Charge Recombination Centers Research Articles

Electroactive and Self‐healing Polyurethane Doped Tin Oxide Interlayers for Efficient Organic Solar Cells†

Comprehensive SummaryTin oxide (SnO2) has been widely used as an electron transport layer (ETL) in optoelectronic devices. However, there are numerous surface or bulk defects in SnO2, working as charge recombination centers to degrade device. Here, an electroactive and self‐healing polyurethane (PHNN) was designed by integrating conjugated unit – naphthalene diimide (NDI) into a typical polyurethane backbone. Numerous hydrogen bonds and π interactions in PHNN work as non‐covalent interactions to endow this polymer with superior self‐healing properties. PHNN contains lots of aliphatic amine and carbonyl groups, which effectively passivate the defects in SnO2. The π stacking of NDI units will facilitate electron delocalization, endowing PHNN with electrical activity compared with traditional polyurethane. Doping SnO2 with PHNN can improve the conductivity and reduce the work function of SnO2 layer, which is conducive to efficient charge extraction and transport. Using PHNN doped SnO2 as ETL for PM6: Y6 and PM6: BTP‐eC9 based inverted organic solar cells can achieve a high efficiency of 17.16% and 17.51%, respectively. Devices containing doped SnO2 ETL show significantly improved efficiency and stability. Thus, the electroactive polyurethane doped SnO2 interlayers show high performance interfacial modification to align energy‐levels in solar cell devices, which have promising applications in organic electronics.

Dual Hole Transport Layers Heterojunction and Band Alignment Engineered Mo:BiVO4 Photoanodes for Efficient Water Splitting.

BiVO4-based photoanode is one of the most promising photoanodes for photoelectrocatalytic water splitting. However, the serious problem of interface charge recombination limits its further development. Here, a Mo:BiVO4/NiOx/CPF-TCzB/NiCoBi photoanode is constructed with double hole transport layer and an energy level gradient to achieve an effective photo-generated holes extraction and accumulation at the surface electrocatalyst. The conjugated polycarbazole framework CPF-TCzB is used as hole transport layer to eliminate the charge recombination center between Mo:BiVO4 and NiCoBi electrocatalyst and realize the extraction and storage of photo-generated hole; NiOx nanoparticles are further inserted between Mo:BiVO4 and CPF-TCzB to form a gradient energy level, eliminating the energy level barrier and optimizing band alignment. As a result, Mo:BiVO4/NiOx/CPF-TCzB/NiCoBi achieves a much higher photocurrent densities of 3.14mA cm-2 than that of Mo:BiVO4 (0.42mA cm-2) at 0.6V versus RHE. This work provides an specific way to adjust the band structure of BiVO4-based photoanodes and realize efficient hole extraction and storage for PEC water splitting.

CdS quantum dots sensitized Ti-MOFs as high-performance photocathodic materials for immunoassay of alpha-fetoprotein based on Ag+ exchange strategy

Cathodic photoelectrochemical (PEC) analysis has drawn much attention because of its excellent anti-interference capability toward reductive substances in samples, but the development high-performance photocathodic materials is challenging. We report here CdS quantum dots (QDs) sensitized titanium-based metal–organic frameworks (Ti-MOFs) as high-performance photocathodic materials for ultrasensitive immunoassay of alpha-fetoprotein (AFP) based on Ag+ exchange strategy. Due to the excellent sensitization effect of CdS QDs, the photocathodic current of CdS QDs decorated MIL-125-NH2(Ti) is 25-fold that of MIL-125-NH2(Ti) alone. The photocathodic current of CdS/MIL-125-NH2(Ti) can be quenched after Ag+ exchange, because CdS is partially converted to Ag2S that serves as a charge-recombination center. Based on the PEC response of CdS/MIL-125-NH2(Ti) to Ag+, a cathodic PEC immunoassay platform is constructed for AFP detection by using CdS/MIL-125-NH2(Ti) as the photoactive material and Ag nanoparticles modified SiO2 nanospheres as labels. The linear range for AFP detection is from 1.0 × 10−4 to 1.0 × 102 ng mL−1, and the detection limit is 20 fg mL−1. The constructed PEC immunosensor is successfully used for detecting AFP in human serum samples. In this work, a novel and high-performance photoactive material is developed for cathodic PEC analysis, and a simple and effective PEC immunoassay platform for AFP detection is constructed based on Ag+ exchange strategy.

Engineering Ba2Bi2O6 Double Perovskite with La3+ for High Current Density Visible Light Photoelectrochemical Hydrogen Evolution.

A Lanthanum ion (La3+) incorporation strategy is implemented to modify Ba2Bi2O6-based double perovskite photoelectrodes. X-ray diffraction (XRD) characterization shows that highly crystalline Ba2La0.4Bi1.6O6 double perovskites with the space group I2/m are successfully prepared. UV-vis absorption spectra and the Tauc-plot reveal an optical band gap Eg ≈1.57 ± 0.01eV. A thickness dependence of the photoelectrodes photoelectrochemical (PEC) performance shows that the submicron (≈1µm) 4-times spin-coated thin film photoelectrode displays strong p-type conductivity, which delivers an encouraging photocurrent density of 0.88mAcm-2 at 0.25VRHE under AM 1.5G illumination. 10-times coated and 20-times coated medium thick (125.8-197µm) photoelectrodes that exhibit moderate p-type conductivity, show further enhanced photocurrent densities of 1.5mAcm-2 at 0VRHE. In contrast, charge recombination centers existing in a standard thick pellet (≈500µm) Ba2La0.4Bi1.6O6 photoelectrode can quench photo-generated charge carriers and greatly undermine PEC activities. The approach to doping at the Bi(III) sites contrasts with earlier efforts that focus on doping at the Bi(V) sites and thus paves the way for further tailoring a family of novel promising photocathode materials for efficient solar-water conversion devices.

A bithiophene-cored interfacial passivating layer for Sb2S3 solar cells with 7.1% efficiency

Sb2S3, which is an excellent performance of the third generation of solar cells with superior photovoltaic properties, high stability and environmental friendliness. However, because of the low formation energies of the cation-replaced-anion antisites and anion vacancies, the presence of these trap states result in increased unpaired Sb atoms, which could serve as charge recombination centers on the surface and grain boundaries. Here, we introduce a bithiophene-cored compound (BTR-TPA, 4,4'-([2,2′-bithiophene]-5,5′-diyl)bis(N,N-bis(4-methoxyphenyl)aniline)) as an interlayer between the Sb2S3 and hole transport layers to passivate the trap states. Suitable energy levels, inhibited antimony oxide impurity phase, low trap states together with remarkable photoelectric properties are obtained via introducing such an interface layer. As a result, the optimal power conversion efficiency (PCE) of Sb2S3 solar cells is raised from 6.25% (control device) to 7.12%. This research demonstrates that interface passivation is an effective means of enhancing the PCE of Sb2S3 solar cells.

Charge Transport Enhancement in BiVO4 Photoanode for Efficient Solar Water Oxidation.

Photoelectrochemical (PEC) water splitting in a pH-neutral electrolyte has attracted more and more attention in the field of sustainable energy. Bismuth vanadate (BiVO4) is a highly promising photoanode material for PEC water splitting. Additionally, cobaltous phosphate (CoPi) is a material that can be synthesized from Earth's rich materials and operates stably in pH-neutral conditions. Herein, we propose a strategy to enhance the charge transport ability and improve PEC performance by electrodepositing the in situ synthesis of a CoPi layer on the BiVO4. With the CoPi co-catalyst, the water oxidation reaction can be accelerated and charge recombination centers are effectively passivated on BiVO4. The BiVO4/CoPi photoanode shows a significantly enhanced photocurrent density (Jph) and applied bias photon-to-current efficiency (ABPE), which are 1.8 and 3.2 times higher than those of a single BiVO4 layer, respectively. Finally, the FTO/BiVO4/CoPi photoanode displays a photocurrent density of 1.39 mA cm-2 at 1.23 VRHE, an onset potential (Von) of 0.30 VRHE, and an ABPE of 0.45%, paving a potential path for future hydrogen evolution by solar-driven water splitting.

Improving the Solar Energy Utilization of Perovskite Solar Cells via Synergistic Effects of Alkylamine and Alkyl Acid on Defect Passivation

Defects in perovskite film are sources of charge recombination centers, which are detrimental to the performance of perovskite solar cells (PSCs). To decrease the density of defects, dodecylamine (DAM), dodecylic acid (DAC), and 12‐aminolauric acid (ALA) are utilized as additives to prepare methyl ammonium lead iodide (MAPbI3) perovskite films. Herein, the passivation effects of these molecules on the properties of the MAPbI3 films and the performances of the corresponding PSCs are studied. The results show that DAM and DAC which contain –NH2 and –COOH groups, respectively, can increase the PCEs of the devices. This result implies that both groups serve as the Lewis base, passivating the defects of undercoordinated Pb2+. For the ALA molecules, the –NH2 and –COOH groups are present simultaneously at the two ends of the molecule; the passivation ability is more significant than the others, which is attributable to the synergistic effects of the two groups. By the passivation of ALA, the PCE of the PSC can increase from 18.42% to 19.96% under one sun illumination. Furthermore, the treatments of the passivation agents also increase the hydrophobicity of the perovskite films, improving the stability of the PSCs.

Enhanced electron density of the π-conjugated structure and in-plane charge transport to boost photocatalytic H2 evolution of g-C3N4

Graphite carbon nitride (g-C3N4) has become an emerging metal-free photocatalyst and attracted the attention of researchers. However, pure g-C3N4 (PCN) prepared by traditional thermal condensation polymerization has a low polymerization of heptazine ring chains and a large number of charge recombination centers, which hinder in-plane charge transport, leading to undesirable photocatalytic performance. Herein, PCN fabrication by thermal treatment with ammonium oxalate monohydrate was performed to produce highly dispersed porous g-C3N4 nanosheets, and the integrity of their in-plane heptazine ring chains was successfully improved without introducing heteroatoms. Electron paramagnetic resonance and 13C nuclear magnetic resonance analyses revealed significantly increased electron density and delocalization of the π-conjugated structure. The obtained samples exhibited acceptable stability and photocatalytic activity, and the hydrogen reduction rates without and with the Pt co-catalyst were 11.2 and 5.3 times that of PCN.

Charge Separation in BaTiO3 Nanocrystals: Spontaneous Polarization Versus Point Defect Chemistry.

The fate of photogenerated charges within ferroelectric metal oxides is key for photocatalytic applications. The authors study the contributions of i) tetragonal distortion, responsible for spontaneous polarization, and ii) point defects, on charge separation and recombination within BaTiO3 (BTO) nanocrystals of cubic and tetragonal structure. Electron paramagnetic resonance (EPR) in combination with O2 photoadsorption experiments show that BTO nanocrystals annealed at 600 °C have a charge separation yield enhanced by a factor > 10 compared to TiO2 anatase nanocrystals of similar geometries. This demonstrates for the first time the beneficial effect of the BTO perovskite nanocrystal lattice on charge separation. Strikingly, charge separation is considerably hindered within BTO nanoparticles annealed ≥ 600 °C, due to the formation of Ba-O divacancies that act as charge recombination centers. The opposing interplay between tetragonal distortion and annealing-induced defect formation inside the lattice highlights the importance of defect engineering within perovskite nanoparticles.

Enhancing the photoelectrochemical activity of monoclinic BiVO4 by discretizing oxygen vacancies: insights from DFT calculations.

Monoclinic bismuth vanadate (BiVO4) has emerged as an excellent optically active photoanode material due to its unique physical and chemical properties. Experiments reported that the low concentration of oxygen vacancies enhances the photoelectrochemical (PEC) activity of BiVO4, but the high concentration of oxygen vacancies decreases the charge carrier lifetime. Using time-domain density functional theory and molecular dynamics, we have demonstrated that the distribution of oxygen vacancies has strong effects on the static electronic structure and nonadiabatic (NA) coupling of the BiVO4 photoanode. The localized oxygen vacancies create charge recombination centers within the band gap and enhance the NA coupling between the VBM and the CBM, resulting in fast charge and energy losses. By contrast, the discrete oxygen vacancies can eliminate the charge recombination centers and decrease the NA coupling between the VBM and the CBM, enhancing the PEC activity of monoclinic BiVO4. Our study suggests that the PEC performance of a photoanode can be improved by changing the distribution of oxygen vacancies.

Regulating excitonic effects in non-oxide based XPSe3 (X = Cd, Zn) monolayers towards enhanced photocatalysis for overall water splitting.

The non-oxide 2D materials have garnered considerable interest due to their potential utilization as photocatalysts, which offer a superior substitute to metal-oxide-based photocatalysts. This study investigates the impact of the dielectric environment on the size and binding energy of excitons in atomically thin, experimentally synthesized semiconducting monolayers [XPSe3, X = (Cd, Zn)] to address the critical problem of electron-hole recombination, which significantly hinders the efficiency of most photocatalysts. We employ a precise non-hydrogenic model surpassing the hydrogenic-based Mott-Wannier model. Our findings are among the first few demonstrations of an increase in exciton size (and decrease in exciton binding energy) as environmental screening increases. These findings have implications for photocatalytic water splitting and are not limited to metal phosphorus trichalcogenides, but can be applied to other classes of 2D materials as well. This work also compares metal-oxide photocatalysts, which have been the focus of much research over the past five decades, to non-oxide-based metal phosphorus trichalcogenide photocatalysts, which offer a superior alternative due to their ability to address issues such as light-harvesting inability in the visible spectrum and unwanted charge recombination centres. Furthermore, the implications of this study extend beyond photocatalysts and are significant for the design and development of next-generation optoelectronic devices that incorporate excitonic processes, such as solar cells, photodetectors, LEDs, etc.

Enhance the photoconversion efficiency of carbon-based perovskite solar cells through the synergetic effect of upconversion nanoparticles Li doped NaYbF4:Ho3+ and 2D g-C3N4

Li doped NaYbF 4 :Ho 3+ -C 3 N 4 (UCNPs-C 3 N 4 ) nanocomposites were successfully prepared and applied in perovskite solar cells (PSCs). The photoelectric conversion efficiency of the modified PSCs can be increased from 11.01% to 14.78%. The improved efficiency can be attributed to the synergistic effect of Li doped NaYbF 4 :Ho 3+ (UCNPs) and 2D g-C 3 N 4 (C 3 N 4 ). On the one hand, UCNPs can continuously absorb two or more low-energy photons and emit one high-energy photon, which allows UCNPs to improve the ability of perovskite layers to capture near-infrared light and convert it into visible light. The perovskite photosensitive layers will further absorb the converted visible light energy, and generate additional photocurrent. On the other hand, g-C 3 N 4 exhibits high electrical conductivity and reduces its intrinsic defect density by effectively passivating the grain boundaries of the charge recombination centers. By performing hydrothermal loading experiments on UCNPs and g-C 3 N 4 , the defect of poor electrical conductivity of UCNPs can be significantly improved. The prepared composite material has higher absorption and utilization rate of sunlight. In conclusion, the synthesized composites are not only beneficial to passivate the defects in the perovskite layer, but also improve the short-circuit current density ( J SC ) and photoconversion efficiency (PCE) of the device. Mechanism of NIR sunlight harvesting in the schematic diagram of PSCs • Upconversion nanoparticles (UCNPs) and two-dimensional graphitic carbon nitride (2D g-C 3 N 4 ) were successfully compounded. • UCNPs convert near-infrared light (NIR) into visible light (VIS). • 2D g-C 3 N 4 can reduce defect density of the perovskite layer. • The poor conductivity of UCNPs are increased by 2D g-C 3 N 4 . • The efficiency of device was optimized from 11.01% to 14.78% due to the synergistic effect of nanocomposites.

Dual-Functional 3-Acetyl-2,5-dimethylthiophene Additive-Assisted Crystallization Control and Trap State Passivation for High-Performance Perovskite Solar Cells

Defect-mediated charge recombination and successive degradation mainly lag the performance of perovskite solar cells (PSCs). Insufficiency or evaporation of organic cations leaves behind the undercoordinated Pb2+ ions, which act as severe charge recombination centers. Herein, theoretical and experimental insights into crystallization control and defect passivation of MAPbI3 perovskite by the dual-functional 3-acetyl-2,5-dimethylthiophene (ADT) molecule are presented. Density functional theory calculations show that both functional groups of ADT possessing different interaction energies could interact with PbI2. The carbonyl group in ADT shows the dominant interaction with Pb2+ forming an intermediate product that might decrease the crystallization rate. Further, the coordinate bonding between ADT and uncoordinated Pb2+ ions in perovskite leads to defect passivation. The 0.6% ADT-modified PSCs possess an average power conversion efficiency (PCE) of 18.22 ± 0.80% and the highest PCE of 19.03%, whereas the pristine PSCs exhibit an average PCE of 16.23 ± 1.32% and the highest PCE of 17.47%. Furthermore, the modified PSCs maintain 80% of the initial PCE up to 650 h during storage at ambient conditions (RH = 35 ± 5%). The present study shows that the simultaneous crystalization control and defect passivation achieved via an ADT additive engineering approach could be an efficient strategy to enhance the PCE and stability of PSCs.

Plasmonic Effects of Au@Ag Nanoparticles in Buffer and Active Layers of Polymer Solar Cells for Efficiency Enhancement.

Embedding nanoparticles (NPs) in the buffer layer of bulk heterojunction polymer solar cells (BHJ PSCs) excites the surface plasmonic polaritons and enhances the pathlength of the light in the solar cells. On the other hand, embedding NPs in the active layer significantly improves absorption and increases the production of electron-hole (e-h) pairs in BHJ PSCs. Increasing the volume ratio of NPs embedded in BHJ PSCs enables the direct interfacing of the NPs with the active layer, which then serves as a charge recombination center. Therefore, this study integrates the aforementioned phenomena by exploiting the effects of embedding plasmonic Au@Ag NPs in the buffer and active layers of PSC and then determining the optimum volume ratio of Au@Ag NPs. The results show the absorption is increased across the 350–750 nm wavelength region, and the PCE of the device with embedded Au@Ag in two locations is enhanced from 2.50 to 4.24%, which implies a 69.6% improvement in the PCE in comparison to the reference cell. This improvement is contributed by the combined localized surface plasmon resonance (LSPR) effects of multi-positional Au@Ag NPs, spiky durian-shaped morphology of Au@Ag NPs, and optimized volume ratio of Au@Ag NPs embedded in the PEDOT: PSS and PTB7:PC71BM layers.

Photocatalytic degradation of phenol by core–shell Cu@TiO2 nanostructures under visible radiation

Even allowing high degradation efficiency, TiO2 does not support many large-scale applications, mainly due to the high operational cost related to the use of artificial radiation sources. On the other hand, it is well known that the TiO2 response to solar radiation can be increased by association with noble metals, due to the phenomenon of surface plasmonic resonance. Thus, the present study aimed to prepare copper nanoparticles and their incorporation into commercial titania (Evonik Aeroxide P-25) by the wet impregnation method. Characterization studies confirmed the formation of a core–shell nanostructure (Cu@TiO2) formed by irregular shape particles with a mean size between 20 and 30 nm. The incorporation of Cu significantly reduced the optical bandgap energy (Eg) of the materials, ranging from 3.17 eV for TiO2 P-25 to 2.67 eV for Cu@TiO2 materials containing 3.0% of copper. Characterization studies carried out by cathodoluminescence shown that high concentrations of copper reduced the lifetime of photogenerated electrons and holes, which suggests its role as a charge recombination center. Thus, the presence of copper decreased the efficiency of TiO2 on the UV–Vis mediated photocatalytic degradation of phenol, while in the presence of visible radiation only Cu@TiO2 materials containing 0.5% of copper showed high degradation efficiency.

Simultaneous Optimization of Charge Transport Properties in a Triple-Cation Perovskite Layer and Triple-Cation Perovskite/Spiro-OMeTAD Interface by Dual Passivation.

Molecular engineering of additives is a highly effective method to increase the efficiency of perovskite solar cells by reducing trap states and charge carrier barriers in bulk and on the thin film surface. In particular, the elimination of undercoordinated lead species that act as the nonradiative charge recombination center or contain defects that may limit interfacial charge transfer is critical for producing a highly efficient triple-cation perovskite solar cell. Here, 2-iodoacetamide (2I-Ac), 2-bromoacetamide (2Br-Ac), and 2-chloroacetamide (2Cl-Ac) molecules, which can be coordinated with lead, have been used by adding them into a chlorobenzene antisolvent to eliminate the defects encountered in the triple-cation perovskite thin film. The passivation process has been carried out with the coordination between the oxygen anion (−) and the lead (+2) cation on the enolate molecule, which is in the resonance structure of the molecules. The Spiro-OMeTAD/triple-cation perovskite interface has been improved by surface passivation by releasing HX (X = I, Br) as a byproduct because of the separation of alpha hydrogen on the molecule. As a result, a solar cell with a negligible hysteresis operating at 19.5% efficiency has been produced by using the 2Br-Ac molecule, compared to the 17.6% efficiency of the reference cell.

Ag-Bi Charge Redistribution Creates Deep Traps in Defective Cs2AgBiBr6: Machine Learning Analysis of Density Functional Theory.

Lead-free double perovskites hold promise for stable and environmentally benign solar cells; however, they exhibit low efficiencies because defects act as charge recombination centers. Identifying trap-assisted loss mechanisms and developing defect passivation strategies constitute an urgent goal. Applying unsupervised machine learning to density functional theory and nonadiabatic molecular dynamics, we demonstrate that negatively charged Br vacancies in Cs2AgBiBr6 create deep hole traps through charge redistribution between the adjacent Ag and Bi atoms. Vacancy electrons are first accepted by Bi and then shared with Ag, as the trap transforms from shallow to deep. Subsequent charge losses are promoted by Ag and Bi motions perpendicular to rather than along the Ag-Bi axis, as can be expected. In contrast, charge recombination in pristine Cs2AgBiBr6 correlates most with displacements of Cs atoms and Br-Br-Br angles. Doping with In to replace Ag at the vacancy maintains the electrons at Bi and keeps the trap shallow.

Dithiol surface treatment towards improved charge transfer dynamic and reduced lead leakage in lead halide perovskite solar cells

AbstractWith efficiency surpassing 25%, perovskite solar cells (PSCs) have received much attention because of their excellent potential in photovoltaic field. However, there are some challenging issues still exist which need to be addressed. One issue is that the surface/interface and grain boundaries related defects and traps could work as charge recombination centers during the device operation, compromising the charge transfer as well as the device performance. Another issue is the leakage of toxic Pb, which may cause undesired contamination to water or soil and make devices not appropriate to work outdoors. Herein, the dithiol molecule was introduced to passivate surface defects and traps as well as reduce the Pb leakage. The unsaturated Pb2+ usually acting as recombination centers could coordinate with thiol group to reduce the recombination. Meanwhile, the beneficial band bend was observed, which facilitates the interface charge transfer. Crucially, we confirmed dithiol molecule could help reduce the Pb leakage. Retarded dissolution of PbI2 into water was observed for perovskite films after dithiol treatment, which eventually contributed less Pb leakage. Overall, this study proposes a universal strategy for defects passivation and reduced lead leakage, which is promising for environmental stable optoelectronic applications.image

Ultrathin carbon interim layer encapsulation for constructing p − n heterojunction photoanode towards photoelectrochemical water splitting

Interfacial charge transfer and separation are both critical to the solar energy conversion efficiency, whereas it remains an enduring challenge. This work demonstrates the synergetic enhancement of interfacial charge transfer efficiency and bulk charge separation by depositing p-type Co3O4 cocatalyst onto n-type TiO2 nanotube arrays (TNTAs) that are uniformly coated with an ultrathin carbon layer, forming a p − n Co3O4/TNTAs heterojunction. Being highly dispersed on the surface of photoanodes, Co3O4 quantum dots retard forming charge recombination centers at the photoanode/cocatalyst interface, which facilitates hole transport. Simultaneously, ultrathin intermediate carbon layer boosts interfacial electron transfer kinetics, resulting in effective spatial charge separation and considerably improved photoelectrochemical (PEC) water splitting performances.

Exploring the Effect of Ammonium Iodide Salts Employed in Multication Perovskite Solar Cells with a Carbon Electrode.

Perovskite solar cells that use carbon (C) as a replacement of the typical metal electrodes, which are most commonly employed, have received growing interest over the past years, owing to their low cost, ease of fabrication and high stability under ambient conditions. Even though Power Conversion Efficiencies (PCEs) have increased over the years, there is still room for improvement, in order to compete with metal-based devices, which exceed 25% efficiency. With the scope of increasing the PCE of Carbon based Perovskite Solar Cells (C-PSCs), in this work we have employed a series of ammonium iodides (ammonium iodide, ethylammonium iodide, tetrabutyl ammonium iodide, phenethylammonium iodide and 5-ammonium valeric acid iodide) as additives in the multiple cation-mixed halide perovskite precursor solution. This has led to a significant increase in the PCE of the corresponding devices, by having a positive impact on the photocurrent values obtained, which exhibited an increase exceeding 20%, from 19.8 mA/cm2, for the reference perovskite, to 24 mA/cm2, for the additive-based perovskite. At the same time, the ammonium iodide salts were used in a post-treatment method. By passivating the defects, which provide charge recombination centers, an improved performance of the C-PSCs has been achieved, with enhanced FF values reaching 59%, which is a promising result for C-PSCs, and Voc values up to 850 mV. By combining the results of these parallel investigations, C-PSCs of the triple mesoscopic structure with a PCE exceeding 10% have been achieved, while the in-depth investigation of the effects of ammonium iodides in this PSC structure provide a fruitful insight towards the optimum exploitation of interface and bulk engineering, for high efficiency and stable C-PSCs, with a structure that is favorable for large area applications.