Liangbin Xiong

Low-Temperature Solution-Processed Tin Oxide as an Alternative Electron Transporting Layer for Efficient Perovskite Solar Cells

Lead halide perovskite solar cells with the high efficiencies typically use high-temperature processed TiO2 as the electron transporting layers (ETLs). Here, we demonstrate that low-temperature solution-processed nanocrystalline SnO2 can be an excellent alternative ETL material for efficient perovskite solar cells. Our best-performing planar cell using such a SnO2 ETL has achieved an average efficiency of 16.02%, obtained from efficiencies measured from both reverse and forward voltage scans. The outstanding performance of SnO2 ETLs is attributed to the excellent properties of nanocrystalline SnO2 films, such as good antireflection, suitable band edge positions, and high electron mobility. The simple low-temperature process is compatible with the roll-to-roll manufacturing of low-cost perovskite solar cells on flexible substrates.

Efficient hole-blocking layer-free planar halide perovskite thin-film solar cells

Efficient lead halide perovskite solar cells use hole-blocking layers to help collection of photogenerated electrons and to achieve high open-circuit voltages. Here, we report the realization of efficient perovskite solar cells grown directly on fluorine-doped tin oxide-coated substrates without using any hole-blocking layers. With ultraviolet-ozone treatment of the substrates, a planar Au/hole-transporting material/CH₃NH₃PbI₃-xClx/substrate cell processed by a solution method has achieved a power conversion efficiency of over 14% and an open-circuit voltage of 1.06 V measured under reverse voltage scan. The open-circuit voltage is as high as that of our best reference cell with a TiO₂ hole-blocking layer. Besides ultraviolet-ozone treatment, we find that involving Cl in the synthesis is another key for realizing high open-circuit voltage perovskite solar cells without hole-blocking layers. Our results suggest that TiO₂ may not be the ultimate interfacial material for achieving high-performance perovskite solar cells.

Performance enhancement of perovskite solar cells with Mg-doped TiO2 compact film as the hole-blocking layer

In this letter, we report perovskite solar cells with thin dense Mg-doped TiO2 as hole-blocking layers (HBLs), which outperform cells using TiO2 HBLs in several ways: higher open-circuit voltage (Voc) (1.08 V), power conversion efficiency (12.28%), short-circuit current, and fill factor. These properties improvements are attributed to the better properties of Mg-modulated TiO2 as compared to TiO2 such as better optical transmission properties, upshifted conduction band minimum (CBM) and downshifted valence band maximum (VBM), better hole-blocking effect, and higher electron life time. The higher-lying CBM due to the modulation with wider band gap MgO and the formation of magnesium oxide and magnesium hydroxides together resulted in an increment of Voc. In addition, the Mg-modulated TiO2 with lower VBM played a better role in the hole-blocking. The HBL with modulated band position provided better electron transport and hole blocking effects within the device.

Effects of annealing temperature of tin oxide electron selective layers on the performance of perovskite solar cells

Efficient lead halide perovskite solar cells have been realized using SnO2 as electron selective layers (ESLs). Here, we report on the effects of the annealing temperature of solution-processed SnO2 ESLs on the performance of perovskite solar cells. We find that the cells using low-temperature annealed SnO2 (LT-SnO2) ESLs outperform the cells using high-temperature annealed SnO2 (HT-SnO2) ESLs, exhibiting higher open circuit voltages and fill factors. Structural, electrical, optical, and electrochemical characterizations reveal the origin of the performance differences: LT-SnO2 produces better film coverage, wider band gap, and lower electron density than that of HT-SnO2. The confluence of these properties results in more effective transportation of electrons and blocking of holes, leading to lower interface recombination. Therefore, LT-SnO2 ESLs are preferred for manufacturing perovskite solar cells on flexible substrates.

Interface engineering in planar perovskite solar cells: energy level alignment, perovskite morphology control and high performance achievement

We report a simple and effective interface engineering method for achieving highly efficient planar perovskite solar cells (PSCs) employing SnO2 electron selective layers (ESLs). Herein, a 3-aminopropyltriethoxysilane (APTES) self-assembled monolayer (SAM) was used to modify the SnO2 ESL/perovskite layer interface. This APTES SAM demonstrates multiple functions: (1) it can increase the surface energy and enhance the affinity of the SnO2 ESL, which induce the formation of high quality perovskite films with a better morphology and enhanced crystallinity. (2) Its terminal functional groups form dipoles on the SnO2 surface, leading to a decreased work function of SnO2 and enlarged built-in potential of SnO2/perovskite heterojunctions. (3) The terminal groups can passivate the trap states at the perovskite surface via hydrogen bonding. (4) The thin insulating layer at the interface can hinder electron back transfer and reduce the recombination process at the interface effectively. With these desirable properties, the best-performing cell employing a APTES SAM modified-SnO2 ESL achieved a PCE over 18% and a steady-state efficiency of 17.54%. Impressively, to the best of our knowledge, the obtained VOC of 1.16 V is the highest value reported for the CH3NH3PbI3 (MAPbI3) system. Our results suggest that the ESL/perovskite interface engineering with a APTES SAM is a promising method for fabricating efficient and hysteresis-less PSCs.

Reducing Hysteresis and Enhancing Performance of Perovskite Solar Cells Using Low-Temperature Processed Y-Doped SnO2 Nanosheets as Electron Selective Layers

Despite the rapid increase of efficiency, perovskite solar cells (PSCs) still face some challenges, one of which is the current-voltage hysteresis. Herein, it is reported that yttrium-doped tin dioxide (Y-SnO2 ) electron selective layer (ESL) synthesized by an in situ hydrothermal growth process at 95 °C can significantly reduce the hysteresis and improve the performance of PSCs. Comparison studies reveal two main effects of Y doping of SnO2 ESLs: (1) it promotes the formation of well-aligned and more homogeneous distribution of SnO2 nanosheet arrays (NSAs), which allows better perovskite infiltration, better contacts of perovskite with SnO2 nanosheets, and improves electron transfer from perovskite to ESL; (2) it enlarges the band gap and upshifts the band energy levels, resulting in better energy level alignment with perovskite and reduced charge recombination at NSA/perovskite interfaces. As a result, PSCs using Y-SnO2 NSA ESLs exhibit much less hysteresis and better performance compared with the cells using pristine SnO2 NSA ESLs. The champion cell using Y-SnO2 NSA ESL achieves a photovoltaic conversion efficiency of 17.29% (16.97%) when measured under reverse (forward) voltage scanning and a steady-state efficiency of 16.25%. The results suggest that low-temperature hydrothermal-synthesized Y-SnO2 NSA is a promising ESL for fabricating efficient and hysteresis-less PSC.

Perovskite Solar Cells Based on Low-Temperature Processed Indium Oxide Electron Selective Layers

Indium oxide (In2O3) as a promising n-type semiconductor material has been widely employed in optoelectronic applications. In this work, we applied low-temperature solution-processed In2O3 nanocrystalline film as an electron selective layer (ESL) in perovskite solar cells (PSCs) for the first time. By taking advantages of good optical and electrical properties of In2O3 such as high mobility, wide band gap, and high transmittance, we obtained In2O3-based PSCs with a good efficiency exceeding 13% after optimizing the concentration of the precursor solution and the annealing temperature. Furthermore, to enhance the performance of the In2O3-based PSCs, a phenyl-C61-butyric acid methyl ester (PCBM) layer was introduced to modify the surface of the In2O3 film. The PCBM film could fill up the pinholes or cracks along In2O3 grain boundaries to passivate the defects and make the ESL extremely compact and uniform, which is conducive to suppressing the charge recombination. As a result, the efficiency of the In2O3-based PSC was improved to 14.83% accompanied with V(OC), J(SC), and FF being 1.08 V, 20.06 mA cm(-2), and 0.685, respectively.

Performance enhancement of high temperature SnO2-based planar perovskite solar cells: electrical characterization and understanding of the mechanism

Mg doping into high temperature processed (HTP) SnO2 as an electron selective layer (ESL) significantly improves perovskite solar cell (PSC) performance including power conversion efficiency (PCE), open circuit voltage, short circuit current (JSC) and fill factor. An optimum Mg content (7.5%) affords a uniform, smooth and dense Mg-doped SnO2 film with high electron mobility and its corresponding PSC displays less hysteresis and achieves a highest steady-state PCE of 14.55%, nearly 92.8% enhancement compared to that with undoped SnO2. Electrical measurements show that suitable Mg doping dramatically reduces free electron density and substantially increases the electron mobility of pristine SnO2. The mechanism of efficiency enhancement for PSCs is proposed as follows: the low free electron density causes suppression of carrier recombination and high electron mobility facilitates fast extraction of electrons from perovskite to ESLs, contributing to an improved JSC. Impedance analysis strongly supports the proposed mechanism and reveals that the higher is the electron mobility, the higher is the electron collection efficiency, and the higher are the JSC and PCE. The HTP SnO2 with a suitable Mg content can be an excellent ESL for PSCs and might well be a suitable candidate of ESLs for CdTe, CuInGaSe and other photovoltaic devices involved in HTP treatment.

In situ synthesis of 3D CoS nanoflake/Ni(OH)2 nanosheet nanocomposite structure as a candidate supercapacitor electrode

A three-dimensional (3D) CoS/Ni(OH)2 nanocomposite structure based on CoS nanoflakes and two-dimensional (2D) Ni(OH)2 nanosheets were in situ synthesized on Ni foam by a whole hydrothermal reaction and electrodeposition process. The 3D CoS/Ni(OH)2 nanocomposite structures demonstrate the combined advantages of a sustained cycle stability of CoS and high specific capacitance from Ni(OH)2. The obtained CoS/Ni(OH)2 nanocomposite structures on Ni foam can directly serve as a binder-free electrode for a supercapacitor. For the 3D CoS/Ni(OH)2 nanocomposite electrode, the high specific capacitance is 1837 F g(-1) at a scan rate of 1 mV s(-1), which is obviously higher than both the bare CoS electrode and Ni(OH)2 electrode. The galvanostatic charge and discharge measurements illustrate that the 3D CoS/Ni(OH)2 nanocomposite electrode possesses excellent cycle stability, and it keeps a 95.8% retention of the initial capacity after 5000 cycles. Electrochemical impedance spectroscopy measurements also confirm that the 3D CoS/Ni(OH)2 nanocomposite electrode has better electrochemical characteristics. These remarkable performances can be attributed to the unique 3D nanoporous structure of CoS/Ni(OH)2 which leads to a large accessible surface area and a high stability during long-term operation. In addition, 2D Ni(OH)2 nanosheets in 3D nanocomposite structures can afford rapid mass transport and a strong synergistic effect of CoS and Ni(OH)2 as individual compositions contribute to the high performance of the nanocomposite structure electrode. These results may promote the design and implementation of nanocomposite structures in advanced supercapacitors.

Effective Carrier‐Concentration Tuning of SnO2 Quantum Dot Electron‐Selective Layers for High‐Performance Planar Perovskite Solar Cells

The carrier concentration of the electron-selective layer (ESL) and hole-selective layer can significantly affect the performance of organic-inorganic lead halide perovskite solar cells (PSCs). Herein, a facile yet effective two-step method, i.e., room-temperature colloidal synthesis and low-temperature removal of additive (thiourea), to control the carrier concentration of SnO2 quantum dot (QD) ESLs to achieve high-performance PSCs is developed. By optimizing the electron density of SnO2 QD ESLs, a champion stabilized power output of 20.32% for the planar PSCs using triple cation perovskite absorber and 19.73% for those using CH3 NH3 PbI3 absorber is achieved. The superior uniformity of low-temperature processed SnO2 QD ESLs also enables the fabrication of ≈19% efficiency PSCs with an aperture area of 1.0 cm2 and 16.97% efficiency flexible device. The results demonstrate the promise of carrier-concentration-controlled SnO2 QD ESLs for fabricating stable, efficient, reproducible, large-scale, and flexible planar PSCs.