RESUMEN
Two-dimensional (2D) and three-dimensional (3D) perovskite heterostructures have played a key role in advancing the performance of perovskite solar cells1,2. However, the migration of cations between 2D and 3D layers results in the disruption of octahedral networks, leading to degradation in performance over time3,4. We hypothesized that perovskitoids, with robust organic-inorganic networks enabled by edge- and face-sharing, could impede ion migration. We explored a set of perovskitoids of varying dimensionality and found that cation migration within perovskitoid-perovskite heterostructures was suppressed compared with the 2D-3D perovskite case. Increasing the dimensionality of perovskitoids improves charge transport when they are interfaced with 3D perovskite surfaces-this is the result of enhanced octahedral connectivity and out-of-plane orientation. The 2D perovskitoid (A6BfP)8Pb7I22 (A6BfP: N-aminohexyl-benz[f]-phthalimide) provides efficient passivation of perovskite surfaces and enables uniform large-area perovskite films. Devices based on perovskitoid-perovskite heterostructures achieve a certified quasi-steady-state power conversion efficiency of 24.6% for centimetre-area perovskite solar cells. We removed the fragile hole transport layers and showed stable operation of the underlying perovskitoid-perovskite heterostructure at 85 °C for 1,250 h for encapsulated large-area devices in ambient air.
RESUMEN
Incorporation of 2D MXenes into the electron transporting layer (ETL) of perovskite solar cells (PSCs) has been shown to deliver high-efficiency photovoltaic (PV) devices. However, the ambient fabrication of the ETLs leads to unavoidable deterioration in the electrical properties of MXene due to oxidation. Herein, sorted metallic single-walled carbon nanotubes (m-SWCNTs) are employed to prepare MXene/SWCNTs composites to improve the PV performance of PSCs. With the optimized composition, a power conversion efficiency of over 21% is achieved. The improved photoluminescence and reduced charge transfer resistance revealed by electrochemical impedance spectroscopy demonstrated low trap density and improved charge extraction and transport characteristics due to the improved conductivity originating from the presence of nanotubes as well as the reduced defects associated with oxygen vacancies on the surface of the SnO2 . The MXene/SWCNTs strategy reported here provides a new avenue for realizing high-performance PSCs.
RESUMEN
2D-layered materials have attracted increasing attention as low-cost supports for developing active catalysts for the hydrogen evolution reaction (HER). In addition, atomically thin Ti3 C2 Tx (MXene) nanosheets have surface termination groups (Tx : F, O, and OH), which are active sites for effective functionalization. In this work, heteroatom (boron)-doped Ti3 C2 Tx (MXene) nanosheets are developed as an efficient solid support to host ultrasmall ruthenium (Ru) nanoparticles for electrocatalytic HER. The quantum-mechanical first-principles calculations and electrochemical tests reveal that the B-doping onto 2D MXene nanosheets can largely improve the intermediate H* adsorption kinetics and reduce the charge-transfer resistance toward the HER, leading to increased reactivity of active sites and favorable electrode kinetics. Importantly, the newly designed electrocatalyst based on Ru nanoparticles supported on B-doped MXene (Ru@B-Ti3 C2 Tx ) nanosheets shows a remarkable catalytic activity with low overpotentials of 62.9 and 276.9 mV to drive 10 and 100 mA cm-2 , respectively, for the HER, while exhibiting excellent cycling stabilities. Moreover, according to the theoretical calculations, Ru@B-Ti3 C2 Tx exhibits a near-zero value of Gibbs free energy (ΔGH* = 0.002 eV) for the HER. This work introduces a facile strategy to functionalize MXene for use as a solid support for efficient electrocatalysts.
RESUMEN
Surface defects in semiconducting materials, though they have been widely studied, remain a prominent source of loss in optoelectronic devices; here we sought a new angle of approach, looking into the dynamic roles played by surface defects under atmospheric stressors and their chemical passivants in the lifetime of optoelectronic materials. We find that surface defects possess properties distinct from those of bulk defects. ab initio molecular dynamics simulations reveal a previously overlooked reversible degradation mechanism mediated by hydrogen vacancies. We find that dynamic surface adsorption affinity (DAA) relative to surface treatment ligands is a surrogate for passivation efficacy, a more strongly-correlated feature than is the static binding strength emphasized in prior reports. This guides us to design targeted passivator ligands with high molecular polarity: for example, 4-aminobutylphosphonic acid exhibits strong DAA and provides defect passivation applicable to a range of perovskite compositions, including suppressed hydrogen vacancy formation, enhanced photovoltaic performances and operational stability in perovskite solar cells.
RESUMEN
Molecular hole-transporting materials (HTMs) having triphenylethylene central core were designed, synthesized, and employed in perovskite solar cell (PSC) devices. The synthesized HTM derivatives were obtained in a two- or three-step synthetic procedure, and their characteristics were analyzed by various thermoanalytical, optical, photophysical, and photovoltaic techniques. The most efficient PSC device recorded a 23.43% power conversion efficiency. Furthermore, the longevity of the device employing V1509 HTM surpassed that of PSC with state-of-art spiro-OMeTAD as the reference HTM.
RESUMEN
Inverted (pin) perovskite solar cells (PSCs) afford improved operating stability in comparison to their nip counterparts but have lagged in power conversion efficiency (PCE). The energetic losses responsible for this PCE deficit in pin PSCs occur primarily at the interfaces between the perovskite and the charge-transport layers. Additive and surface treatments that use passivating ligands usually bind to a single active binding site: This dense packing of electrically resistive passivants perpendicular to the surface may limit the fill factor in pin PSCs. We identified ligands that bind two neighboring lead(II) ion (Pb2+) defect sites in a planar ligand orientation on the perovskite. We fabricated pin PSCs and report a certified quasi-steady state PCE of 26.15 and 24.74% for 0.05- and 1.04-square centimeter illuminated areas, respectively. The devices retain 95% of their initial PCE after 1200 hours of continuous 1 sun maximum power point operation at 65°C.
RESUMEN
Atomically thin Ti3C2T x (MXene) nanosheets with rich termination groups, acting as active sites for effective functionalization, are used as an efficient solid support to host rhenium (Re) nanoparticles for the electrocatalytic hydrogen evolution reaction (HER). The newly designed electrocatalyst - Re nanoparticles anchored on Ti3C2T x MXene nanosheets (Re@Ti3C2T x ) - exhibited promising catalytic activity with a low overpotential of 298 mV to achieve a current density of 10 mV cm-2, while displaying excellent stability. In comparison, the pristine Ti3C2T x MXene requires higher overpotential of 584 mV to obtain the same current density. After being stored under ambient conditions for 30 days, Re@Ti3C2T x retained 100% of its initial catalytic activity for the HER, while the pristine Ti3C2T x retained only 74.8% of its initial value. According to our theoretical calculations using density functional theory, dual Re anchored MXene (Re@Ti3C2T x ) exhibits a near-zero value of Gibbs free energy (ΔG H* = -0.06 eV) for the HER, demonstrating that the presence of Re significantly enhances the electrocatalytic activity of MXene nanosheets. This work introduces a facile strategy to develop an effective electrocatalyst for electrocatalytic hydrogen production.
RESUMEN
Three-dimensional (3D) perovskite solar cells (PSCs) containing additives capable of forming two-dimensional (2D) structures in neat films have attracted attention due to their ability to enhance power conversion efficiency (PCE) in combination with improved operational stability. Herein, a newly designed fluorinated ammonium salt, 2-(perfluorophenyl)ethanaminium bromide:chloride50:50 (FEABr:Cl50:50), is introduced into CsMAFAPbI3-based PSCs with a standard n-i-p architecture. FEABr:Cl50:50 was used as an additive in the tin(IV) oxide (SnO2) electron transporting layer (ETL) as well as a surface treatment for the perovskite film. Used in this dual way, the additive was found to passivate charge-trapping defects within the SnO2 ETL and regulate the crystal growth of the perovskite layer. When FEABr:Cl50:50 was deposited onto the surface of the 3D perovskite film, it formed a thin hydrophobic 2D capping layer. Adopting this dual strategy led to the perovskite film having larger grain sizes, improved quality, and overall better device performance. As a result, the best-performing device exhibited a PCE of over 23% with negligible hysteresis in an n-i-p device architecture with an area of 0.2 cm2. Furthermore, unencapsulated devices with the hydrophobic 2D capping layer showed improved stability compared to the control device when measured under continuous light irradiation at a maximum power point (MPP) at 80 ± 5 °C in a humid (≈50%) environment.
RESUMEN
Compared with the n-i-p structure, inverted (p-i-n) perovskite solar cells (PSCs) promise increased operating stability, but these photovoltaic cells often exhibit lower power conversion efficiencies (PCEs) because of nonradiative recombination losses, particularly at the perovskite/C60 interface. We passivated surface defects and enabled reflection of minority carriers from the interface into the bulk using two types of functional molecules. We used sulfur-modified methylthio molecules to passivate surface defects and suppress recombination through strong coordination and hydrogen bonding, along with diammonium molecules to repel minority carriers and reduce contact-induced interface recombination achieved through field-effect passivation. This approach led to a fivefold longer carrier lifetime and one-third the photoluminescence quantum yield loss and enabled a certified quasi-steady-state PCE of 25.1% for inverted PSCs with stable operation at 65°C for >2000 hours in ambient air. We also fabricated monolithic all-perovskite tandem solar cells with 28.1% PCE.
RESUMEN
p-Type inorganic nickel oxide (NiOx) exhibits high transparency, tunable-optoelectronic properties, and a work function (WF) that is potentially suitable for hole extraction in inverted perovskite solar cells (PSCs). However, NiOx films possess surface defects that lead to high interfacial recombination and an energy offset with the ionization potential of the perovskite. Herein, we show that fluorinated 3-(2,3,4,5,6-pentafluorophenyl)propan-1-aminium iodide (FPAI) can be used to modify the electronic properties of the NiOx anode interlayer. The FPAI modification led to good perovskite crystal growth and films with reduced surface defects. The FPAI modification also increased the WF of NiOx and improved charge extraction. These improvements led to an increased Voc value compared with control devices without FPAI modification, 1.05 V versus 1.00 V, and a higher short-circuit current and larger fill factor. As a result, the best PSCs with FPAI-modified NiOx had a power conversion efficiency of 19.3%. Finally, the PSCs with the FPAI-modified NiOx layer were found to have improved stability.
RESUMEN
Organic-inorganic hybrid perovskite solar cells (PSCs) have attracted significant attention in recent years due to their high-power conversion efficiency, simple fabrication, and low material cost. However, due to their high sensitivity to moisture and oxygen, high efficiency PSCs are mainly constructed in an inert environment. This has led to significant concerns associated with the long-term stability and manufacturing costs, which are some of the major limitations for the commercialization of this cutting-edge technology. Over the past few years, excellent progress in fabricating PSCs in ambient conditions has been made. These advancements have drawn considerable research interest in the photovoltaic community and shown great promise for the successful commercialization of efficient and stable PSCs. In this review, after providing an overview to the influence of an ambient fabrication environment on perovskite films, recent advances in fabricating efficient and stable PSCs in ambient conditions are discussed. Along with discussing the underlying challenges and limitations, the most appropriate strategies to fabricate efficient PSCs under ambient conditions are summarized along with multiple roadmaps to assist in the future development of this technology.
RESUMEN
Graphene - two-dimensional (2D) sheets of carbon atoms linked in a honeycomb pattern - has unique properties that exhibit great promise for various applications including solar cells. Herein we prepared two-dimensional (2D) reduced graphene oxide (rGO) nanosheets from naturally abundant graphite flakes (obtained from Tuv aimag in Mongolia) using solution processed chemical oxidation and thermal reduction methods. As a proof of concept, we used our rGO as a hole transporting material (HTM) in perovskite solar cells (PSCs). Promisingly, the use of rGO in the hole transporting layer (HTL) not only enhanced the photovoltaic efficiency of PSCs, but also improved the device stability. In particular, the best performing PSC employing rGO nanosheets exhibited a power conversion efficiency (PCE) of up to 18.13%, while the control device without rGO delivered a maximum efficiency of 17.26%. The present work demonstrates the possibilities for solving PSC issues (stability) using nanomaterials derived from naturally abundant graphite sources.
RESUMEN
Incorporation of as prepared single-walled carbon nanotubes (SWCNTs) into the electron transporting layer (ETL) is an effective strategy to enhance the photovoltaic performance of perovskite solar cells (PSCs). However, the fundamental role of the SWCNT electrical types in the PSCs is not well understood. Herein, we prepared semiconducting (s-) and metallic (m-) SWCNT families and integrated them into TiO2 photoelectrodes of the PSCs. Based on experimental and theoretical studies, we found that the electrical type of the nanotubes plays an important role in the devices. In particular, the mixture of s-SWCNTs and m-SWCNTs (2:1 w/w)-based PSCs exhibited a remarkable efficiency of up to 19.35%, which was significantly higher than that of the best control cell (17.04%). In this class of PSCs, semiconducting properties of s-SWCNTs play a critical role in extracting and transporting electrons, whereas m-SWCNTs provide high conductance throughout the electrode.
RESUMEN
Single-walled carbon nanotubes (SWCNTs) have attracted significant attention due to their outstanding mechanical, chemical and optoelectronic properties, which makes them promising candidates for use in a wide range of applications. However, as-produced SWCNTs have a wide distribution of various chiral species with different properties (i.e. electronic structures). In order to take full advantage of SWCNT properties, highly purified and well-separated SWCNTs are of great importance. Recent advances have focused on developing new strategies to effectively separate nanotubes into single-chirality and/or semiconducting/metallic species and integrating them into different applications. This review highlights recent progress in this cutting-edge research area alongside the enormous development of their identification and structural characterization techniques. A comprehensive review of advances in both controlled synthesis and post-synthesis separation methods of SWCNTs are presented. The relationship between the unique structure of SWCNTs and their intrinsic properties is also discussed. Finally, important future directions for the development of sorting and purification protocols for SWCNTs are provided.
RESUMEN
Incorporating appropriate plasmonic nanostructures into photovoltaic (PV) systems is of great utility for enhancing photon absorption and thus improving device performance. Herein, the successful integration of plasmonic gold nanostars (AuNSs) into mesoporous TiO2 photoelectrodes for perovskite solar cells (PSCs) is reported. The PSCs fabricated with TiO2 -AuNSs photoelectrodes exhibited a device efficiency of up to 17.72 %, whereas the control cells without AuNSs showed a maximum efficiency of 15.19 %. We attribute the origin of increased device performance to enhanced light absorption and suppressed charge recombination.