodological advancements beneficial to the broader scientific community. Collaboration with computational scientists using MD simulations has provided deeper insight into molecular interactions on metal oxide surfaces, aiding in the understanding of interface formation as a function of molecular structures. The ER has also combined advanced surface characterization techniques, revealing comprehensive details of surface interaction and phase conversion at the nanometer scale.

Anticipated impacts of this MSCA include pioneering directions in perovskite solar module demonstration, utilizing various high-planarity dye molecules and non-invasive ammonium ligands for effective interfacial passivation. Enhanced by MD simulations, the surface characterization techniques could guide future nanoscale surface chemistry development in next-generation optoelectronics. The socio-economic impact underscores the advancement of perovskite photovoltaic commercialization, contributing to reduced solar energy costs and aligning with global sustainability efforts for accelerated energy transition.
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