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151. High-Rate, Ultra long Cycle-Life Lithium/Sulfur Batteries Enabled by Nitrogen-Doped Graphene

Author

Qiu, Yongcai, Li, Wanfei, Zhao, Wen, Li, Guizhu, Hou, Yuan, Liu, Meinan, Zhou, Lisha, Ye, Fangmin, Li, Hongfei, Wei, Zhanhua, Yang, Shihe, Duan, Wenhui, Ye, Yifan, Guo, Jinghua, Zhang, Yuegang, Qiu, Yongcai, Li, Wanfei, Zhao, Wen, Li, Guizhu, Hou, Yuan, Liu, Meinan, Zhou, Lisha, Ye, Fangmin, Li, Hongfei, Wei, Zhanhua, Yang, Shihe, Duan, Wenhui, Ye, Yifan, Guo, Jinghua, and Zhang, Yuegang

Abstract

Nitrogen-doped graphene (NG) is a promising conductive matrix material for fabricating high-performance Li/S batteries. Here we report a simple, low-cost, and scalable method to prepare an additive-free nanocomposite cathode in which sulfur nanoparticles are wrapped inside the NG sheets (S@NG). We show that the Li/S@NG can deliver high specific discharge capacities at high rates, that is, similar to 1167 mAh g(-1) at 0.2 C, similar to 1058 mAh g(-1) at 0.5 C, similar to 971 mAh g(-1) at 1 C, similar to 802 mAh g(-1) at 2 C, and similar to 606 mAh g(-1) at 5 C. The cells also demonstrate an ultralong cycle life exceeding 2000 cycles and an extremely low capacity-decay rate (0.028% per cycle), which is among the best performance demonstrated so far for Li/S cells. Furthermore, the S@NG cathode can be cycled with an excellent Coulombic efficiency of above 97% after 2000 cycles. With a high active S content (6096) in the total electrode weight, the S@NG cathode could provide a specific energy that is competitive to the state-of-the-art Li-ion cells even after 2000 cycles. The X-ray spectroscopic analysis and ab initio calculation results indicate that the excellent performance can be attributed to the well-restored C C lattice and the unique lithium polysulfide binding capability of the N functional groups in the NG sheets. The results indicate that the S@NG nanocomposite based Li/S cells have a great potential to replace the current Li-ion batteries.

Published
2014

152. Cost-efficient clamping solar cells using candle soot for hole extraction from ambipolar perovskites

Author

Wei, Zhanhua, Yan, Keyou, Chen, Haining, Yi, Ya, Zhang, Teng, Long, Xia, Li, Jinkai, Zhang, Lixia, Wang, Jiannong, Yang, Shihe, Wei, Zhanhua, Yan, Keyou, Chen, Haining, Yi, Ya, Zhang, Teng, Long, Xia, Li, Jinkai, Zhang, Lixia, Wang, Jiannong, and Yang, Shihe

Abstract

Ambient-unstable hole transporters and expensive and complicated noble metal electrode deposition are incompatible with the large scale and low-cost production of perovskite solar cells and thus would hamper their commercialization. Herein we report a new modality of perovskite solar cells that do away with the use of conventional hole transporters by directly clamping a selective hole extraction electrode made of candle soot and a deliberately engineered perovskite photoanode. The key soot/perovskite interface, which promotes hole extraction and electron blocking by forming a Schottky junction, was established seamlessly by pre-wetting and reaction embedding the carbon particles. Femtosecond time-resolved photoluminescence revealed a high hole extraction rate at 1.92 ns(-1). We have now achieved 11.02% efficiency, making an important step towards roll-to-roll production of perovskite solar cells.

Published
2014

153. Enhanced Charge Collection for Splitting of Water Enabled by an Engineered Three-Dimensional Nanospike Array

Author

Qiu, Yongcai, Leung, Siu Fung, Wei, Zhanhua, Lin, Qingfeng, Zheng, Xiaoli, Zhang, Yuegang, Fan, Zhiyong, Yang, Shihe, Qiu, Yongcai, Leung, Siu Fung, Wei, Zhanhua, Lin, Qingfeng, Zheng, Xiaoli, Zhang, Yuegang, Fan, Zhiyong, and Yang, Shihe

Abstract

Photoelectrochemical (PEC) water splitting is a promising method of converting solar energy to hydrogen fuel from water using photocatalysts. Despite much effort in preparing mesoporous thin films on planar substrates, relatively little attention has been paid to their deposition on three-dimensional (3D) substrates, which could improve electron collection and enhance light-trapping. Here, we report the first synthesis of hierarchically branched anatase TiO2 nanotetrapods, achieved by dissolution and nucleation processes on a ZnO nanotetrapods template. When used as a photoanode for efficient PEC water splitting, the unique branched anatase TiO2 nanotetrapods yielded a photocurrent density of 0.54 mA cm-2 at applied potential of 0.35 V vs RHE, much higher than that of commercial TiO2 nanoparticles under otherwise identical conditions. Moreover, when the nanotetrapods were deposited on an ordered, purposely engineered 3D F-doped tin oxide (FTO) nanospike array, the photocurrent density was upgraded to 0.72 mA cm-2. This large photocurrent enhancement can be attributed to the ultrahigh contact surface area with the electrolyte, which is bequeathed by the hierarchically branched TiO2 nanotetrapods with a skin layer of vertically aligned ultrathin nanospines, as well as the short charge transport distance and enhanced light-trapping due to the peculiar 3D FTO nanospike array we have engineered by design.

Published
2014

154. A three-dimensional hexagonal fluorine-doped tin oxide nanocone array: A superior light harvesting electrode for high performance photoelectrochemical water splitting

Author

Li, Jinkai, Qiu, Yongcai, Wei, Zhanhua, Lin, Qingfeng, Zhang, Qianpeng, Yan, Keyou, Chen, Haining, Xiao, Shuang, Fan, Zhiyong, Yang, Shihe, Li, Jinkai, Qiu, Yongcai, Wei, Zhanhua, Lin, Qingfeng, Zhang, Qianpeng, Yan, Keyou, Chen, Haining, Xiao, Shuang, Fan, Zhiyong, and Yang, Shihe

Abstract

Photonic nanostructures hold great promise in promoting light harvesting. Here we report the first design and construction of a three-dimensional (3D) hexagonal nanocone array of fluorine-doped tin oxide (FTO) on glass as an excellent electrode for photoelectrochemical (PEC) water splitting. The PEC current density with suitably deposited Ti-doped hematite at 1.23 V vs. the reversible hydrogen electrode (RHE) was increased by 86% to 2.24 ± 0.02 mA cm-2 compared to that with the planar counterpart, mainly ascribable to the special light harvesting effect and the electrode surface area provided by 3D FTO. Upon the embedment of a gold layer to concentrate the incident light onto the hematite layer and the deposition of the Co-Pi catalyst with a modified procedure, the photocurrent experienced a large cathodic shift of onset potential by 360 mV and soared to a high value of 3.39 ± 0.01 mA cm-2 (at 1.23 V), yielding a power conversion efficiency of 0.70% at a potential as low as 0.88 V vs. RHE.

Published
2014

155. High-Performance Hole-Extraction Layer of Sol-Gel-Processed NiO Nanocrystals for Inverted Planar Perovskite Solar Cells

Author

Zhu, Zonglong, Bai, Yang, Zhang, Teng, Liu, Zhike, Long, Xia, Wei, Zhanhua, Wang, Zilong, Zhang, Lixia, Wang, Jiannong, Yan, Feng, Yang, Shihe, Zhu, Zonglong, Bai, Yang, Zhang, Teng, Liu, Zhike, Long, Xia, Wei, Zhanhua, Wang, Zilong, Zhang, Lixia, Wang, Jiannong, Yan, Feng, and Yang, Shihe

Abstract

Hybrid organic/inorganic perovskite solar cells have been rapidly evolving with spectacular successes in both nanostructured and thin-film versions. Herein, we report the use of a simple sol-gel-processed NiO nanocrystal (NC) layer as the hole-transport layer in an inverted perovskite solar cell. The thin NiO NC film with a faceted and corrugated surface enabled the formation of a continuous and compact layer of well-crystallized CH3NH3PbI3 in a two-step solution process. The hole-extraction and -transport capabilities of this film interfaced with the CH3NH3PbI3 film were higher than those of organic PEDOT:PSS layers. The cell with a NiO NC film with a thickness of 30-40nm exhibited the best performance, as a thinner layer led to a higher leakage current, whereas a thicker layer resulted in a higher series resistance. With the NiO film, we observed a cell efficiency of 9.11%, which is by far the highest reported for planar perovskite solar cells based on an inorganic hole-extracting layer.

Published
2014

156. High-Efficiency All-Polymer Solar Cells Based on a Pair of Crystalline Low-Bandgap Polymers

Author

Mu, Cheng, Liu, Peng, Ma, Wei, Jiang, Kui, Zhao, Jingbo, Zhang, Kai, Chen, Zhihua, Wei, Zhanhua, Yi, Ya, Wang, Jiannong, Yang, Shihe, Huang, Fei, Facchetti, Antonio, Ade, Harald, Yan, He, Mu, Cheng, Liu, Peng, Ma, Wei, Jiang, Kui, Zhao, Jingbo, Zhang, Kai, Chen, Zhihua, Wei, Zhanhua, Yi, Ya, Wang, Jiannong, Yang, Shihe, Huang, Fei, Facchetti, Antonio, Ade, Harald, and Yan, He

Abstract

(Chemical Equation Presented) All-polymer solar cells based on a pair of crystalline low-bandgap polymers (NT and N2200) are demonstrated to achieve a high short-circuit current density of 11.5 mA cm-2 and a power conversion efficiency of up to 5.0% under the standard AM1.5G spectrum with one sun intensity. The high performance of these NT:N2200-based cells can be attributed to the low optical bandgaps of the polymers and the reasonably high and balanced electron and hole mobilities of the NT:N2200 blends due to the crystalline nature of the two polymers.

Published
2014

157. Solution-Processed, Barrier-Confined, and 1D Nanostructure Supported Quasi-quantum Well with Large Photoluminescence Enhancement

Author

Yan, Keyou, Zhang, Lixia, Qin, Kuang, Wei, Zhanhua, Yi, Ya, Wang, Jiannong, Yang, Shihe, Yan, Keyou, Zhang, Lixia, Qin, Kuang, Wei, Zhanhua, Yi, Ya, Wang, Jiannong, and Yang, Shihe

Abstract

Planar substrate supported semiconductor quantum well (QW) structures are not amenable to manipulation in miniature devices, while free-standing QW nanostructures, e.g., ultrathin nanosheets and nanoribbons, suffer from mechanical and environmental instability. Therefore, it is tempting to fashion high-quality QW structures on anisotropic and mechanically robust supporting nanostructures such as nanowires and nanoplates. Herein, we report a solution quasi-heteroepitaxial route for growing a barrier-confined quasi-QW structure (ZnSe/CdSe/ZnSe) on the supporting arms of ZnO nanotetrapods, which have a 1D nanowire structure, through the combination of ion exchange and successive deposition assembly. This resulted in highly crystalline and highly oriented quasi-QWs along the whole axial direction of the arms of the nanotetrapod because a transition buffer layer (ZnxCd1-xSe) was formed and in turn reduced the lattice mismatch and surface defects. Significantly, such a barrier-confined QW emits excitonic light similar to 17 times stronger than the heterojunction (HJ)-type structure (ZnSe/CdSe, HJ) at the single-particle level. Time-resolved photoluminescence from ensemble QWs exhibits a lifetime of 10 ns, contrasting sharply with similar to 300 ps for the control HJ sample. Single-particle PL and Raman spectra suggest that the barrier layer of QW has completely removed the surface trap states on the HJ and restored or upgraded the photoelectric properties of the semiconductor layer. Therefore, this deliberate heteroepitaxial growth protocol on the supporting nanotetrapod has realized a several micrometer long QW structure with high mechanical robustness and high photoelectric quality. We envision that such QWs integrated on 1D nanostructures will largely improve the performance of solar cells and bioprobes, among others.

Published
2014

158. Efficient Photoelectrochemical Water Splitting with Ultrathin films of Hematite on Three-Dimensional Nanophotonic Structures

Author

Qiu, Yongcai, Leung, Siu Fung, Zhang, Qianpeng, Hua, Bo, Lin, Qingfeng, Wei, Zhanhua, Tsui, Kwong Hoi, Zhang, Yuegang, Yang, Shihe, Fan, Zhiyong, Qiu, Yongcai, Leung, Siu Fung, Zhang, Qianpeng, Hua, Bo, Lin, Qingfeng, Wei, Zhanhua, Tsui, Kwong Hoi, Zhang, Yuegang, Yang, Shihe, and Fan, Zhiyong

Abstract

Photoelectrochemical (PEC) solar water splitting represents a clean and sustainable approach for hydrogen (H-2) production and substantial research are being performed to improve the conversion efficiency. Hematite (alpha-Fe2O3) is considered as a promising candidate for PEC water splitting due to its chemical stability, appropriate band structure, and abundance. However, PEC performance based on hematite is hindered by the short hole diffusion length that put a constraint on the active layer thickness and its light absorption capability. In this work, we have designed and fabricated novel PEC device structure with ultrathin hematite film deposited on three-dimensional nanophotonic structure. In this fashion, the nanophotonic structures can largely improve the light absorption in the ultrathin active materials. In addition, they also provide large surface area to accommodate the slow surface water oxidation process. As the result, high current density of 3.05 mA cm(-2) at 1.23 V with respect to the reversible hydrogen electrode (RHE) has been achieved on such nanophotonic structure, which is about three times of that for a planar photoelectrode. More importantly, our systematic analysis with experiments and modeling revealed that the design of high performance PEC devices needs to consider not only total optical absorption, but also the absorption profile in the active material, in addition to electrode surface area and carrier collection.

Published
2014

159. Three-dimensional metal/oxide nanocone arrays for high-performance electrochemical pseudocapacitors

Author

Qiu, Yongcai, Zhao, Yihua, Yang, Xiaowei, Li, Wanfei, Wei, Zhanhua, Xiao, Junwu, Leung, Siu Fung, Lin, Qingfeng, Wu, Hongkai, Zhang, Yuegang, Fan, Zhiyong, Yang, Shihe, Qiu, Yongcai, Zhao, Yihua, Yang, Xiaowei, Li, Wanfei, Wei, Zhanhua, Xiao, Junwu, Leung, Siu Fung, Lin, Qingfeng, Wu, Hongkai, Zhang, Yuegang, Fan, Zhiyong, and Yang, Shihe

Abstract

Three-dimensional (3D) electrodes are critical for enabling high-performance power sources. We report here on the design and fabrication, by combining imprint and soft-printing technologies, of 3D nanocone arrays as a novel platform for high performance pseudocapacitors. Such purpose-built 3D nanocone arrays have the advantages of simplicity/versatility/reliability of fabrication, generality to a vast range of active materials, high electrode surface area, and ease of electrolyte permeation. As a demonstration of principle, Au and MnO2 were sequentially deposited forming a 3D Au/MnOx nanocone array electrode for a pseudocapacitor device. This device achieved a specific mass (areal) capacitance of 840.3 F g-1 (88.2 mF cm-2) at a current density of 2 A g-1. Additionally, the asymmetric supercapacitor using the Au/MnOx nanocone array as the positive electrode and a carbon-based material as the negative electrode achieved a capacitance of 108.5 F g-1 at a current density of 1 A g-1, corresponding to an energy density of as high as 46.8 W h kg-1 at a power density of 0.72 kW kg-1. The cell still preserved 96.5% of the initial capacitance even after 2000 cycles at a current density of 2 A g-1. The initial result is at least on a par with those of the best asymmetric supercapacitors reported so far, and thus bolsters the development value of the conductive nanocone arrays for high-performance supercapacitors and other energy-storage devices.

Published
2014

160. Magnetic-field-assisted aerosol pyrolysis synthesis of iron pyrite sponge-like nanochain networks as cost-efficient counter electrodes in dye-sensitized solar cells

Author

Wei, Zhanhua, Qiu, Yongcai, Chen, Haining, Yan, Keyou, Zhu, Zonglong, Kuang, Qin, Yang, Shihe, Wei, Zhanhua, Qiu, Yongcai, Chen, Haining, Yan, Keyou, Zhu, Zonglong, Kuang, Qin, and Yang, Shihe

Abstract

Aerosol pyrolysis of Fe(CO)(5) in an atmosphere of sulfur vapor under a magnetic field is shown to controllably produce iron pyrite (FeS2) three-dimensional nanochain networks. The formation processes of the FeS2 nanochain networks are systematically studied: (1) thermal decomposition of Fe(CO)(5) followed by Fe nanoparticle assembly into one-dimensional chains and then three-dimensional networks under a magnetic field and (2) subsequent sulfurization in a sulfur vapor atmosphere to form a sponge-like thin film of FeS2 nanochain networks. A control experiment performed in the absence of magnetic field yielded randomly packed FeS2 nanoparticles, rather than the inter-connected nanochain networks. The nanochain networks and their surfactant-free surfaces brought about by our new synthesis will enable a host of photoelectric applications. For example, when used as the counter electrode in dye-sensitized solar cells, the FeS2 nanochain networks are almost as efficient as noble Pt, and more impressively, their catalytic activity faded by only 8% even after 2000 cycles. This work opens up fresh opportunities to make smart use of earth-abundant materials in areas of sustainable energy and environment.

Published
2014

161. Selective laser sintering of TiO2 nanoparticle film on plastic conductive substrate for highly efficient flexible dye-sensitized solar cell application

Author

Ming, Liqun, Yang, Huan, Zhang, Wenjun, Zeng, Xianwei, Xiong, Dehua, Xu, Zhen, Wang, Huan, Chen, Wei, Xu, Xiaobao, Wang, Mingkui, Duan, Jun, Cheng, Yi-Bing, Zhang, Jie, Bao, Qiaoliang, Wei, Zhanhua, Yang, Shihe, Ming, Liqun, Yang, Huan, Zhang, Wenjun, Zeng, Xianwei, Xiong, Dehua, Xu, Zhen, Wang, Huan, Chen, Wei, Xu, Xiaobao, Wang, Mingkui, Duan, Jun, Cheng, Yi-Bing, Zhang, Jie, Bao, Qiaoliang, Wei, Zhanhua, and Yang, Shihe

Abstract

In this paper, we report a novel selective laser sintering of TiO2 nanoparticle (Degussa P25) film on plastic conductive substrates for highly efficient flexible dye-sensitized solar cell (DSC) applications. The so-called "selective sintering" means that the absorbed laser energy can effectively promote the electrical contacts between the TiO2 nanoparticles, but does not cause damage to the plastic conductive substrate. The choice of the near-infrared (wavelength = 1064 nm) laser source is critical for the effectiveness of the laser sintering. The laser sintering technology can effectively decrease electron transport resistance and increase recombination resistance of the TiO2 nanoparticle film characterized by electrochemical impedance spectroscopy and transient photovoltage/photocurrent decay measurements, resulting in much improved charge collection efficiency. Thus, compared to the reference sample, the laser sintered film has achieved an improved short-circuit current density from 9.2 to 10.4 mA cm(-2), fill factor from 0.71 to 0.77, and solar conversion efficiency from 4.5% to 5.7%. The fast and effective selective laser sintering technique has great potential to be integrated into scalable roll-to-roll manufacturing of highly efficient flexible DSCs.

Published
2014

162. Near field enhanced photocurrent generation in p-type dye-sensitized solar cells

Author

Xu, Xiaobao, Cui, Jin, Han, Junbo, Zhang, Junpei, Zhang, Yibo, Luan, Lin, Alemu, Getachew, Wang, Zhong, Shen, Yan, Xiong, Dehua, Chen, Wei, Wei, Zhanhua, Yang, Shihe, Hu, Bin, Cheng, Yibing, Wang, Mingkui, Xu, Xiaobao, Cui, Jin, Han, Junbo, Zhang, Junpei, Zhang, Yibo, Luan, Lin, Alemu, Getachew, Wang, Zhong, Shen, Yan, Xiong, Dehua, Chen, Wei, Wei, Zhanhua, Yang, Shihe, Hu, Bin, Cheng, Yibing, and Wang, Mingkui

Abstract

Over the past few decades, the field of p-type dye-sensitized solar cell (p-DSSC) devices has undergone tremendous advances, in which Cu-based delafossite nanocrystal is of prime interest. This paper presents an augment of about 87% improvement in photocurrent observed in a particular configuration of organic dye P1 sensitized CuCrO2 delafossite nanocrystal electrode coupled with organic redox shuttle, 1-methy-1H-tetrazole- 5-thiolate and its disulfide dimer when Au nanoparticles (NPs, with diameter of about 20 nm) is added into the photocathode, achieving a power convert efficiency of 0.31% (measured under standard AM 1.5 G test conditions). Detailed investigation shows that the local electrical-magnetic field effect, induced by Au NPs among the mesoporous CuCrO2 film, can improve the charge injection efficiency at dye/semiconductor interface, which is responsible for the bulk of the gain in photocurrent.

Published
2014

163. Near-Infrared Photoresponse of One-Sided Abrupt MAPbI3/TiO2 Heterojunction through a Tunneling Process.

Author

Yan, Keyou, Wei, Zhanhua, Zhang, Tiankai, Zheng, Xiaoli, Long, Mingzhu, Chen, Zefeng, Xie, Weiguang, Zhang, Teng, Zhao, Yuda, Xu, Jianbin, Chai, Yang, and Yang, Shihe

Subjects
*HETEROJUNCTIONS, *QUANTUM tunneling, *PEROVSKITE, *TITANIUM oxides, *SEMICONDUCTORS, *INFRARED absorption, *PHOTOVOLTAIC power generation, *QUANTUM efficiency
Abstract

Trap states in semiconductors usually degrade charge separation and collection in photovoltaics due to trap-mediated nonradiative recombination. Here, it is found that perovskite can be heavily doped in low concentration with non-ignorable broadband infrared absorption in thick films and their trap states accumulate electrons through infrared excitation and hot carrier cooling. A hybrid one-sided abrupt perovskite/TiO2 p-N heterojunction is demonstrated that enables partial collection of these trap-filled charges through a tunneling process instead of detrimental recombination. The tunneling is from broadband trap states in the wide depleted p-type perovskite, across the barrier of the narrow depleted TiO2 region (<5 nm), to the N-type TiO2 electrode. The trap states inject carriers into TiO2 through tunneling and produce around-unity peak external quantum efficiency, giving rise to near-infrared photovoltaics. The near-infrared response allows photodetecting devices to work in both diode and conductor modes. This work opens a new avenue to explore the near-infrared application of hybrid perovskites. [ABSTRACT FROM AUTHOR]

Published
2016
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165. High-Efficiency All-Polymer Solar Cells Based on a Pair of Crystalline Low-Bandgap Polymers

Author

Mu, Cheng, primary, Liu, Peng, additional, Ma, Wei, additional, Jiang, Kui, additional, Zhao, Jingbo, additional, Zhang, Kai, additional, Chen, Zhihua, additional, Wei, Zhanhua, additional, Yi, Ya, additional, Wang, Jiannong, additional, Yang, Shihe, additional, Huang, Fei, additional, Facchetti, Antonio, additional, Ade, Harald, additional, and Yan, He, additional

Published
2014
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168. High-Rate, Ultralong Cycle-Life Lithium/Sulfur Batteries Enabled by Nitrogen-Doped Graphene

Author

Qiu, Yongcai, primary, Li, Wanfei, additional, Zhao, Wen, additional, Li, Guizhu, additional, Hou, Yuan, additional, Liu, Meinan, additional, Zhou, Lisha, additional, Ye, Fangmin, additional, Li, Hongfei, additional, Wei, Zhanhua, additional, Yang, Shihe, additional, Duan, Wenhui, additional, Ye, Yifan, additional, Guo, Jinghua, additional, and Zhang, Yuegang, additional

Published
2014
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174. Near Field Enhanced Photocurrent Generation in P-type Dye-Sensitized Solar Cells

Author

Xu, Xiaobao, primary, Cui, Jin, additional, Han, Junbo, additional, Zhang, Junpei, additional, Zhang, Yibo, additional, Luan, Lin, additional, Alemu, Getachew, additional, Wang, Zhong, additional, Shen, Yan, additional, Xiong, Dehua, additional, Chen, Wei, additional, Wei, Zhanhua, additional, Yang, Shihe, additional, Hu, Bin, additional, Cheng, Yibing, additional, and Wang, Mingkui, additional

Published
2014
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177. Selective laser sintering of TiO2 nanoparticle film on plastic conductive substrate for highly efficient flexible dye-sensitized solar cell application

Author

Ming, Liqun, primary, Yang, Huan, additional, Zhang, Wenjun, additional, Zeng, Xianwei, additional, Xiong, Dehua, additional, Xu, Zhen, additional, Wang, Huan, additional, Chen, Wei, additional, Xu, Xiaobao, additional, Wang, Mingkui, additional, Duan, Jun, additional, Cheng, Yi-Bing, additional, Zhang, Jie, additional, Bao, Qiaoliang, additional, Wei, Zhanhua, additional, and Yang, Shihe, additional

Published
2014
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180. Perovskite light-emitting diodes with external quantum efficiency exceeding 20 per cent

Author

Lin, Kebin, Xing, Jun, Quan, Li Na, de Arquer, F. Pelayo García, Gong, Xiwen, Lu, Jianxun, Xie, Liqiang, Zhao, Weijie, Zhang, Di, Yan, Chuanzhong, Li, Wenqiang, Liu, Xinyi, Lu, Yan, Kirman, Jeffrey, Sargent, Edward H., Xiong, Qihua, and Wei, Zhanhua

Abstract

Metal halide perovskite materials are an emerging class of solution-processable semiconductors with considerable potential for use in optoelectronic devices1–3. For example, light-emitting diodes (LEDs) based on these materials could see application in flat-panel displays and solid-state lighting, owing to their potential to be made at low cost via facile solution processing, and could provide tunable colours and narrow emission line widths at high photoluminescence quantum yields4–8. However, the highest reported external quantum efficiencies of green- and red-light-emitting perovskite LEDs are around 14 per cent7,9and 12 per cent8, respectively—still well behind the performance of organic LEDs10–12and inorganic quantum dot LEDs13. Here we describe visible-light-emitting perovskite LEDs that surpass the quantum efficiency milestone of 20 per cent. This achievement stems from a new strategy for managing the compositional distribution in the device—an approach that simultaneously provides high luminescence and balanced charge injection. Specifically, we mixed a presynthesized CsPbBr3perovskite with a MABr additive (where MA is CH3NH3), the differing solubilities of which yield sequential crystallization into a CsPbBr3/MABr quasi-core/shell structure. The MABr shell passivates the nonradiative defects that would otherwise be present in CsPbBr3crystals, boosting the photoluminescence quantum efficiency, while the MABr capping layer enables balanced charge injection. The resulting 20.3 per cent external quantum efficiency represents a substantial step towards the practical application of perovskite LEDs in lighting and display.

Published
2018
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182. Versatile and High‐Performance LiTaO3:Tb3+, Gd3+ Perovskite for Multimode Anti‐counterfeiting, Flexible X‐Ray Imaging, Continuous Stress Sensing, and Non‐Real‐Time Recording.

Author

Lyu, Tianshuai, Dorenbos, Pieter, and Wei, Zhanhua

Subjects
*X-ray imaging, *OPTICALLY stimulated luminescence, *PEROVSKITE, *THERMOLUMINESCENCE, *LUMINESCENCE, *GAMMA ray bursts, *CHARGE carriers
Abstract

Multimode luminescence relates to how charge carriers are transported and recombined in response to various physical excitations. It shows promising applications in many fields like advanced anti‐counterfeiting, information storage and encryption. Enabling a stable single compound with multimode luminescence is a unique technology but still remains a challenge. Herein, a versatile and high‐performance energy storage LiTaO3:0.01Tb3+,xGd3+ perovskite is discovered by utilizing the interplay of electron‐trapping defect levels and hole‐trapping Tb3+. It combines an excellent charge carrier storage capacity (≈7 and 12 times higher than state‐of‐the‐art BaFBr(I):Eu2+ and Al2O3:C), >1200 h storage duration, >40 h afterglow, efficient optically stimulated luminescence, persistent mechanoluminescence, and force‐induced charge carrier storage features. Particularly, it well responds to various stimuli channels, i.e., wide‐range X‐rays to 850 nm infrared photons, thermal activation, mechanical force grinding, or compression. To elucidate this multimode luminescence, charge carrier trapping and release processes in LiTaO3:0.01Tb3+,xGd3+ with various physical stimulations will be unraveled by combining the vacuum‐referred binding diagram construction, spectroscopy, thermoluminescence, and mechanoluminescence techniques. The versatile and high‐performance LiTaO3:0.01Tb3+,xGd3+ enables promising proof‐of‐concept multimode luminescence applications in advanced anti‐counterfeiting, flexible X‐ray imaging, continuous compression force sensing, and non‐real‐time recording. [ABSTRACT FROM AUTHOR]

Published
2023
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185. Liquid phase deposition of TiO2 nanolayer affords CH3NH3PbI3/nanocarbon solar cells with high open-circuit voltage.

Author

Chen, Haining, Wei, Zhanhua, Yan, Keyou, Yi, Ya, Wang, Jiannong, and Yang, Shihe

Abstract

Hybrid organic/inorganic perovskite solar cells are attracting intense attention and further developments largely hinge on understanding the fundamental issues involved in the cell operation. In this paper, a liquid phase deposition (LPD) method is developed to design and grow a TiO2 nanolayer at room temperature for carbon-based perovskite solar cells. The TiO2 nanolayer grown on FTO glass is compact but polycrystalline consisting of tiny anatase TiO2 nanocrystals intimately stacked together. By directly exploiting this TiO2 nanolayer in a solar cell of TiO2 nanolayer/CH3NH3PbI3/nanocarbon, we have achieved a Voc as high as 1.07 V, the highest value reported so far for hole transporter-free CH3NH3PbI3 solar cells. This is rationalized by the slower electron injection and longer electron lifetime due to the TiO2 nanolayer, which enhances the electron accumulation in CH3NH3PbI3 and consequently the Voc. By employing a rutile TiO2 nanorod (NR) array as a base structure for the LPD-TiO2 nanolayer to support the CH3NH3PbI3 layer, the photocurrent density is considerably increased without obviously compromising the Voc (1.01 V). As a result, the power conversion efficiency is boosted from 3.67% to 8.61%. More elaborate engineering of the TiO2 nanolayer by LPD in conjunction with judicious interfacing with other components has the potential to achieve higher performances for this type of solar cell. [ABSTRACT FROM AUTHOR]

Published
2014
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186. Efficient Perovskite Light-Emitting Diodes with Chemically Bonded Contact and Regulated Charge Behavior

Author

Zhao, Yaping, Feng, Wenjing, Li, Mingliang, Lu, Jianxun, Qin, Xiangqian, Lin, Kebin, Luo, Jiefeng, Zhang, Wen-Hua, Lim, Eng Liang, and Wei, Zhanhua

Abstract

Efficient charge injection and radiative recombination are essential to achieving high-performance perovskite light-emitting diodes (Pero-LEDs). However, the perovskite emission layer (EML) and the electron transport layer (ETL) form a poor physically interfacial contact and non-negligible charge injection barrier, limiting the device performance. Herein, we utilize a phosphine oxide, 2,4,6-tris[3-(diphenylphosphinyl)phenyl]-1,3,5-triazine (PO-T2T), to treat the perovskite/ETL interface and form a chemically bonded contact. Specifically, PO-T2T firmly bonds on the perovskite’s surface and grain boundaries through a dative bond, effectively passivating the uncoordinated lead defects. Additionally, PO-T2T has high electron mobility and establishes an electron transport highway to bridge the ETL and EML. As a result, a maximum external quantum efficiency (EQEmax) of 22.06% (average EQEmaxof 20.02 ± 1.00%) and maximum luminance (Lmax) of 103286 cd m–2have been achieved for the champion device. Our results indicate that EML/ETL interface modifications are crucial for the fabrication of highly efficient Pero-LEDs.

Published
2023
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187. Efficient Perovskite Light-Emitting Diodes by Buried Interface Modification with Triphenylphosphine Oxide

Author

Zhao, Yaping, Li, Mingliang, Qin, Xiangqian, Yang, PanPan, Zhang, Wen-Hua, and Wei, Zhanhua

Abstract

Metal halide perovskite films are prepared mainly by solution-based methods. However, the preparation process is prone to produce massive defects at the interface between the perovskite emitting layer and the charge transport layers, limiting the perovskite light-emitting diode device performance. Aiming at this problem, researchers have proposed many effective strategies to passivate these interface defects. However, most previous research studies only focus on modifying the perovskite top interface, and very few reports deal with the buried interface. Here, we deposited triphenylphosphine oxide (TPPO) molecules between the perovskite and the hole transport layer (HTL) and realized the buried interface modification. Adding TPPO avoids the contact recombination of the perovskite and HTL and improves the film quality by increasing the substrate wettability. Moreover, the lone pair electrons of P═O can interact with the uncoordinated lead (Pb2+) of the perovskite and passivate halogen vacancy defects, and the insulation property of TPPO helps to balance the injection of holes and electrons. As a result, a maximum external quantum efficiency (EQEmax) of 21.01% was obtained with an average of 18.4 ± 0.9% over 30 devices, and the device reproducibility was greatly enhanced.

Published
2023
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189. Efficient Tin-Based Perovskite Solar Cells Enabled by Precisely Synthesized Single-Isomer Fullerene Bisadducts with Regulated Molecular Packing

Author

Yang, Panpan, Sun, Chao, Fu, Xifeng, Cheng, Shuo, Chen, Jingfu, Zhang, Hui, Nan, Zi-Ang, Yang, Jinxin, Zhao, Xin-Jing, Xie, Li-Qiang, Meng, Lingyi, Tian, Chengbo, and Wei, Zhanhua

Abstract

Designing and synthesizing fullerene bisadducts with a higher-lying conduction band minimum is promising to further improve the device performance of tin-based perovskite solar cells (TPSCs). However, the commonly obtained fullerene bisadduct products are isomeric mixtures and require complicated separation. Moreover, the isomeric mixtures are prone to resulting in energy alignment disorders, interfacial charge loss, and limited device performance improvement. Herein, we synthesized single-isomer C60- and C70-based diethylmalonate functionalized bisadducts (C60BB and C70BB) by utilizing the steric-hindrance-assisted strategy and determined all molecular structures involved by single crystal diffraction. Meanwhile, we found that the different solvents used for processing the fullerene bisadducts can effectively regulate the molecular packing in their films. The dense and amorphous fullerene bisadduct films prepared by using anisole exhibited the highest electron mobility. Finally, C60BB- and C70BB-based TPSCs showed impressive efficiencies up to 14.51 and 14.28%, respectively. These devices also exhibited excellent long-term stability. This work highlights the importance of developing strategies to synthesize single-isomer fullerene bisadducts and regulate their molecular packing to improve TPSCs’ performance.

Published
2023
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190. Inkjet Printing and Instant Chemical Transformation of a CH3NH3PbI3/Nanocarbon Electrode and Interface for Planar Perovskite Solar Cells.

Author

Wei, Zhanhua, Chen, Haining, Yan, Keyou, and Yang, Shihe

Subjects
*INK-jet printing, *NONIMPACT printing, *CHEMICAL amplification, *CATALYSIS, *CARBON compounds
Abstract

A planar perovskite solar cell that incorporates a nanocarbon hole-extraction layer is demonstrated for the first time by an inkjet printing technique with a precisely controlled pattern and interface. By designing the carbon plus CH3NH3I ink to transform PbI2 in situ to CH3NH3PbI3, an interpenetrating seamless interface between the CH3NH3PbI3 active layer and the carbon hole-extraction electrode was instantly constructed, with a markedly reduced charge recombination compared to that with the carbon ink alone. As a result, a considerably higher power conversion efficiency up to 11.60 % was delivered by the corresponding solar cell. This method provides a major step towards the fabrication of low-cost, large-scale, metal-electrode-free but still highly efficient perovskite solar cells. [ABSTRACT FROM AUTHOR]

Published
2014
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193. Exploring the Critical Factors Toward Spectrally Stable Mixed‐Halide Blue Perovskite LEDs.

Author

Wei, Lulu, Tian, Shubing, Sun, Mingze, Song, Ruili, Wang, Yunhu, Zhang, Mingming, Wang, Lei, Wei, Zhanhua, and Xing, Jun

Abstract

Metal mixed‐halide perovskite has demonstrated considerable potential in the development of solution‐treated blue light‐emitting diodes (LEDs) with high external quantum efficiency, excellent color purity, and tunable wavelength. However, the severe phase segregation of mixed‐halide perovskite under bias voltage would lead to the spectral instability of LEDs. Therefore, suppressing phase segregation of Br/Cl perovskite towards spectrally stable blue perovskite LEDs (PeLEDs) is a big challenge. In this work, we systematically explore the influence of perovskite component, preparation conditions, and device structures on the spectral stability of PeLEDs. We have observed that the stable spectra increased the proportion of Cs in the A‐site cations, passivator, and the annealing temperature of perovskite films. Finally, we achieve a spectra‐stable and high‐performance blue PeLED under optimized conditions. Our findings provide important guidance for preparing spectrally stable PeLEDs. [ABSTRACT FROM AUTHOR]

Published
2024
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194. Recrystallizing Sputtered NiOx for Improved Hole Extraction in Perovskite/Silicon Tandem Solar Cells.

Author

Jin, Yongbin, Feng, Huiping, Li, Yingji, Zhang, Hong, Chen, Xuelin, Zhong, Yawen, Zeng, Qinghua, Huang, Jiarong, Weng, Yalian, Yang, Jinxin, Tian, Chengbo, Zhang, Jinyan, Xie, Liqiang, and Wei, Zhanhua

Subjects
*SILICON solar cells, *NICKEL oxide, *SOLAR cells, *COMPLEX compounds, *SURFACE chemistry
Abstract

Sputtering nickel oxide (NiOx) is a production‐line‐compatible route for depositing hole transport layers (HTL) in perovskite/silicon tandem solar cells. However, this technique often results in films with low crystallinity and structural flaws, which can impair electronic conductivity. Additionally, the complex surface chemistry and inadequate Ni3+/Ni2+ ratio impede the effective binding of self‐assembled monolayers (SAMs), affecting hole extraction at the perovskite/HTL interface. Herein, these issues are addressed using a recrystallization strategy by treating sputtered NiOx thin films with sodium periodate (NaIO4), an industrially available oxidant. This treatment improved crystallinity and increased the Ni3+/Ni2+ ratio, resulting in a higher content of nickel oxyhydroxide. These enhancements strengthened the SAM's anchoring capability on NiOx and improved the hole extraction at the perovskite/HTL interface. Moreover, the NaIO4 treatment facilitated Na+ diffusion within the perovskite layer and minimized phase separation, thus improving device stability. As a result, single‐junction perovskite solar cells with a 1.68 eV bandgap achieve a power conversion efficiency (PCE) of 23.22% for an area of 0.12 cm2. Perovskite/silicon tandem cells with an area of 1 cm2 reached a PCE of 30.48%. Encapsulated tandem devices retained 95% of their initial PCE after 300 h of maximum power point tracking under 1‐sun illumination at 25 °C. [ABSTRACT FROM AUTHOR]

Published
2024
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195. Cross‐Linkable Fullerene Electron Transport Layer with Internal Encapsulation Capability for Efficient and Stable Inverted Perovskite Solar Cells.

Author

Hou, Enlong, Cheng, Shuo, Qiu, Yujue, Chen, Xingyu, Chen, Jingfu, Sun, Chao, Zhang, Hui, Yang, Jinxin, Zhao, Xinjing, Xie, Liqiang, Chen, Zuochang, Tian, Chengbo, and Wei, Zhanhua

Abstract

A stable and compact fullerene electron transport layer (ETL) is crucial for high‐performance inverted perovskite solar cells (PSCs). However, traditional fullerene‐based ETLs like C60 and PCBM are prone to aggregate under operational conditions, a challenge recently recognized by academic and industrial researchers. Here, we designed and synthesized a novel cross‐linkable fullerene molecule, bis((3‐methyloxetan‐3‐yl)methyl) malonate‐C60 monoadduct (BCM), for use as an ETL in PSCs. Upon a low‐temperature annealing at 100 °C, BCM undergoes in situ cross‐linking to form a robust cross‐linked BCM (CBCM) film, which demonstrates excellent electron mobility and a suitable band structure for efficient PSCs. Our results show that PSCs incorporating CBCM‐based ETL achieve an impressive efficiency of 25.89 % (certified: 25.36 %), significantly surpassing the 23.25 % efficiency of PCBM‐based devices. The intramolecular covalent interactions within CBCM films effectively prevent aggregation and enhance film compactness, creating an internal encapsulation layer that mitigates the decomposition and ion migration of perovskite components. Consequently, CBCM‐based PSCs show exceptional stability, maintaining 97.8 % of their initial efficiency after 1000 hours of maximum power point tracking, compared to only 78.6 % retention in PCBM‐based devices after less than 820 hours. [ABSTRACT FROM AUTHOR]

Published
2024
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197. Indirect evidence of Bi3+ valence change and dual role of Bi3+ in trapping electrons and holes for multimode X-ray imaging, anti-counterfeiting, and non-real-time force sensing.

Author

Lyu, Tianshuai, Dorenbos, Pieter, and Wei, Zhanhua

Subjects
*VALENCE fluctuations, *X-ray imaging, *BINDING energy, *LEGAL evidence, *LUMINESCENCE quenching, *ELECTRON traps, *CHARGE carriers, *GAMMA ray bursts, *ELECTRIC charge
Abstract

Discovering bismuth based smart materials that can respond to thermal, mechanical, and wide range X-ray to infrared photon excitation remains a challenge. Such materials have various uses like in advanced information encryption. In this work, valence state change between Bi2+, Bi3+, and Bi4+, and the dual role of Bi3+ in trapping electrons and holes have been studied in Bi3+ or/and Ln3+ (Ln=Tb or Pr) doped LiScGeO 4 family of compounds by vacuum referred binding energy (VRBE) diagram construction, thermoluminescence, and spectroscopy. Electron release from Bi2+ has been evidenced. It can be used to experimentally determine the VRBE in the Bi2+ 2P 1/2 ground state and to realize Bi3+ negative quenching luminescence. Particularly, a new force induced charge carrier storage phenomenon has been discovered for non-real-time force recording. Wide range of emission tailorable afterglow, unique Bi3+ ultraviolet-A, white, and infrared afterglow have been demonstrated by using Bi3+ as a hole trapping and recombination center and using energy transfer processes from Bi3+ to Tb3+, Pr3+, Dy3+, or Cr3+. Proof-of-concept advanced anti-counterfeiting, information encryption, and X-ray imaging will be demonstrated. This work not only develops smart storage phosphors, but more importantly unravels the valence change between Bi2+, Bi3+, or Bi4+ and how it can affect the trapping and release of charge carriers with thermal, optical, or mechanical excitation. This work therefore can promote the discovery and development of Bi3+ based smart materials for various applications. Discovering bismuth based smart materials that can respond to thermal, mechanical, and wide range X-ray to infrared photon excitation remains a challenge. Such materials have various uses like in advanced information encryption. In this work, valence state change between Bi2+, Bi3+, and Bi4+, and the dual role of Bi3+ in trapping electrons and holes have been studied in Bi3+ or/and Ln3+ (Ln=Tb or Pr) doped LiScGeO 4 family of compounds by vacuum referred binding energy (VRBE) diagram construction, thermoluminescence, and spectroscopy. Electron release from Bi2+ has been evidenced. [Display omitted] [ABSTRACT FROM AUTHOR]

Published
2024
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198. Efficient and Stable Inverted Perovskite Solar Cells Enabled by a Fullerene‐Based Hole Transport Molecule.

Author

Luo, Jiefeng, Zhang, Hui, Sun, Chao, Hou, Enlong, Wang, Xin, Guo, Sai, Chen, Jingfu, Cheng, Shuo, Chen, Shanshan, Zhao, Xinjing, Xie, Liqiang, Meng, Lingyi, Tian, Chengbo, and Wei, Zhanhua

Subjects
*ENERGY levels (Quantum mechanics), *SOLAR cells, *HOMOGENEOUS nucleation, *CHARGE exchange, *HOLE mobility
Abstract

Designing an efficient modification molecule to mitigate non‐radiative recombination at the NiOx/perovskite interface and improve perovskite quality represents a challenging yet crucial endeavor for achieving high‐performance inverted perovskite solar cells (PSCs). Herein, we synthesized a novel fullerene‐based hole transport molecule, designated as FHTM, by integrating C60 with 12 carbazole‐based moieties, and applied it as a modification molecule at the NiOx/perovskite interface. The in situ self‐doping effect, triggered by electron transfer between carbazole‐based moiety and C60 within the FHTM molecule, along with the extended π conjugated moiety of carbazole groups, significantly enhances FHTM's hole mobility. Coupled with optimized energy level alignment and enhanced interface interactions, the FHTM significantly enhances hole extraction and transport in corresponding devices. Additionally, the introduced FHTM efficiently promotes homogeneous nucleation of perovskite, resulting in high‐quality perovskite films. These combined improvements led to the FHTM‐based PSCs yielding a champion efficiency of 25.58 % (Certified: 25.04 %), notably surpassing that of the control device (20.91 %). Furthermore, the unencapsulated device maintained 93 % of its initial efficiency after 1000 hours of maximum power point tracking under continuous one‐sun illumination. This study highlights the potential of functionalized fullerenes as hole transport materials, opening up new avenues for their application in the field of PSCs. [ABSTRACT FROM AUTHOR]

Published
2024
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199. Management of Triplet States in Modified Mononuclear Ruthenium(II) Complexes for Enhanced Photocatalysis.

Author

Liang, Ping, Wang, Zhaolong, Hao, Siwei, Chen, Kai‐Kai, Wu, Kaifeng, and Wei, Zhanhua

Abstract

Controlling the interplay between relaxation and charge/energy transfer processes in the excited states of photocatalysts is crucial for the performance of artificial photosynthesis. Metal‐to‐ligand charge‐transfer triplet states (3MLCT*) of ruthenium(II) complexes are broadly implemented for photocatalysis, but an effective means of managing the triplets for enhanced photocatalysis has been lacking. Herein, We proposed a strategy to considerably prolong the triplet excited‐state lifetime by decorating a ruthenium(II) phosphine complex (RuP‐1) with pendent polyaromatic hydrocarbons (PAHs). Systematic studies demonstrate that in RuP‐4 decorated with anthracene, sub‐picosecond electron transfer from anthracene to 3MLCT* leads to a charge‐separated state that can mediate the formation of the intra‐ligand triplet state (3IL) of anthracene, resulting in an exceptionally long excited‐state up to several milliseconds. This triplet management strategy enables impressive photocatalytic reduction of CO2 to CO with a turnover number (TON) of 404, an optimized quantum yield of 43 % and 100 % selectivity, which is the highest reported performance for mononuclear photocatalysts without additional photosensitizers. RuP‐4 also catalyzes photochemical hydrogen generation under argon. This work opens up an avenue for regulating the excited‐state charge/energy flow for the development of long‐lived 3IL multi‐functional mononuclear photocatalysts to boost artificial photosynthesis. [ABSTRACT FROM AUTHOR]

Published
2024
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200. Quantitative Surface Passivation Through Drop‐on‐Demand Inkjet Printing Enables Highly Efficient Perovskite Solar Cells.

Author

Tan, Li, Jiang, Hengyi, Yang, Rui, Shen, Lina, Sun, Chao, Jin, Yongbin, Guan, Xiang, Song, Peiquan, Zheng, Lingfang, Tian, Chengbo, Xie, Liqiang, Yang, Jinxin, and Wei, Zhanhua

Subjects
*SURFACE passivation, *SOLAR cells, *PEROVSKITE, *ENERGY levels (Quantum mechanics), *INK, *SILICON solar cells, *SURFACE defects
Abstract

Deposition of a passivation layer on top of the perovskite is proven to be an effective method for improving the efficiency and long‐term stability of perovskite solar cells (PSCs). And the spin‐coating method is the most typical and popular method developed for this purpose. However, the spin‐coating method wastes substantial passivator materials, thus the quantitative relationship between the passivator amount and the device performance cannot be obtained. Herein, a quantitative deposition method is developed through drop‐on‐demand inkjet printing to investigate the influence of 2‐adamantylamine hydrochloride (2‐ADAHCl) deposition surface density on the device performance, which is found to have a significant impact on the device performance. A low deposition surface density of 1.1 µg cm−2 does not reach its optimum passivation capability. In contrast, an excess deposition surface density of 10.1 µg cm−2 would lead to energy level mismatch and large series resistance at the perovskite/hole transport layer (HTL) interface, thus resulting in inferior device properties. At an optimum deposition surface density of 2.5 µg cm−2, perovskite surface defects are greatly suppressed, and the interfacial contact between perovskite and HTL is improved. Finally, PSCs with a high efficiency of 24.57% are achieved with improved operational and environmental stabilities. [ABSTRACT FROM AUTHOR]

Published
2024
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