Abstract
1. Introduction
Since the first organic–inorganic hybrid perovskite solar cell (PSCs) was proposed by Miyasaka’s group[
CsPbX3 is a promising candidate to conquer these problems because Cs+ is the most feasible inorganic cation to replay volatility and hygroscopic A-site with suitable tolerance factor[
CsPbI3 has four different phases (cubic (α), tetragonal (β), orthorhombic (γ) and non-perovskite yellow (δ) phase) and each phase transforms under different temperatures[
In this review, we aim to summarize the latest works about CsPbI3 PSCs based on HI hydrolysis-derived intermediate. First, we briefly review the different crystal and electronic structures of CsPbI3. We then trace the history and disputes of HI hydrolysis-derived intermediate to make this review more logical. Afterward, we highlight the functions of HI hydrolysis-derived intermediate, and systematically summarize some advanced works about HI hydrolysis-derived intermediate on CsPbI3 PSCs. Finally, present issues and outlines are discussed to further increase the CsPbI3 PSCs performance.
2. Crystal/electronic structure
Photo-electric properties (e.g., optical transitions, charger transfer) are greatly related to crystal and electronic properties (e.g., phase transition, energy band)[
2.1. Crystal structure
The CsPbI3 perovskite structure can be described as: Pb-site and I-site ion form a corner sharing [PbI6]4– octahedron, while the Cs cation resides in the cuboctahedral cavities[
Figure 1.(Color online) (a) The structure and transition of CsPbI3 phases versus temperature. Reproduced with permission[
The detailed transition temperature between each phase was researched by Even et al., based on density functional theory (DFT) analyzation. The increasing thermal parameters of I– tended to strength the dynamic motion of the corner-connected [PbI6/2]– octahedral, which further induced a change of the unit cell volume and made δ-phase transformed to α-phase at 595 K. Then, with dynamic states gradually relaxing, α-phase transitions to β-phase at 539 K; β-phase transitions to γ-phase at 425 K; finally γ-phase turns to yellow non-perovskite phase (δ-phase) at RT[
The different stability of each phases can be ascribed to the different dissociated energies. The dissociation energy from CsPbI3 to CsI and PbI2 for α-, γ-, and δ-phase are 0.04, –0.09 and –0.16 eV, respectively. δ-phase CsPbI3 shows a small Pb–I–Pb bond angel (95.09° and 91.40°) than α-phase CsPbI3 (180°) and γ-phase CsPbI3 (154.74°), which reduces the orbital overlap between Pb and I atoms and also makes δ-phase CsPbI3 with a deeper defect transition energy level than α-, γ-phase. This indicates that δ-phase is the most stable phase because of its lowest dissociation energy[
2.2. Electronic structure
The valence band maximum (VBM) of CsPbI3 perovskite is constituted of antibonding hybridized Pb 6s and X np orbitals, among which X np takes the lead. However, Pb 6p is in the dominant place of conduction band minimum (CBM), as shown in Fig. 1(c)[
The calculated electronic of α-, β- and γ-CsPbI3 are depicted in Figs. 1(d) and 1(e)[
3. The functions of HI hydrolysis-derived intermediate
We summarize the performance of CsPbI3 PSCs after introducing HI hydrolysis-derived intermediate in Table 1 (sPCE is the stable PCE). Its main functions can be summarized as following:
1) Reducing crystallization energy barrier in low temperature fabrication;
2) Increasing iodide coordination numbers to decrease structural disorder, modifying structure and forming higher-order iodoplumbate complexes;
3) Slowing down the rapid crystalline process and obtaining high-quality CsPbI3 film;
4) Inducing strain to generate distorted metastable phase (β- and γ- CsPbI3);
5) Modifying the band gap of perovskites films.
4. History and disputes of HI hydrolysis-derived intermediate
The solution one-step method has advantages of simple, convenience and facile process, and can also be compatible roll-to-roll fabrication technology[
4.1. HI
In the early stage, researchers focused on using HI additive in CsPbI3 PSCs fabrication to cause a microstrain and induce a low temperature phase transition process. Meanwhile, extra halides in HI precursor solution tended to fill the vacancies of perovskites, resulting in change of metal–halogen–metal bond connectivity, and consequently cell volumes and optical bandgap[
In 2015, HI was first used as an additive in CsPbI3 PSCs. Snaith et al. introduced a small amount of HI in the precursor solution before spin-coating. They found that HI additive could change the solubility of precursor materials and induce a strain to lower the temperature phase transition. Then, strain triggered small crystals appearing and significantly stabilized its structure in RT, as shown in Fig. 2(a)[
Figure 2.(Color online) (a) The diagrammatic of HI fabricated CsPbI3. Reproduced with permission[
4.2. PbI2·xHI or HPbI3
In addition to HI additive, HI hydrolysis-derived intermediate is more effective because it eliminates water in the HI solution and is an intermediate compound to increase perovskite crystallinity[
Zhu et al. introduced HPbI3 into the CsPbI3 PSCs and assisted with a triple cation NH3+C2H4NH2+C2H4NH3+ (named as DETA3+) to further stabilize the α-CsPbI3 perovskite phases[
4.3. PbI2·xDMAI or DMAPbI3
Kanatzidis et al. recently claimed that HPbI3 did not exist and was replaced by a compound of DMAPbI3, which generated through DMF hydrolysis in HI solution. Importantly, they pointed out that some early reports of inorganic perovskite are actually the hybrid perovskite. They found that DMAPbI3 possessed a larger tolerance factor and mixing with Cs+ could adjust tolerance factor (t) of the compounds (Cs1−xDMAxPbI3) toward an ideal factor (t, 0.9–1). Finally, they achieved a champion PCE of 12.62% in Cs1−xDMAxPbI3-based PSCs, as shown in Fig. 2(d)[
Figure 3.(Color online) (a) Schematic illustration the fabrication process of Cs
Zhao et al. used PbI2·xDMAI to fabricate CsPbI3 PSCs recently, and they concluded that the fabricated perovskites are actually all inorganic composition because the organic ion DMA+ are easily lost during the high-temperature (210 °C) annealing process[
Our groups also confirmed this conclusion. We synthesized a series of intermediate compounds (DMAI and DMAPbI3) by different ratio of HI/DMF, and used them to fabricate CsPbI3 PSCs. After detailed analysis, we found that the major component of CsPbI3 was still inorganic in this reaction route. Most of DMA+ organic molecules lost during the annealing process, and only a small amount of DMA+ remained to stabilize perovskite structure. Excessive DMA+ interacted with Pb2+ to further passivate CsPbI3 surface, as shown in Fig. 3(d)[
In conclusion, the organic molecule DMAI mainly influence the crystallization kinetics and perovskite phase. During the annealing process, DMAI will sublimate quickly, change the rate of crystallization and form metastable (β- and γ-) phase based CsPbI3. The controllable crystallization kinetics and stable (β- and γ-) phase are beneficial to morphology and stability of perovskite, respectively. Besides, DMA+ (2.72 Å) possesses a larger ionic radius than Cs+ (1.88 Å)[
5. Applying HI hydrolysis-derived intermediate in CsPbI3 PSCs
5.1. α-phase CsPbI3 based PSCs
As we discussed earlier, HI hydrolysis-derived intermediate showed a lot of advantages in high-quality film fabrication and device performance. Importantly, perovskite films with better crystallinity, morphology, and higher range of absorption are the foundation of efficiency.
The first working α-CsPbI3 PSCs with a PCE of 2.9% was fabricated in low temperature (100 °C) by Snaith and his cooperators via a small amount HI additive adding[
Figure 4.(Color online) (a) The detail information of PbI2.HI and PbI2 fabricated perovskite, inserted pictures are their digital photos. Reproduced with permission[
Compared with HI, the absence of H2O molecules in HI hydrolysis-derived intermediate can optimize the perovskite crystallinity and morphology. Chen and his cooperators replaced PbI2 with HPbI3 in fabricating stable α-CsPbI3 film. They found that the bandgap was shifted from 1.72 to 1.68 eV owing to formation of tensile lattice strain. Finally, a HTL free α-CsPbI3 was obtained with a higher PCE of 9.5%. Besides, the optimal device showed enhanced stability, which maintained 90% of its initial PCE under illumination for more than 3000 h in dry environment, as shown in Fig. 4(b)[
5.2. Metastable (β- and γ-) phase CsPbI3 based PSCs
Recently, the CsPbI3 films fabricated by HI hydrolysis-derived intermediate were proved metastable phases (combined β-phase CsPbI3 with γ-phase CsPbI3).
The β-phase CsPbI3 can also be formed at low temperature and show more stable perovskite structure than α-phase one. However, it is difficult to deposit and stabilize its perovskite structure[
Figure 5.(Color online) (a) Schematic illustration of CHI crack-filling interface engineering. Reproduced with permission[
The γ-phase CsPbI3 is the most stable black phase because of its lowest dissociation energy[
In our recent research, we reported the synergistic effect of HI and PEAI additives, where HI transferred to an intermediate (HPbI3+x) to fabricate distorted black phase-based CsPbI3 thin films and PEAI induced a steric effects to avoid phase transition. It is noteworthy that the best device maintained 92% of its initial PCE for 60 days storage in ambient (RH ~ 20%–30%, 25 °C), while the reference one degraded to 0.65% in the same condition for 8 days, as shown in Fig. 5(d)[
One of the notorious problems to limit CsPbI3 performance is the lower JSC compared with hybrid one. Thus, we have also developed several strategies to increase its JSC, such as harvesting short wavelength ultraviolet light (UV-light) or near-infrared (NIR) light, and designing device structure to capture light. First, we developed a downconversion nanoparticles (DCNPs) nitrogen-doped graphene quantum dots (N-GQDs) as an energy-down-shift to harvest the short wavelength (< 350 nm) UV-light. After combining it with HPbI3-formed γ-CsPbI3, the optimal device showed an improved short circuit current density (JSC) from 18.67 to 19.15 mA/cm2, with an increase of 2.57%. Meanwhile, its performance was greatly increased 3.15%, from 15.53% to 16.02%[
5.3. Low dimension CsPbI3 based PSCs
Reducing dimension can further increase the stability of CsPbI3 PSCs because reducing materials dimension can lead to more symmetric crystal structure and show a smaller surface energy[
However, the poor solubility of CsX in the precursor solution would severely limited the thickness of CsPbI3 film and influence the light absorption. Chen et al. used HPbX3 and CsAc as new precursor to overcome the poor solubility of Cs+ precursor and fabricate α-CsPbX3 with optimal thickness. They introduced phenylethylammonium iodide (PEAI) to HPbX3 and CsAc system and further controlled the dimension of CsPbX3 from three dimension (3D) to two dimension (2D). Finally, a champion PCE of 12.4% in 2D CsPbI3 perovskite was obtained, and maintained 93% of its initial PCE in ambient for 40 days, as shown in Fig. 6(a)[
Figure 6.(Color online) (a) The structure and decomposition energies of different n values PEA2Cs
Pradhan et al. fabricated stable CsPbI3 nanocrystals (NCs) with superior stability by using a higher temperature (260 °C) than usual (160 °C), and adding olelyamine (OLA) and HI respectively in the reaction process (noted that only OLA or HI are less efficient). Taking the NMR analyzation into account, they found that higher temperature helped the OLA+ ligands to occupy the Cs+ position on the surface and further stabilized its structure[
6. Prospects and outlook
Although lots of advanced works about HI hydrolysis-derived intermediate have been done to boost PCE of CsPbI3 PSCs, its PCE still far behind the hybrid ones. Therefore, we need to analyze the urgent problems that remain and develop corresponding strategies to improve the performance of CsPbI3 perovskites.
In conclusion, CsPbI3 perovskite, particularly the metastable phases (β- and γ-Phase CsPbI3), is a promising material to replace the unstable hybrid perovskite. Besides, CsPbI3 PSCs with suitable bandgap make it more suitable to apply in tandem solar cells and commercialization. Based on these advantages, we conclude that CsPbI3 PSCs maybe the mainstream research direction in the near future, and we should adopt a positive attitude to it.
Acknowledgements
This work was funded by the National Natural Science Foundation of China (51902148, 61704099 and 51801088), the Fundamental Research Funds for the Central Universities (lzujbky-2020-61, lzujbky-2019-88 and lzujbky-2020-kb06), and the Special Funding for Open and Shared Large-Scale Instruments and Equipments of Lanzhou University (LZU-GXJJ-2019C023 and LZU-GXJJ-2019C019).
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