Abstract
1. Introduction
The energy crisis caused by the massive consumption of fossil fuels is a serious problem that must be addressed today. Since the Second World War, many countries have committed to the development of renewable energy, including nuclear energy, wind energy, solar energy and tidal energy; of these, solar energy is favored, being both eco-friendly and economical. In the last decade, significant progress has been made in the field of perovskite solar cells (PSCs), with third-generation photovoltaic materials representing a promising candidate to replace monocrystalline silicon. Given perovskite’s power conversion efficiency (PCE), ranging from 5.8% to 25.5%[
Of the various all-inorganic perovskites, CsPbI3 and CsPbI2Br have relatively narrow bandgaps, (Eg), together with a wide light absorption range, and have achieved efficiencies of about 19%[
CsPbBr2I was first discussed by Ma et al. in 2016[
Phase segregation has always been the most worthwhile area of study in relation to hybrid halide PSCs. For example, I– and Br– in the crystal lattice of MAPb(BrxI1−x)3 and CsPb(I1−xBrx)3 migrate due to the halide ions obtaining sufficient migration energy under light[
In this review, we first introduce the crystal structure and photoelectric properties of CsPbBr2I. Secondly, by analyzing the structure of CsPbBr2I, the reasons for its high thermal stability and phase transition are revealed. Next, we discuss possible strategies to suppress light-induced phase transition, such as reducing the numbers of grain boundaries by improving the spin-coating of the membrane, so as to prepare a large-grain membrane, reducing the grain boundary’s surface energy by modifying the interface, and changing the bonding length via ion doping. Finally, we discuss the problems in this field, and provide an outlook for the future of CsPbBr2I.
2. The crystal/electronic structure and optical properties of CsPbBr2I
2.1. Crystal structure
Like other CsPbX3 (X = I–, Br–), the crystal structure of CsPbBr2I can be described as the Pb site, and X site ions form a [MX6]4– corner-shared octahedron; Cs+ is located in the center of the octahedron, as shown in Fig. 1(a)[
Figure 1.(Color online) (a) Crystal structure of cubic CsPbX3 perovskite. Reproduced with permission[
where rA, rB, and rX are the ionic radii of their respective ions in the ABX3. With respect to CsPbX3, the halide anion has a smaller negative charge than the oxide anion, and the halide ion has a large radius. This requires a large cation ion radius, and low valence at the A site, so Cs+ is the appropriate choice for inorganic ions, and is sufficient to maintain the perovskite structure[
According to Eq. (1), when 0.8 < t < 1, the perovskite phase structure has a relatively high PCE. When t < 0.8, the efficiency of the resulting non-perovskite phase is very low. In theory, by introducing other ions to tune the t value to between 0.9 and 1, we could increase the stability of CsPbBr2I.
2.2. Electronic structure
The electronic structures of different components of CsPbX3 share great commonalities. The valence band maximum (VBM) of CsPbBr2I is primarily composed of anti-bonding hybrid Pb 6s, and X np (X = I−, Br−) orbitals, where the main contribution is X np. The conduction band minimum (CBM) is determined by the anti-bonding mixture of Pb 6p and X np orbitals, and the main contribution is Pb 6p, as shown in Fig. 1(b)[
2.3. Optical properties
The optical properties of CsPbBr2I are described in terms of absorption and quantum yield (QY).
(1) Fig. 1(d) shows that as the iodine concentration increases, the wavelength becomes longer, and the absorption begins to shift[
(2) QY is a measure of the capacity of optoelectronic devices to absorb light-emitting electrons. For a QY of CsPbX3 between 10%–90%, Samanta et al. measured the fluorescence QY of CsPbBr3 and CsPbBr2I to be ~40% and ~10%. This indicates the presence of many inherent trap states in CsPbBr2I, which affect the low-emission intensity. The main trapping states result from iodine-induced distortion of the corner sharing [Pb(Br/I)6] octahedral of the cubic CsPb(Br/I)3 nanocrystals, leading to the formation of a twisted crystal structure[
3. Phase transition of all-inorganic halide perovskite
Stability is a major challenge for all inorganic CsPb(I1−xBrx)3 (0 ≤ x ≤ 1); this includes both thermal stability and optical stability. The stability of CsPb(I1−xBrx)3 is dependent on the ratio of Br/I content. Fig. 2(a) shows that when x > 0.2, CsPb(I 1−xBrx)3 has a stable orthorhombic perovskite structure at room temperature. When x < 0.2, the perovskite structure tends to transform to the delta phase at room temperature, i.e., a thermally-induced phase transition, including for CsPbI 3[
Figure 2.(Color online) (a) Illustration depicting the perovskite crystal structure as a function of the iodine/bromine ratio. Reproduced with permission[
However, with an increase in the Br/I content, the thermal stability of the material is generally overcome, while the optical stability of the material gradually weakens, i.e., light-induced phase segregation. When x > 0.2, phase segregation occurs under light, which specifically manifests as a large number of I ions gathering at grain boundary or grain surface to form a compound, resulting in lower cell efficiency. This is primarily because mixed halide anions cannot exist uniformly in the lattice, due to ionic radius and electronegativity problems. When the external light provides energy, the two kinds of ions tend to segregate [
Taking into account the above two issues, the Br/I ratio in CsPbBr2I determines its characteristic of strong thermal stability, but also causes phase segregation under illumination. In the following section, we will first analyze the thermal stability mechanism of CsPbBr2I, then discuss the internal causes of severe phase segregation in CsPbBr2I, and finally provide some strategies to prevent phase segregation.
3.1. Thermally induced phase transition
For the all-inorganic version, a substantial change in the crystal structure, namely phase transition, will occur at different temperatures. Phase transition is the transition between different crystal lattices and it is accompanied by the absorption or release of heat. In this part, we first discuss the mechanism of thermally induced phase transition, and then elaborate the phase transition of CsPbBr2I.
3.1.1. Mechanism of thermally induced phase transition
A phase transition is a change in the crystalline structure of the same substance at different temperatures. Each crystal structure at different temperetures is known as a phase. Since different crystal structures have different optical properties and cell parameters, perovskite materials have different light absorption rates at different temperatures, with the result that different efficiencies are produced under different phases[
3.1.2. CsPbBr2I thermally-induced phase transition
The crystal structure of CsPbBr2I is mainly high-temperature (α-perovskite), inculding the space group Pm-3m, and the low-temperature non-perovskite phase (δ-perovskite), Pmnb[
In an inert environment, with a decrease in temperature, the high-temperature phase forms a metastable state, and remains at room temperature, thereby maintaining extremely high efficiency. As shown in Fig. 2(d), the transition from the high-temperature to the low-temperature phase is reversible. However, for CsPbI3, after about 320 °C heating and cooling, a high-temperature metastable phase forms at room temperature, and heating the metastable phase again causes it to transform extremely easily into a low-temperature non-perovskite phase. As the I– on the CsPb(I1−xBrx)3 (0 ≤ x ≤ 1) lattice is partially replaced with Br–, the bromine-rich crystal structure has a more suitable t, and is not prone to thermodynamic phase transition[
3.2. Light-induced phase transition
Unlike monocrystalline silicon solar cells, CsPbBr2I halide perovskite is composed of different anions, and the migration of these anions requires relatively low energy. When there is ambient light to provide energy, ion migration will occur, and anions will migrate. In this section, we discuss the phase-segregation phenomenon of CsPbBr2I under light.
3.2.1. The origin of photo-induced phase segregation
Although newly-prepared CsPb(I1−xBrx)3 (0 < x < 1) halide is evenly mixed, with an increase in Br content, it will display a red-shifted photoluminescence peak, which splits into two smaller peaks with different absorption wavelengths under illumination, as shown in Fig. 3(a)[
Figure 3.(Color online) (a) The photoluminescence peak of these mixed-halide perovskites shifted exclusively to 1.87 eV after continuous illumination. The solid lines denote the spectra taken from freshly made samples, and the dashed lines dentote the measurements following 10 min illumination at an intensity of 0.3 W/cm2. Reproduced with permission[
Like most CsPb(I1−xBrx)3 (0 < x < 1) perovskites, regardless of the CsPbBr 2I spin-coating methods, there is a large difference between the forward sweep and the reverse sweep voltage, resulting in a very low average voltage. This is due to I– and Br– agglomeration at the grain boundary and crystal surface, respectively, under light, which causes phase segregation of CsPbBr2I, resulting in severe hysteresis and low efficiency. Li et al. first used scanning electron microscopy (SEM) and cathodoluminescence (CL) to conduct microscopic analyses of CsPbBr2I[
3.2.2. The mechanism of photo-induced phase segregation
The study of hybrid halide perovskite ion migration has a history of more than 30 years. As for how the halide phase is segregated, although it still cannot be observed with specific equipment, some studies have found that ion migration triggers phase segregation[
In the above equation, Δhmix is the volumetric enthalpy, T·Δsmix is the volumetric entropy, and ΣiciW ir2 denotes the cohesive energies.
Using density functional theory (DFT) calculations, we find that, regardless of the size of the crystal grains, the ΔG is negative for any content of XBr in the dark, which proves that the phase of the mixed halide is stable under dark conditions, as shown in Fig. 3(e). While light-induced polarons are introduced under illumination, polarons can generate lattice strain energy by lengthening or shortening the chemical bond between the Pb-site and the halogens, and the Gibbs free energy (ΔGlight) of the mixed phase under illumination depends on the lattice strain energy (Δgs > 0) originating from the light-induced polaron and Δ Gdark. Because Δgs > 0, according to Eq. (3), when the grain size, r, is large enough, the ΔGlight will be greater than zero under light, meaning that a driving force of phase separation will be generated, so that the mixed halide will exhibit phase separation under light. Br–- and I–-rich domains are formed by dispersing and mixing the halide phase, as shown in Fig. 3(f):
However, the assumption above assumes that the temperature in the dark is the same as the temperature under light. In fact, the presence of light will inevitably cause the temperature to rise.
Li et al. pointed out that the hysteresis index of CsPbBr2I could be as high as 43.8%, far higher than for CsPbI3 or CsPbI2Br. In order to reduce the hysteresis of CsPbBr2I, and improve the efficiency of devices in which it is utilized, in this work, we focus primarily on methods of suppressing phase segregation, thereby reducing the hysteresis.
4. Suppressed phase segregation of CsPbBr2I
In summary, the light stability of halide materials is the main obstacle to the development of CsPb(I1−xBrx)3 (0 < x < 1) PSCs, represented here by CsPbBr 2I. Based on studies of the phase-segregation mechanism, we believe that phase segregation must be suppressed at the grain boundary, the film surface, and the lattice interior.
(1) For grain boundaries, a film with large grains and few grain boundaries can be prepared by improving the preparation method.
(2) For the surface of the film, serial passivation can be used to reduce the surface energy and suppress ions’ bias polymerization.
(3) For the inside of the grain boundary, ion doping can be used to enhance bonding, which effectively inhibits the ion migration caused by lattice expansion due to photo-generated carriers.
These three strategies for phase segregation suppression are described in detail below.
4.1. Preparation of large grain film
The defects on the perovskite film and numerous grain boundaries possess high energy; when halide ions migrate under light, these defects will adsorb halide ions, causing halide ions to agglomerate, and phase segregation to occur. As such, the preparation of perovskite films with large grains, no pinholes, and no cracks is key to suppressing phase segregation and obtaining high PCE for perovskite devices[
(1) The continuous exploration and improvement of film preparation methods has led to developments in spin-coating-based methods, and includes other film preparation methods such as the doctor blade, inkjet-printing, and slot-die coating for film preparation[
(2) Optimization of the technology under different preparation methods, such as annealing temperature and time, the composition of the solvent, and the modification of some intermediates.
Combining the two approaches above, we have improved the traditional film preparation methods and preparation processes, and developed new CsPbBr2I spin-coating methods, which have continuously improved solar cell efficiency. In the next section, we investigate traditional spin-coating methods, and examine the improved processes for each type of film[
4.1.1. Dual source thermal evaporation
The first CsPbBr2I film was first prepared using the dual source thermal evaporation method; as shown in Fig. 4(a), its efficiency reached 4.7%. This method can be used for large-scale production and coating in industry. The process involves loading CsI and PbBr2 into the device with a 1 : 1 ratio, heating of the two substances to a predetermined temperature, and evaporating to the preheated TiO2 substrate to prepare the CsPbIBr2 sample.
Figure 4.(Color online) (a) Schematic diagram of dual-source thermal evaporation. Reproduced with permission[
Since the entire spin-coating process is carried out in steam, there is no residual liquid on the substrate, and the thickness of the film can be controlled by controlling the spraying rate[
4.1.2. One-step method
The traditional one-step method is to dissolve CsI and PbBr2 dimethyl sulfoxide (DMSO) in a 1 : 1 ratio, spin-coating them onto a TiO2/SnO2 substrate, and annealing to obtain a CsPbIBr2 film. Although the one-step method is extremely easy to operate, it has many shortcomings, such as poor solubility of Br– in the solution, resulting in uneven film composition, lattice defects, and a reduction in the quality of the film. In addition, DMSO combines with PbBr2, forming a complex PbBr2-DMSO intermediate, which prevents the crystallization of CsPbBr2I film, and results in isolated holes on the film[
In order to overcome these problems, Que et al. preheated the substrate prior to spin-coating, which resulted in improved film coverage, as shown in Fig. 4(b), where the resulting grain size is 0.2–2 μm. However, the preheating temperature of the substrate is not easy to control. If the preheating temperature is too high, disorder in the [Cs-PbBr2]+ arrays in the initial formation will cause frost on the film’s surface, and have an impact on overall device performance. Zhu et al. used the method of intermolecular exchange to prepare their CsPbBr2I film, as shown in Fig. 4(c). The method involves a precursor CsPbBr2I film, prepared according to the one-step method, which is then coated onto the TiO2 substrate. For the intermolecular exchange, a methanol solution containing CsI is spin-coated onto the CsPbBr2I precursor film, then washed with anhydrous IPA (isopropanol). After annealing, the resulting CsPbBr2I film exhibited long-term stability and a greatly improved efficiency as compared to the traditional one-step method[
Whether employing a one-step method, preheating assisted deposition, or intermolecular exchange, since the formation of CsPbBr2I crystals requires high formation energy, high-temperature annealing can result in the growth of large grains, which increases production costs, and limits its application in flexible devices. In order to reduce the formation energy of CsPbBr2I crystals to lower the annealing temperature, Zhang et al. treated their CsPbBr2I film with methylammonium halides (MAX, X = I, Br) prior to annealing, so that the MA+ was at the center of the CsPbBr2I crystal nucleation, thereby greatly reducing its formation energy, meaning that the final annealing temperature could be reduced to 150 °C[
4.1.3. Two steps method
Given that, in the one-step method, the solubility of Br– in the precursor solution is relatively small, and ion doping is difficult, a two-step method has been proposed to resolve this difficulty. This primarily consists of dissolving PbBr2 in N, N-dimethylformamide (DMF) and DMSO as a precursor solution, and spinning it on the substrate, followed by drying on the heating stage for a period of time. The prepared film is then immersed in a methanol solution of CsI for a period of time, before being annealed to obtain a CsPbBr2I film with an efficiency of 8.25%[
Having discussed the basic spin coating method and its improvements above, we find that each method has certain drawbacks, and that some process parameters are not ideal, such as the annealing temperature, substrate temperature, annealing time, spray rate, etc. All in all, making perovskite films with few defects and large grains helps reduce hysteresis and improve efficiency.
4.2. Passivation of film surface
Halide phase segregation will generate a large number of mobile ions near the grain boundaries or inside the crystal grains of the CsPbBr2I film. These mobile ions accumulate near the CsPbBr2I/ETL interface to form an incident electron injection barrier, which is not conducive to small extraction[
(1) TiO2 is the most widely-used charge transport material, but its disadvantages include higher sintering temperature, narrow band gap, and relatively low electron mobility[
Figure 5.(Color online) (a) Illustration of CsXth decomposition, and sulfur doping in perovskite. Reproduced with permission[
(2) CsPbBr2I film produced with SnO2 as the transport layer has high crystallinity and extremely uniform crystal grains, but the opening voltage is relatively low, while TiO2 is conducive to the separation and extraction of charges[
(3) In addition to the above two methods, ZnO and In2S3 can also be used as ETL transport layers for CsPbBr2I[
4.3. Doping increases bond strength
Doping could introduce other ions into the crystal lattice, altering the crystal structure to suppress phase segregation and improve the performance of the material[
Figure 6.(Color online) (a) Relation of the tolerance factor (
By summarizing the effects of doping, we can then analyze the effect of doping on CsPbBr2I performance from A site and B site, respectively.
4.3.1. A-site doping
In CsPbBr2I, the Cs+ at the A site determines the space size of the corner-sharing [PbBr6]4- octahedra, and the introduction of ions with an A radius greater than Cs, such as (FA or MA), or ions less than Cs+, can inhibit phase segregation. Its main effect is to reduce lattice distortion caused by excited carriers through the substitution of other A-site ions, which promotes the thermodynamic stability of the uniform phase, and inhibits segregation[
4.3.2. B-site doping
With regard to B-site doping, the optical characteristics are mainly affected by CBM and VBM. Therefore, a partially-doped metal site (B-site cation) is a more direct and effective way to change the effect of photo striction on light illumination, and may eliminate the phase segregation problem[
Given that the energy level of B-site Pb is relatively deep, B-site doping with other metal ions may cause new deep defects, which will serve as scattering centers to further affect the original photoelectric properties of CsPbBr2I[
(1) Among other kinds of perovskite doping, Mn2+ doping has proved to be an effective method to adjust the electronic and optical properties of semiconductor nanocrystals[
(2) Sn doping in organic–inorganic lead-halide perovskites can narrow the bandgap and achieve high cell efficiency. Li et al. used the one-step antisolvent method to prepare CsPb1−xSnxBr2I (x = 0.00, 0.25, 0.5, 0.75, and 1.00) films with adjustable Eg between 2.04 and 1.64 eV[
(3) Ba2+ doping results in a CsPbBr2I film with a good crystalline morphology. Liu et al. partially replaced Pb in CsPbBr2I with Ba (II, IR = 135 pm), which resulted in an undesirable t of less than 0.8. Ba(II) doping improves the device efficiency to 10.51%, as compared with an efficiency of 8.4% for a film not doped with Ba2+[
Doping has achieved good results in terms of suppressing phase segregation. However, there are a series of scientific problems still to be resolved regarding doping. Issues such as whether dopants should be introduced into the crystal lattice, or just isolated on the surface, and how doping ions adjust the properties of the perovskite remain a mystery. In addition, the uniformity of the doped phase needs to be investigated by means of a high-resolution and high-sensitivity characterization method.
5. Challenges and prospects
To summarize this article, we find that the biggest advantage of CsPbBr2I is that it will not fail due to thermodynamic phase change during external temperature change; i.e., it exhibits thermal stability. Its biggest shortcoming is that phase segregation can occur on exposure to light, causing hysteresis, which seriously affects efficiency. From the perspective of film preparation and interface modification, the efficiency of CsPbBr2I still shows room for improvement. In addition, the process of transferring CsPbBr2I from laboratory to commercial use represents a significant challenge. Below, we provide a brief summary of the challenges we face in the further development of CsPbBr2I, and look forward to its application prospects.
5.1. Challenges
5.2. Outlook
Third-generation perovskite photovoltaic devices are primarily being developed with an eye to energy conservation and environmental protection. In the current experimental development stage, the selection of materials used to make devices is slowly shifting towards low cost and environmental protection considerations.
Acknowledgements
This work was funded by the National Natural Science Foundation of China (52073131, 51902148, 61704099, 61874166, U1832149, 51801088 and 51802024), the Natural Science Foundation of Gansu Province (20JR5RA227, 20JR5RA217, 20JR5RA278), and the Fundamental Research Funds for the Central Universities (lzujbky-2020-61, lzujbky-2019-88 and lzujbky-2020-kb06).
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