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While perovskite photovoltaic (PV) devices are on the verge of their commercialization, promising methods to recycle or remanufacture fully-encapsulated perovskite solar cells (PSCs) and modules are still missing. Through detailed life-cycle assessment shown in this work, we identify that the majority of the greenhouse gas emissions can be reduced by re-using the glass substrate and parts of the PV cells. Based on these analytical findings, we develop a novel thermally-assisted mechanochemical approach to remove the encapsulants, the electrode and the perovskite absorber, allowing to re-use most of the device constituents for remanufacturing PSCs, which recovered nearly 90% of their initial performance. This remanufacturing strategy allows to save up to 33% of the module’s global warming potential. Finally, we demonstrate that the CO2-footprint of these remanufactured devices can become less than 30g/kWh, which is the value for state-of-the-art c-Si PV modules and can even reach 15g/kWh assuming a similar lifetime

Carbon-based electrodes have been widely applied in perovskite solar cells (PSCs) because of their chemical inertness and compatibility with up-scalable techniques, signifying their solid potential for mass-production. The material scarcity and complexity of metal ore extraction further highlights that conventionally used noble metal electrodes cannot represent a sustainable option for back-contact in PSCs, while cells with carbon-based electrodes represent an excellent solution to these problems. However, their power conversion efficiencies (PCEs) still lag behind the traditionally processed cells with metal electrodes, resulting in a considerable efficiency gap. To overcome this issue, we propose the use of low-temperature carbon-based (LTCB) electrodes, which offer several key advantages in comparison to mesoscopic high-temperature treated ones: (1) larger choice of selective layers, (2) applicability to all perovskite crystallization methods, (3) compatibility with flexible substrates and (4) faster deposition process. In this review, we analyze numerous techniques to formulate the LTCB-paste and ways to deposit it on the cell stack which have been developed in order to improve the interfacial contact and electrode conductivity. Besides describing the current state-of-the-art perovskite solar cells with LTCB-electrodes, the most promising strategies to enhance the PCE of such photovoltaic (PV) devices are discussed. Overall, we emphasize that PSCs with a LTCB-electrode combine high device stability, low manufacturing costs and low environmental impact, while having options for pushing the efficiency of carbon-based PSCs closer to the record-breaking cells, all of which are vital in order to fulfill the true potential of perovskite PV.

One of the main issues hindering the commercialization of perovskite photovoltaics (PV) is device stability. A myriad of various strategies to stabilize the perovskite layer against degradation under continuous illumination has been demonstrated in perovskite community, such as perovskite passivation with 2D perovskites, organic hydrophobic layers, ionic liquids, as well as the deployment of robust inorganic charge transport layers. However, for commercially established PV technologies, the most detrimental degradation occurs in fact under reverse bias. A cell in a module can be placed under reverse bias due to significant current mismatch between series-interconnected cells, which typically happens under operational conditions when shading takes place. Such situation causes the non-shaded solar cells to act as a reverse-bias voltage source on the shaded cell, causing it to operate at high negative voltages, dissipating its energy as heat producing a so-called This phenomenon is commonly known as "hot-spot" degradation and is considered to be one of the most severe degradation mechanisms even in crystalline silicon PV. Concomitantly, only few studies on the reverse bias degradation in perovskite PV devices have been published, revealing that this is a severe source of degradation. Thus, reverse bias degradation presents one of the most fundamental challenges for commercializing not only single-junction perovskite PV modules, but also the ones with tandem configurations. In this work, we demonstrate that perovskite PV devices with mesoscopic scaffold and carbon-based electrode have outstanding resilience against reverse bias degradation and are able to withstand negative voltages up to -9V. The presence of chemically inert carbon electrode, utilization of single-halide mixed-dimensional 2D/3D perovskite and robust inorganic charge transport layers helps to avoid commonly-occurring issues in state-of-the-art cells, like localized -melting of metal electrodes, ion diffusion and halide segregation. Looking more in-depth at the nature of reverse bias degradation in PSCs we demonstrate that the issue of iodine loss still prevails even in such stable devices. Low activation energy of I- vacancies causes an accumulation of charges at the interfaces, resulting in significant bend bending at the interfaces between perovskite and charge-transport layer. Under reverse bias the bending increases until the so-called "breakdown voltage" is reached beyond which holes are able to tunnel through to the valence band of perovskite. This hole-tunneling oxidizes incorporated iodine to create iodine vacancies and thermodynamically favorable iodine compounds, which decompose perovskite structure. Thus, iodine loss can cause device degradation, if it is exposed to reverse-bias for long time durations. For reverse bias voltages exceeding -9V, via thermographic imaging we overserved in-operando formation of hotspots and thermal degradation of perovskite into PbI2. To demonstrate that modules with carbon electrodes would be able to withstand hot-spot conditions, we manufactured modules with carbon back electrodes of 10x10cm2 size and 11.1% power conversion efficiency and subjected them to requirements of IEC61215 hot-spot test at an accredited laboratory Fraunhofer ISE PV Modules Testlab, which has never been done before according to our knowledge. Finally, the modules were able to pass the conditions of the IEC tests for c-Si and thin-film technologies confirming that mesoscopic scaffold and carbon electrodes provide effective stabilization strategy for perovskite PV devices against reverse-bias degradation. (Bogachuk et al. 2021) This work for the first time demonstrates that perovskite-based modules with carbon-based modules can withstand severe reverse bias, which is an essential attribute of this emerging technology on its path towards commercialization.

Carbon-electrode-based perovskite solar cells (C-PSCs) are promising candidates for commercialization due to their high stability. However, the absence of a hole selective layer (HSL) often limits their performance, yielding low fill factors (FFs). Herein, a certified FF of 78.8% obtained through HSL-free C-PSCs is focused. This is found to approach the highest values reported for metal-electrode-based PSCs employing highly selective HSLs. The loss mechanisms affecting the FF in fully printed HSL-free C-PSCs are thus investigated. Methods commonly used to analyze and quantify the impact of recombination and transport losses on the FF of established photovoltage devices are assessed, and their applicability in C-PSCs is examined. In the improved devices, non-radiative recombination contributes to only 3%abs loss with respect to the FF in the radiative limit, which is attributed to an optimal diode ideality factor approaching 1.0. Moreover, contributions of shunt resistive losses are determined to be negligible. Interfacial series resistance losses at the perovskite/carbon interface are identified as the main loss channel, highlighting the importance of the quality of the contact between the perovskite and the back-contact electrode.

The photocurrent density-voltage (J(V)) curve is the fundamental characteristic to assess opto-electronic devices, in particular solar cells. However, it only yields information on the performance integrated over the entire active device area. Here, a method to determine a spatially resolved photocurrent image by voltage-dependent photoluminescence microscopy is derived from basic principles. The opportunities and limitations of the approach are studied by the investigation of III-V and perovskite solar cells. This approach allows the real-time assessment of the microscopically resolved local J(V) curve, the steady-state Jsc, as well as transient effects. In addition, the measurement contains information on local charge extraction and interfacial recombination. This facilitates the identification of regions of non-ideal charge extraction in the solar cells and enables to link these to the processing conditions. The proposed technique highlights that, combined with potentiostatic measurements, luminescence microscopy turns out to be a powerful tool for the assessment of performance losses and the improvement of solar cells.

One of the major perovskites used as a light absorber in perovskite solar cells (PSCs) is methylammonium lead iodide (MAPI). MAPI perovskite shows many optimal optoelectronic properties making it a high-performance solar cell material. Nonetheless, PSCs face some limitations related to stability and degradation against moisture, and toxicity due their lead content. The goal of this work is to study the partial substitution of lead iodide (PbI2) with the inorganic compound copper iodide (CuI) to enhance the solar cell stability thanks to the hydrophobic properties of the latter. XRD showed a tetragonal crystal structure growth for the MAI[(PbI2)1−x(CuI)x] perovskite films. Even for 20 mol%, CuI was well incorporated into the perovskite lattice structure producing a slight change in the lattice parameters. SEM analysis showed a clear improvement of the film’s morphology with the CuI substitution (less pinholes, better uniformity). The optical absorption edges and calculated optical bandgap, around 1.55 eV, remain unchanged with CuI partial substitution. With the increase in CuI/PbI2 ratio photovoltaic properties of the MAI[(PbI2)1−x(CuI)x] devices improved, higher VOC and JSC are observed. Finally, the stability was studied during 150 days in air and an enhancement of PSCs properties was observed for CuI substituted PbI2 PSCs.

Interface engineering and passivating contacts are key enablers to reach the highest efficiencies in photovoltaic devices. While printed carbon-graphite back electrodes for hole-transporting material (HTM)-free perovskite solar cells (PSCs) are appealing for fast commercialization of PSCs due to low processing costs and extraordinary stability, this device architecture so far suffers from severe performance losses at the back electrode interface. Herein, a 2D perovskite passivation layer as an electron blocking layer (EBL) at this interface to substantially reduce interfacial recombination losses is introduced. The formation of the 2D perovskite EBL is confirmed through X-ray diffraction, photoemission spectroscopy, and an advanced spectrally resolved photoluminescence microscopy mapping technique. Reduced losses that lead to an enhanced fill factor and V-OC are quantified by electrochemical impedance spectroscopy and J(SC)-V-OC measurements. This enables reaching one of the highest reported efficiencies of 18.5% for HTM-free PSCs using 2D perovskite as an EBL with a significantly improved device stability.

Funder: UNIQUE, Funder: National University of Ireland Travelling Studentship, Funder: Engineering and Physical Sciences Research Council; Id: http://dx.doi.org/10.13039/501100000266, Funder: Cambridge Trust Scholarship, Funder: Robert Gardiner Scholarship, Carbon-based electrodes represent a promising approach to improve stability and up-scalability of perovskite photovoltaics. The temperature at which these contacts are processed defines the absorber grain size of the perovskite solar cell: in cells with low-temperature carbon-based electrodes (L-CPSCs), layer-by-layer deposition is possible, allowing perovskite crystals to be large (>100 nm), while in cells with high-temperature carbon-based contacts (H-CPSCs), crystals are constrained to 10-20 nm size. To enhance the power conversion efficiency of these devices, the main loss mechanisms were identified for both systems. Measurements of charge carrier lifetime, quasi-Fermi level splitting (QFLS) and light-intensity-dependent behavior, supported by numerical simulations, clearly demonstrate that H-CPSCs strongly suffer from non-radiative losses in the perovskite absorber, primarily due to numerous grain boundaries. In contrast, large crystals of L-CPSCs provide long carrier lifetime (1.8 µs) and exceptionally high QFLS of 1.21 eV for an absorber bandgap of 1.6 eV. These favorable characteristics explain the remarkable open-circuit voltage (VOC) of over 1.1 V in hole-selective layer-free L-CPSCs. However, the low photon absorption and poor charge transport in these cells limit their potential. Finally, effective strategies are provided to reduce non-radiative losses in H-CPSCs, transport losses in L-CPSCs and to improve photon management in both cell types.