Highly Efficient Infrared Light-Converting Perovskite Solar Cells: Direct

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Highly Efficient Infrared Light Converting Perovskite Solar Cells: Direct Electrons Injection from NaYF4:Yb3+, Er3+ to the TiO2 Yahan Wu, Xihong Ding, Xiaoqiang Shi, Tasawar Hayat, Ahmed Alsaedi, Yong Ding, Li'e Mo, and Songyuan Dai ACS Sustainable Chem. Eng., Just Accepted Manuscript • DOI: 10.1021/ acssuschemeng.8b02500 • Publication Date (Web): 12 Sep 2018 Downloaded from http://pubs.acs.org on September 12, 2018

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ACS Sustainable Chemistry & Engineering

Highly Efficient Infrared Light Converting Perovskite Solar Cells: Direct Electrons Injection from NaYF4:Yb3+, Er3+ to the TiO2 Yahan Wu,a Xihong Ding,a Xiaoqiang Shi,a Tasawar Hayat,c,d Ahmed Alsaedi,c Yong Ding,*a Li-E Mo,*b and Songyuan Dai*a,b,c a

Beijing Key Laboratory of Novel Thin-Film Solar Cells, North China Electric Power

University, NO.2, Beinong Road, Changping District, Beijing, 102206, P. R. China b

Key Laboratory of Photovolatic and Energy Conservation Materials, Institute of

Applied Technology, Hefei Institutes of Physical Science, Chinese Academy of Sciences, 2221 Changjiangxi Road, Shushan District, Hefei, 230031, P. R. China c

NAAM Research Group, Department of Mathematics, Faculty of Science, King

Abdulaziz University, P.O BOX 80203, Jeddah 21589, Saudi Arabia d

Department of Mathematics, Quaid-I-Azam University, Islamabad 44000, Pakistan

1

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ABSTRACT Organic-inorganic hybrid perovskite solar cells (PSCs) exhibit high photovoltaic performance, while its utilization of infrared and near infrared (NIR) irradiation are poor. Up-conversion material can high-convert the NIR into visible light, providing the PSCs with a possibility of utilizing NIR. In this report, the critical TiO2 mesoporous layer was successfully improved with the incorporation of 30 nm cubic NaYF4:Yb3+, Er3+ up-conversion nanoparticles (UCNPs). Transmission electron microscope and fluorescence spectrum of mesoporous layer confirmed the formation of the shared interface between TiO2 and UCNPs. The NaYF4:Yb3+, Er3+ nanoparticles can convert the 980 nm NIR into 520, 545 nm and 660 nm emissions, in which the excited electrons at 520 and 545 nm can directly inject into the conduction band of TiO2 by shared interfaces. Meanwhile, the visible light (660 nm) can be absorbed by perovskite layer. At last, the device not only enhanced short-circuit current but also exhibited high power conversion efficiency.

KEYWORDS: NaYF4:Yb3+, Er3+, nanoparticles, electron injection, mesoporous layers, perovskite solar cells

INTRODUCTION Among the variety of photoelectric conversion materials, organometal trihalide perovskites are considered to be the excellent one for perovskite solar cells (PSCs). Based on the merits of high absorption coefficient,1 narrow band gap,2 high charge-carrier mobilities,3,4 structures and preparation methods,5-7 the PSCs exhibit outstanding character for photoelectric conversion. Nowadays it achieves significant efficiency over 22.7%.8 The perovskite sensitizers have typical ABX3 structure, where A is methylamine (MA), formamidine (FA), Cs, or Rb, B is Pb, Bi, or, Sn and X is halogen or SCN.9,10 However, they absorb only a part of incident light (300-800 nm). The infrared and near-infrared (NIR) spectrum comprise almost half of the energy of the solar radiation.11 Thus, utilizing the infrared and NIR spectrum become highly valuable for energy conversion. Usually, the NIR energy problem could be solved by up-conversion materials.12,13 Among these materials, the NaYF4:Yb3+, Er3+ is effective photoluminescence up-conversion material, which is used in bio-imaging optics,14 lasers15 and solar cells.16 2


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In silicon solar cells, the NaYF4: Yb3+, Er3+ was employed as bottom material to improve the power conversion efficiency (PCE).17 In dye-sensitized solar cells (DSSCs), for optimizing the path length of the incident light and achieving better NIR response, NaYF4:Yb3+, Er3+ was employed due to its abilities of up-converting and light scattering.18-21 In PSCs, Roh et al. incorporated the β-NaYF4:Yb3+,Er3+ in PSCs as up-converting mesoporous layer to obtain better NIR light harvesting.22 Therefore, it is expected that up-conversion materials could be widely used in PSCs to improve the photovoltaic performance. Utilizing up-conversion materials with the appropriate energy levels could lead to direct electrons injection from the NaYF4:Yb3+, Er3+ material to the conduction band (CB) of titanium dioxide in DSSCs.23 However, there are rare reports on utilizing electrons injection from the up-conversion material to the CB of titanium dioxide in PSCs to improve photovoltaic. In this study, 30 nm α-NaYF4:Yb3+, Er3+ were simply synthesized as an up-converting mesoporous layer. In order to improve photovoltaic by means of electrons transport from NaYF4:Yb3+, Er3+ to TiO2, the new mesoporous layer was sintered at 510oC to form the shared interfaces between NaYF4:Yb3+, Er3+ and TiO2. Meanwhile, the NaYF4:Yb3+, Er3+ could also convert NIR into visible light to facilitate the absorption of perovskite layer. Finally, the best PCE of device with UCNPs is 17.23%, which increased efficiency by 13.43% for the device with pure TiO2.

RESULTS AND DISCUSSION For simplicity, the NaYF4:Yb3+, Er3+ up-conversion nanoparticles are named as UCNPs. The size of TiO2 nanoparticles incorporated into mesoporous layer is about 30 nm. In order to avoid the influence on perovskite nucleation and growth, we synthesized the same size UCNPs to incorporate in TiO2 mesoporous layer. The information about nanoparticles synthesis of UCNPs is detailed in Experiment Section in Supporting Information. Figure 1a, 1b show representative transmission electron microscopy (TEM) images of UCNPs with different magnification. UCNPs are uniform and monodisperse. The average size of UCNPs is about 30 nm in diameter as shown in Figure 1b. All UCNPs display typical cubic phase diffraction peaks, including notable characteristic peaks at 28.2° and 46.9° correspond to (111) and (220), respectively. As depicted in Figure 1e, the peak positions in X-ray diffraction (XRD) pattern of UCNPs are consistent with the calculated pattern for α-NaYF4:Yb3+, 3



Er3+ crystal (Joint Committee for Powder Diffraction Standards, JCPDS No. 77-2042).24

Figure 1. (a, b) TEM images of UCNPs with different magnification. (c, d) SEM images of TiO2 and TiO2/UCNPs mesoporous layer in 510οC. (e) XRD pattern of UCNPs. (f) XRD pattern of TiO2/UCNPs mesoporous layer in 510οC. In order to prepare the TiO2/UCNPs mesoporous layer, UCNPs and TiO2 particles are blended and sintered at 510oC for 30 min (Experiment Section in Supporting Information). Figure 1c and 1d depict the scanning electron microscope (SEM) images of TiO2 and TiO2/UCNPs mesoporous layer. Due to the size of UCNPs and TiO2 are very similar, it is hard to determine the existence of UCNPs in TiO2/UCNPs mesoporous layer. XRD was used to verify the components of TiO2/UCNPs mesoporous layer. In addition to the characteristic peaks of UCNPs at 28.2° and 46.9°, the typical diffraction peaks of anatase phase TiO2, including the notable characteristic peaks at 25.3° correspond to (101) (Figure 1f). The peak positions of the sample are consistent with the calculated pattern of anatase phase TiO2 (Joint Committee for Powder Diffraction Standards, JCPDSNo.21-1272).25

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Figure 2. TEM images of (a) UCNPs, (b) TiO2/UCNPs in 510oC. (c) Schematic of TiO2/UCNPs mesoporous layer. Although the agglomeration of nanoparticles are determined in SEM, it is difficult to confirm the formation of the shared interfaces between UCNPs and TiO2. To prove the existence of some shared interfaces, the sintered products are characterized by TEM. The interlayer spacing of 0.315 nm corresponds to the plane (111) of UCNPs was shown in Figure 2a. After sintering, the mixture of TiO2 and UCNPs begin to reunite (Figure 2c). Some crystal interfaces between TiO2 and UCNPs, TiO2 and TiO2 disappear and some shared interfaces are obtained as showed in Figure 2b. It suggests that interlayer spacing of 0.35 nm is corresponds to the anatase (101) plane of TiO2, which is consistent with previous reports.26,27 Especially, the interlayer spacing of 0.315 nm corresponding to (111) plane of cubic UCNPs is also found in Figure 2b.Therefore, these images suggest that an interface existed between TiO2 and UCNPs after sintering at 510oC.

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Figure 3. (a) Crystal and shared interfaces of TiO2 and UCNPs. (b) Fluorescence spectra of UCNPs, TiO2/UCNPs and TiO2/UCNPs in 510oC. (c) Energy level of UCNPs, TiO2, MAPbI3, Spiro-OMeTAD and Au. Table 1 Electrochemical and physical characteristics of MAPbI3, Spiro-OMeTAD and Au. EHOMO/EVB a (V)

EOXb [V vs. NHE]

MAPbI3

-5.4

0.9

Spiro-OMeTAD

-5.2

0.7

Au

-5.1

0.6

a Normal hydrogenelectrode (NHE) vs. vacuum level is 4.5V; b Redox potential is referenced by adding of ferrocene (E(Fc/Fc+)=630 mVvs.NHE).

In order to determine whether the excited electrons in emission level (520, 545 nm) have injected to CB of TiO2 by the shared interfaces (Figure 3a). The room temperature fluorescence spectra of UCNPs, TiO2/UCNPs and TiO2/UCNPs calcined at 510oC are measured with an excitation at 980 nm. Absorption spectra of the UCNP/TiO2 and TiO2 film are shown in Figure S1. For UCNPs, the emission bands at 520 nm (2H11/2–4I15/2), 545 nm (4S3/2–4I15/2) and 660 nm (4F9/2–4I15/2) are all clearly observed in Figure 3b. For TiO2/UCNPs in 510oC, although the red emission band is 6


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as strong as ever, the green emissions at 520 nm and 545 nm are almost disappeared. However, as elucidated in the Figure 1e and 1f, the peak positions of UCNPs correspond well to the peaks of the TiO2/UCNPs. It can be concluded that the disappearance of 520 nm and 545 nm emission bands in TiO2/UCNPs in 510oC is not induced by the structure and phase transition in UCNPs and TiO2. These results suggest that in TiO2/UCNPs in 510oC, the excited electrons located at the green emission level of UCNPs are quenched via a nonradiative path.23 Besides, the fluorescence spectrum of the TiO2/UCNPs is very similar to the UCNPs. The vanishment of green emission bands of TiO2/UCNPs in 510oC can not be induced by adding titanium dioxide simply. Therefore, the disappearance of the green emission bands of TiO2/UCNPs in 510oC is resulted from the calcination of TiO2/UCNPs. It is also consistent with the TEM results above. Calcination causes the disappearance of some crystal interfaces and the formation of some shared interfaces between TiO2 and UCNPs. In this way, the electrons can successfully transmit from the excited levels of UCNPs to CB of the TiO2. According to energy levels of UCNPs, TiO2 and CH3NH3PbI3 (MAPbI3) (Figure 3c), the green emission levels of UCNPs are above the TiO2 CB, and its ground state is below the valence band of MAPbI3 layer. Valence band of MAPbI3 (-5.4 eV) and highest occupied molecular orbital (HOMO) levels of Spiro-OMeTAD and Au (-5.2 eV and -5.1 eV) are shown in Table 1.28 The EOX value can be deduced from the equation of EOX [V vs. NHE] = -4.5-EHOMO (EVB). The EOX value of MAPbI3, Spiro-OMeTAD and Au are calculated as 0.9, 0.7 and 0.6 V vs. NHE.29 Therefore, photoelectrons generated in high excited state of UCNPs can inject into TiO2 CB and the holes on the ground state of UCNPs can be successfully extracted to the valence band of MAPbI3 layer.30

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Figure 4. (a) Cross-sectional SEM and (b) Configuration images of the device with TiO2/UCNPs mesoporous layer. (c) The current density-voltage curves and (d) IPCE measurement of the devices with TiO2/UCNPs and TiO2. Table 2. Parameters of J-V curves of PSCs. Jsc [mA⋅cm-2]

Sample Device with TiO2/UCNPs

Device with TiO2

Voc [V]

FF (%)

PCE (%)

Reverse

21.29

1.06

76.65

17.23

Forward

21.09

1.05

73.05

16.19

Reverse

19.19

1.04

75.84

15.19

Forward

19.12

1.03

70.87

13.91

8


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Figure 5. (a) PCE, (b) Jsc, (c) Voc and (d) FF of the devices with TiO2/UCNPs and TiO2. To verify that the doping of UCNPs into TiO2 mesoporous layer could effectively improve the photocurrent of PSCs, the films with TiO2/UCNPs and TiO2 are fabricated into PSCs devices. As shown in Figure 4a and 4b, the cross section images of optimized PSCs device, the emerging layer sequence of the new structure is FTO/blocking layer/ TiO2/UCNPs/MAPbI3/HTM/Au. The perovskite layer is produced by the method from mixture of MAI and PbI2 as the reported procedures.31-34 We observe that the thickness of MAPbI3 is about 500 nm in cross section image. To clarify the photovoltaic performance of PSCs with TiO2/UCNPs, the optimum current density-voltage (J-V) curves of devices with TiO2 and TiO2/UCNPs mesoporous layer are presented in Figure 4c. The devices with TiO2 mesoporous layer exhibit the poor PCE of 15.19%, with short-circuit photocurrent density (Jsc) of 19.19 mA cm−2. However, by replacing the film with TiO2/UCNPs mesoporous layer, Jsc of the device is increased from 19.19 to 21.29 mA cm−2. Finally, a PCE of 17.23% is obtained on the device with TiO2/UCNPs, which is 13.43% higher than device with TiO2. Table 2 lists the associated photovoltaic parameters of devices with TiO2 and TiO2/UCNPs. Figure 4d represents incident photon-to-current efficiency (IPCE) measurement of the devices with TiO2/UCNPs and TiO2. The IPCE value in region of 350-750 nm is obviously augmented by incorporating UCNPs in mesoporous layer, owing to the electrons directly transmission from UCNPs to TiO2 CB. Besides, the IPCE value has an additional improvement in 660 nm due to red emission bands at about 660 nm of UCNPs. The above results agree well with the conclusion of proposed energy levels in Figure 3c. Besides, the enhancement of Jsc, the open-circuit voltage (Voc) has the slight increasement from 1.04 to 1.06 V. The impedance spectra and light intensity dependence of Voc are collected to investigate the enhancement of Voc.35,36 Figure S2 presents the impedance spectra of devices with TiO2, TiO2/UCNPs (bare) and TiO2/UCNPs at a frequency range from 100000 Hz to 0.1 Hz at 0.8 V bias voltages under dark conditions. The recombination resistance for the device with TiO2 and TiO2/UCNPs (bare) are similar, indicating that the enhancement of Voc is not just the incorporation of UCNPs. By treating TiO2/UCNPs mesoporous layer surface by TiCl4 aqueous solution in this paper (Experimental Section in Supporting Information), the recombination process on the TiO2/UCNPs/MAPbI3 interface is remarkably retarded. Thus, the device with 9



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TiO2/UCNPs represents the increased Voc because of lower recombination. The decreased slope of device with TiO2/UCNPs in Figure S3 also indicates that the device with TiO2/UCNPs exhibiting the reduced trap assisted carrier recombination. The various photovoltaic parameters distributions of 20 devices with TiO2 and TiO2/UCNPs are summarized in Figure 5. The PCE and Jsc of device with TiO2/UCNPs are obviously enhanced by absorbing NIR light.

CONCLUSION In

conclusion,

we

successfully

incorporated

UCNPs

into

TiO2

as

mesoporous layer in PSCs. The shared interface between TiO2 and UCNPs was formed by calcination at 510oC. The TEM and fluorescence spectrum of mesoporous layer confirmed the formation of the shared interface between TiO2 and UCNPs. The electrons on the green emission level (520, 545 nm) can inject to the TiO2 CB by the shared interfaces. In addition, the visible light at 660 nm can be absorbed by perovskite layer. At last, the device with TiO2/UCNPs mesoporous layer obtain the best PCE of 17.23%.

ACKNOWLEDGMENTS This work was supported by the National Key Basic Research Program of China (973 Program) under Grant No.

2015CB932201,

the

National

Key

Research

and

Development Program of China (NO. 2016YFA0202400), the 111 project (NO. B16016), and the National Natural Science Foundation of China (No. 51572080, 51772095, 51702096, and U1705256), the Fundamental Research Funds for the Central Universities (2018QN055).

ASSOCIATED CONTENT Supporting Information. Experimental section; Absorption spectrum of UCNP/TiO2 film; Nyquist plots for devices with TiO2, TiO2/UCNPs and TiO2/UCNPs with TiCl4; Light intensity dependence of open-circuit voltage for devices with TiO2/UCNPs and TiO2

AUTHOR INFORMATION 10


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Corresponding Author *E-mail: [email protected] (Y Ding) *E-mail: [email protected] (LE Mo) *E-mail: [email protected]. Phone: +86 1061772268

Notes The authors declare no competing financial interest.

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The up-conversion material is incorporated into TiO2 mesoporous layer for highly efficient perovskite solar cells to utilize NIR light

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Highly Efficient Infrared Light-Converting Perovskite Solar Cells: Direct

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