共查询到20条相似文献,搜索用时 15 毫秒
1.
Bin Yang Junsheng Chen Songqiu Yang Feng Hong Lei Sun Peigeng Han Prof. Dr. Tõnu Pullerits Prof. Dr. Weiqiao Deng Prof. Dr. Keli Han 《Angewandte Chemie (International ed. in English)》2018,57(19):5359-5363
Lead‐free perovskite nanocrystals (NCs) were obtained mainly by substituting a Pb2+ cation with a divalent cation or substituting three Pb2+ cations with two trivalent cations. The substitution of two Pb2+ cations with one monovalent Ag+ and one trivalent Bi3+ cations was used to synthesize Cs2AgBiX6 (X=Cl, Br, I) double perovskite NCs. Using femtosecond transient absorption spectroscopy, the charge carrier relaxation mechanism was elucidated in the double perovskite NCs. The Cs2AgBiBr6 NCs exhibit ultrafast hot‐carrier cooling (<1 ps), which competes with the carrier trapping processes (mainly originate from the surface defects). Notably, the photoluminescence can be increased by 100 times with surfactant (oleic acid) added to passivate the defects in Cs2AgBiCl6 NCs. These results suggest that the double perovskite NCs could be potential materials for optoelectronic applications by better controlling the surface defects. 相似文献
2.
Wuqian Guo Xitao Liu Shiguo Han Yi Liu Zhiyun Xu Prof. Maochun Hong Prof. Junhua Luo Prof. Zhihua Sun 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(33):13983-13988
Although two-dimensional (2D) metal–halide double perovskites display versatile physical properties due to their huge structural compatibility, room-temperature ferroelectric behavior has not yet been reported for this fascinating family. Here, we designed a room-temperature ferroelectric material composed of 2D halide double perovskites, (chloropropylammonium)4AgBiBr8, using an organic asymmetric dipolar ligand. It exhibits concrete ferroelectricity, including a Curie temperature of 305 K and a notable spontaneous polarization of ≈3.2 μC cm−2, triggered by dynamic ordering of the organic cation and the tilting motion of heterometallic AgBr6/BiBr6 octahedra. Besides, the alternating array of inorganic perovskite sheets and organic cations endows large mobility-lifetime product (μτ=1.0×10−3 cm2 V−1) for detecting X-ray photons, which is almost tenfold higher than that of CH3NH3PbI3 wafers. As far as we know, this is the first study on an X-ray-sensitive ferroelectric material composed of 2D halide double perovskites. Our findings afford a promising platform for exploring new ferroelectric materials toward further device applications. 相似文献
3.
《Angewandte Chemie (International ed. in English)》2017,56(41):12471-12475
Lead‐based perovskite nanocrystals (NCs) have outstanding optical properties and cheap synthesis conferring them a tremendous potential in the field of optoelectronic devices. However, two critical problems are still unresolved and hindering their commercial applications: one is the fact of being lead‐based and the other is the poor stability. Lead‐free all‐inorganic perovskite Cs3Bi2X9 (X=Cl, Br, I) NCs are synthesized with emission wavelength ranging from 400 to 560 nm synthesized by a facile room temperature reaction. The ligand‐free Cs3Bi2Br9 NCs exhibit blue emission with photoluminescence quantum efficiency (PLQE) about 0.2 %. The PLQE can be increased to 4.5 % when extra surfactant (oleic acid) is added during the synthesis processes. This improvement stems from passivation of the fast trapping process (2–20 ps). Notably, the trap states can also be passivated under humid conditions, and the NCs exhibited high stability towards air exposure exceeding 30 days. 相似文献
4.
Chengmin Ji Dhananjay Dey Yu Peng Xitao Liu Lina Li Prof. Junhua Luo 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(43):19095-19099
Polarization-sensitive ultraviolet (UV) photodetection is highly indispensable in military and civilian applications and has been demonstrated with various wide-band photodetectors. However, it still remains elusive to achieve the self-powered devices, which can be operated in the absence of external bias. Herein, for the first time, ferroelectricity-driven self-powered photodetection towards polarized UV light was successfully demonstrated in a 2D wide-band gap hybrid ferroelectric (BPA)2PbBr4 (BPA=3-bromopropylammonium) ( 1 ). We found that the prominent spontaneous polarization in 1 results in a bulk photovoltaic effect (BPVE) of 0.85 V, that independently drives photoexcited carriers separation and transport and thus supports self-powered ability. This self-powered detector shows strong polarization sensitivity to linearly polarized UV illumination with a polarization ratio up to 6.8, which is superior to that of previously reported UV-polarized photodetectors (ZnO, GaN, and GeS2). 相似文献
5.
制备了铅基弛豫铁电体0.9Pb(Mg1/3Nb2/3)O3-0.1PbTiO3和Pb(Zn1/3Nb2/3)O3基陶瓷. 铅基弛豫铁电体PMNT, PZN基陶瓷弛豫过程可用局域冻结模型描述. 在微畴-宏畴转变过程中, 弛豫铁电体产生结构起伏; 在相同的频率条件下, 弛豫铁电体的结构起伏程度越大, 弛豫程度越低. 在微畴-宏畴转变过程中, 随微畴的增大, 弛豫铁电体的弛豫特性减弱或消失. 相似文献
6.
Meiying Leng Zhengwu Chen Ying Yang Dr. Zha Li Kai Zeng Kanghua Li Dr. Guangda Niu Yisu He Qingchao Zhou Prof. Jiang Tang 《Angewandte Chemie (International ed. in English)》2016,55(48):15012-15016
Lead halide perovskite quantum dots (QDs) are promising candidates for future lighting applications, due to their high quantum yield, narrow full width at half maximum (FWHM), and wide color gamut. However, the toxicity of lead represents a potential obstacle to their utilization. Although tin(II) has been used to replace lead in films and QDs, the high intrinsic defect density and oxidation vulnerability typically leads to unsatisfactory material properties. Bismuth, with much lower toxicity than lead, is promising to constitute lead‐free perovskite materials because Bi3+ is isoelectronic to Pb2+ and more stable than Sn2+. Herein we report, for the first time, the synthesis and optical characterization of MA3Bi2Br9 perovskite QDs with photoluminescence quantum yield (PLQY) up to 12 %, which is much higher than Sn‐based perovskite nanocrystals. Furthermore, the photoluminescence (PL) peaks of MA3Bi2X9 QDs could be easily tuned from 360 to 540 nm through anion exchange. 相似文献
7.
《化学:亚洲杂志》2017,12(9):958-962
Perovskite solar cells are considered a promising technology for solar‐energy conversion, with power conversion efficiencies currently exceeding 20 %. In most of the reported devices, Spiro‐OMeTAD is used for positive‐charge extraction and transport layer. Although a number of alternative hole‐transporting materials with different aromatic or heteroaromatic fragments have already been synthesized, a cheap and well‐performing hole‐transporting material is still in high demand. In this work, a two‐step synthesis of a carbazole‐based hole‐transporting material is presented. Synthesized compounds exhibited amorphous nature, good solubility and thermal stability. The perovskite solar cells employing the newly synthesized material generated a power conversion efficiency of 16.5 % which is slightly lower than that obtained with Spiro‐OMeTAD (17.5 %). The low‐cost synthesis and high performance makes our hole‐transport material promising for applications in perovskite‐based optoelectronic devices. 相似文献
8.
Yitao Dai Corentin Poidevin Cristina Ochoa‐Hernndez Alexander A. Auer Harun Tüysüz 《Angewandte Chemie (International ed. in English)》2020,59(14):5788-5796
Direct selective oxidation of hydrocarbons to oxygenates by O2 is challenging. Catalysts are limited by the low activity and narrow application scope, and the main focus is on active C?H bonds at benzylic positions. In this work, stable, lead‐free, Cs3Bi2Br9 halide perovskites are integrated within the pore channels of mesoporous SBA‐15 silica and demonstrate their photocatalytic potentials for C?H bond activation. The composite photocatalysts can effectively oxidize hydrocarbons (C5 to C16 including aromatic and aliphatic alkanes) with a conversion rate up to 32900 μmol gcat?1 h?1 and excellent selectivity (>99 %) towards aldehydes and ketones under visible‐light irradiation. Isotopic labeling, in situ spectroscopic studies, and DFT calculations reveal that well‐dispersed small perovskite nanoparticles (2–5 nm) possess enhanced electron–hole separation and a close contact with hydrocarbons that facilitates C(sp3)?H bond activation by photoinduced charges. 相似文献
9.
Wuqian Guo Xitao Liu Shiguo Han Yi Liu Zhiyun Xu Maochun Hong Junhua Luo Zhihua Sun 《Angewandte Chemie (International ed. in English)》2020,59(33):13879-13884
Although two‐dimensional (2D) metal–halide double perovskites display versatile physical properties due to their huge structural compatibility, room‐temperature ferroelectric behavior has not yet been reported for this fascinating family. Here, we designed a room‐temperature ferroelectric material composed of 2D halide double perovskites, (chloropropylammonium)4AgBiBr8, using an organic asymmetric dipolar ligand. It exhibits concrete ferroelectricity, including a Curie temperature of 305 K and a notable spontaneous polarization of ≈3.2 μC cm?2, triggered by dynamic ordering of the organic cation and the tilting motion of heterometallic AgBr6/BiBr6 octahedra. Besides, the alternating array of inorganic perovskite sheets and organic cations endows large mobility‐lifetime product (μτ=1.0×10?3 cm2 V?1) for detecting X‐ray photons, which is almost tenfold higher than that of CH3NH3PbI3 wafers. As far as we know, this is the first study on an X‐ray‐sensitive ferroelectric material composed of 2D halide double perovskites. Our findings afford a promising platform for exploring new ferroelectric materials toward further device applications. 相似文献
10.
Muhammed Hamdan Aravind Kumar Chandiran 《Angewandte Chemie (International ed. in English)》2020,59(37):16033-16038
Halide perovskites show incredible photovoltaic power conversion efficiency coupled with several hundreds of hours of device stability. However, their stability is poor in aqueous electrolyte media. Reported here is a vacancy ordered halide perovskite, Cs2PtI6, which shows extraordinary stability under ambient conditions (1 year), in aqueous media of extreme acidic (pH 1), basic (pH 13), and under electrochemical reduction conditions. It was employed as an electrocatalyst and photoanode for hydrogen production and water oxidation, respectively. The catalyst remains intact for at least 100 cycles of electrochemical cycling and six hours of hydrogen production at pH 1. Cs2PtI6 was employed as a photoanode for PEC water oxidation, and the material displayed a photocurrent of 0.8 mA cm?2 at 1.23 V (vs. RHE) under simulated AM1.5G sunlight. Using constant voltage measurement, Cs2PtI6 exhibited over 12 hours of PEC stability without loss of performance. 相似文献
11.
Muhammed Hamdan Dr. Aravind Kumar Chandiran 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):16167-16172
Halide perovskites show incredible photovoltaic power conversion efficiency coupled with several hundreds of hours of device stability. However, their stability is poor in aqueous electrolyte media. Reported here is a vacancy ordered halide perovskite, Cs2PtI6, which shows extraordinary stability under ambient conditions (1 year), in aqueous media of extreme acidic (pH 1), basic (pH 13), and under electrochemical reduction conditions. It was employed as an electrocatalyst and photoanode for hydrogen production and water oxidation, respectively. The catalyst remains intact for at least 100 cycles of electrochemical cycling and six hours of hydrogen production at pH 1. Cs2PtI6 was employed as a photoanode for PEC water oxidation, and the material displayed a photocurrent of 0.8 mA cm−2 at 1.23 V (vs. RHE) under simulated AM1.5G sunlight. Using constant voltage measurement, Cs2PtI6 exhibited over 12 hours of PEC stability without loss of performance. 相似文献
12.
Fuxiang Ji Johan Klarbring Dr. Feng Wang Dr. Weihua Ning Dr. Linqin Wang Dr. Chunyang Yin Dr. José Silvestre Mendoza Figueroa Dr. Christian Kolle Christensen Dr. Martin Etter Prof. Thomas Ederth Prof. Licheng Sun Prof. Sergei I. Simak Prof. Igor A. Abrikosov Prof. Feng Gao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(35):15303-15306
Environmentally friendly halide double perovskites with improved stability are regarded as a promising alternative to lead halide perovskites. The benchmark double perovskite, Cs2AgBiBr6, shows attractive optical and electronic features, making it promising for high-efficiency optoelectronic devices. However, the large band gap limits its further applications, especially for photovoltaics. Herein, we develop a novel crystal-engineering strategy to significantly decrease the band gap by approximately 0.26 eV, reaching the smallest reported band gap of 1.72 eV for Cs2AgBiBr6 under ambient conditions. The band-gap narrowing is confirmed by both absorption and photoluminescence measurements. Our first-principles calculations indicate that enhanced Ag–Bi disorder has a large impact on the band structure and decreases the band gap, providing a possible explanation of the observed band-gap narrowing effect. This work provides new insights for achieving lead-free double perovskites with suitable band gaps for optoelectronic applications. 相似文献
13.
An Above‐Room‐Temperature Ferroelectric Organo–Metal Halide Perovskite: (3‐Pyrrolinium)(CdCl3)
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Dr. Heng‐Yun Ye Dr. Yi Zhang Dr. Da‐Wei Fu Prof. Ren‐Gen Xiong 《Angewandte Chemie (International ed. in English)》2014,53(42):11242-11247
Hybrid organo–metal halide perovskite materials, such as CH3NH3PbI3, have been shown to be some of the most competitive candidates for absorber materials in photovoltaic (PV) applications. However, their potential has not been completely developed, because a photovoltaic effect with an anomalously large voltage can be achieved only in a ferroelectric phase, while these materials are probably ferroelectric only at temperatures below 180 K. A new hexagonal stacking perovskite‐type complex (3‐pyrrolinium)(CdCl3) exhibits above‐room‐temperature ferroelectricity with a Curie temperature Tc=316 K and a spontaneous polarization Ps=5.1 μC cm?2. The material also exhibits antiparallel 180° domains which are related to the anomalous photovoltaic effect. The open‐circuit photovoltage for a 1 mm‐thick bulky crystal reaches 32 V. This finding could provide a new approach to develop solar cells based on organo–metal halide perovskites in photovoltaic research. 相似文献
14.
Pressure‐Induced Emission Enhancement,Band‐Gap Narrowing,and Metallization of Halide Perovskite Cs3Bi2I9
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Long Zhang Chunming Liu Lingrui Wang Prof. Cailong Liu Prof. Kai Wang Prof. Bo Zou 《Angewandte Chemie (International ed. in English)》2018,57(35):11213-11217
Low‐toxicity, air‐stable bismuth‐based perovskite materials are attractive substitutes for lead halide perovskites in photovoltaic and optoelectronic devices. The structural, optical, and electrical property changes of zero‐dimensional perovskite Cs3Bi2I9 resulting from lattice compression is presented. An emission enhancement under mild pressure is attributed to the increase in exciton binding energy. Unprecedented band gap narrowing originated from Bi?I bond contraction, and the decrease in bridging Bi‐I‐Bi angle enhances metal halide orbital overlap, thereby breaking through the Shockley–Queisser limit under relatively low pressure. Pressure‐induced structural evolutions correlate well with changes in optical properties, and the changes are reversible upon decompression. Considerable resistance reduction implies a semiconductor‐to‐conductor transition at ca. 28 GPa, and the final confirmed metallic character by electrical experiments indicates a wholly new electronic property. 相似文献
15.
卤化钙钛矿由于具有低成本、高效率等特点,最近作为非常有前景的太阳能电池吸收层材料被广泛研究。卤化钙钛矿型太阳能电池效率在短短的几年间由3.8%(2009年)迅速增加到22.1%(2016年)。卤化钙钛矿型太阳能电池的出现彻底改变了太阳能电池领域,不仅因为它们快速增长的效率,而且因为它们在材料生长和结构方面的可控性。卤化钙钛矿型太阳能电池的优越性能说明卤化钙钛矿材料具有独特的物理性质。在本综述中,我们总结了卤化钙钛矿材料最近几年在结构、电学、光学方面的理论研究成果,这些都与它们在太阳能电池方面的应用密切相关。我们也将探讨一些卤化钙钛矿型太阳能电池目前遇到的挑战以及可能的理论解决途径。 相似文献
16.
Fuxiang Ji Johan Klarbring Feng Wang Weihua Ning Linqin Wang Chunyang Yin Jos Silvestre Mendoza Figueroa Christian Kolle Christensen Martin Etter Thomas Ederth Licheng Sun Sergei I. Simak Igor A. Abrikosov Feng Gao 《Angewandte Chemie (International ed. in English)》2020,59(35):15191-15194
Environmentally friendly halide double perovskites with improved stability are regarded as a promising alternative to lead halide perovskites. The benchmark double perovskite, Cs2AgBiBr6, shows attractive optical and electronic features, making it promising for high‐efficiency optoelectronic devices. However, the large band gap limits its further applications, especially for photovoltaics. Herein, we develop a novel crystal‐engineering strategy to significantly decrease the band gap by approximately 0.26 eV, reaching the smallest reported band gap of 1.72 eV for Cs2AgBiBr6 under ambient conditions. The band‐gap narrowing is confirmed by both absorption and photoluminescence measurements. Our first‐principles calculations indicate that enhanced Ag–Bi disorder has a large impact on the band structure and decreases the band gap, providing a possible explanation of the observed band‐gap narrowing effect. This work provides new insights for achieving lead‐free double perovskites with suitable band gaps for optoelectronic applications. 相似文献
17.
Lang Liu Yang Bai Xiao Zhang Yuequn Shang Chenyue Wang Hao Wang Cheng Zhu Chen Hu Jiafeng Wu Huanping Zhou Yujing Li Shihe Yang Zhijun Ning Qi Chen 《Angewandte Chemie (International ed. in English)》2020,59(15):5979-5987
Lead halide perovskites with mixed cations/anions often suffer from phase segregation, which is detrimental to device efficiency and their long‐term stability. During perovskite film growth, the gel stage (in between liquid and crystalline) correlates to phase segregation, which has been rarely explored. Herein, cation diffusion kinetics are systematically investigated at the gel stage to develop a diffusion model obeying Fick's second law. Taking 2D layered perovskite as an example, theoretical and experimental results reveal the impact of diffusion coefficient, temperature, and gel duration on the film growth and phase formation. A homogenous 2D perovskite thin film was then fabricated without significant phase segregation. This in‐depth understanding of gel stage and relevant cation diffusion kinetics would further guide the design and processing of halide perovskites with mixed composition to meet requirements for optoelectronic applications. 相似文献
18.
Wenxin Mao Christopher R. Hall Anthony S. R. Chesman Craig Forsyth Yi‐Bing Cheng Noel W. Duffy Trevor A. Smith Udo Bach 《Angewandte Chemie (International ed. in English)》2019,58(9):2893-2898
Mixed organolead halide perovskites (MOHPs), CH3NH3Pb(BrxI1?x)3, have been shown to undergo phase segregation into iodide‐rich domains under illumination, which presents a major challenge to their development for photovoltaic and light‐emitting devices. Recent work suggested that phase‐segregated domains are localized at crystal boundaries, driving investigations into the role of edge structure and the growth of larger crystals with reduced surface area. Herein, a method for growing large (30×30×1 μm3) monocrystalline MAPb(BrxI1?x)3 single crystals is presented. The direct visualization of the growth of nanocluster‐like I‐rich domains throughout the entire crystal revealed that grain boundaries are not required for this transformation. Narrowband fluorescence imaging and time‐resolved spectroscopy provided new insight into the nature of the phase‐segregated domains and the collective impact on the optoelectronic properties. 相似文献
19.
Inorganic-organic halide perovskites pose a once-in-a-generation opportunity to revolutionize photovoltaic technology as they are excellent semiconductor candidates with a combination of many desirable attributes. Specifically, halide perovskite solar cells with extremely high device efficiency are easily fabricated and present great promise for commercialization in the near future. However, their non-ideal environmental stability under real operating conditions can limit their further development. Both the academic and industrial research communities have been devoting considerable effort to overcome this critical deficiency through material and device engineering. Significant progress has been reported in this direction, and in this perspective, we review the recent strategies that promise to improve solar cell stability focusing on two interwoven topics. The first one is the development of environmentally stable semiconductor materials, while the second one is dedicated to the reported progress in improving solar cell device stability. Although, the currently adopted methods have not resolved the above problems, yet they build a foundation of principles for future advances to overcome them. In this regard, we believe commercial perovskite-related photovoltaics might indeed be on the horizon, not only replacing the currently commercially available ones, but also improving them. 相似文献
20.
Siping Liu Dr. Bin Yang Dr. Junsheng Chen Prof. Dr. Donghui Wei Dr. Daoyuan Zheng Qingkun Kong Prof. Dr. Weiqiao Deng Prof. Dr. Keli Han 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(49):22109-22113
Thermally activated delayed fluorescence (TADF) is generally observed in solid-state organic molecules or metal-organic complexes. However, TADF in all-inorganic colloidal nanocrystals (NCs) is rare. Herein, we report the first colloidal synthesis of an air-stable all-inorganic lead-free Cs2ZrCl6 perovskite NCs. The Cs2ZrCl6 NCs exhibit long-lived triplet excited state (138.2 μs), and feature high photoluminescence (PL) quantum efficiency (QY=60.37 %) due to TADF mechanism. The emission color can be easily tuned from blue to green by synthesizing the mixed-halide Cs2ZrBrxCl6−x (0≤x≤1.5) NCs. Femtosecond transient absorption and temperature dependent PL measurements are performed to clarify the emission mechanism. In addition, Bi3+ ions are successfully doped into Cs2ZrCl6 NCs, which further extends the PL properties. This work not only develops a new lead-free halide perovskite NCs for potential optoelectronic applications, but also offers unique strategies for developing new inorganic phosphors. 相似文献