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Ruddlesden-Popper
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2023 · IF 10.9

Effects of pressure and doping on Ruddlesden-Popper phases Lan+1NinO3n+1

Mingxin Zhang,Cuiying Pei,Qi Wang,Yi Zhao,Changhua Li,Weizheng Cao,Shihao Zhu,Juefei Wu,Yanpeng Qi

Recently, the discovery of superconductivity with a critical temperature T c up to 80 K in Ruddlesden–Popper phases La n +1 Ni n O 3 n +1 ( n = 2) under pressure has garnered considerable attention. Up to now, the superconductivity was only observed in La 3 Ni 2 O 7 single crystal grown with the optical-image floating zone furnace under oxygen pressure. It remains to be understood the effect of chemical doping on superconducting La 3 Ni 2 O 7 as well as other Ruddlesden–Popper phases. Here, we systematically investigate the effect of external pressure and chemical doping on polycrystalline Ruddlesden–Popper phases. Our results demonstrate that the application of pressure and doping effectively tunes the transport properties of Ruddlesden–Popper phases. We find pressure-induced superconductivity up to 86 K in La 3 Ni 2 O 7 polycrystalline sample, while no signatures of superconductivity are observed in La 2 NiO 4 and La 4 Ni 3 O 10 polycrystalline samples under high pressure up to 50 GPa. Our study sheds light on the exploration of high- T c superconductivity in nickelates.

研究领域: 凝聚态物理 · 材料科学
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IEEE Sensors Letters · 2025 · IF 2.2

Photodetection and Imaging Applications of BA2MA4Pb5I16 Ruddlesden-Popper Perovskite

Min Zhang,Yuancheng Wang,Xiao Wang,Dingyu Yang

Photodetectors serve as a critical link between photonic and electronic systems, playing a key role in the caption, transmission, and processing of information. Low-dimensional Ruddlesden-Popper (RP) perovskites exhibit remarkable environmental stability, minimal ion migration, and tunable structure, offering significant benefits for the development of stable and practical optoelectronic devices. In this work, the liquid-phase perovskite BA2MA4Pb5I16·xCH3NH2 was effectively synthesized by reacting methylamine gas molecules with RP perovskite powder through a solid-gas interaction, eliminating the requirement for high-boiling-point solvents. Photodetectors and pixelated imaging devices were constructed by spin-coating technique. Detectors with outstanding sensitivity for detecting faint light and fast response capabilities was realized, facilitating high-resolution imaging of various objects. This study offers novel insights and approaches to promote the application of perovskite materials in the field of photodetection and imaging.

CAS / MDL: 1310-58-3 75-05-8
研究领域: 材料科学 · 光电子学 · 纳米技术 · 应用物理学 · 化学工程
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Advanced Energy Materials · 2020 ·Vol. 10 ·期 23 ·2000687 · IF 25.245

Energetics and Energy Loss in 2D Ruddlesden–Popper Perovskite Solar Cells

Jianming Yang,Shaobing Xiong,Jingnan Song,Hongbo Wu,Yihan Zeng,Linyang Lu,Kongchao Shen,Tianyu Hao,Zaifei Ma,Feng Liu,Chungang Duan,Mats Fahlman,Qinye Bao

2D Ruddlesden–Popper perovskites (RPPs) are emerging as potential challengers to their 3D counterpart due to superior stability and competitive efficiency. However, the fundamental questions on energetics of the 2D RPPs are not well understood. Here, the energetics at (PEA) 2 (MA) n −1 Pb n I 3 n +1 /[6,6]-phenyl-C61-butyric acid methyl ester (PCBM) interfaces with varying n values of 1, 3, 5, 40, and ∞ are systematically investigated. It is found that n–n junctions form at the 2D RPP interfaces ( n = 3, 5, and 40), instead of p–n junctions in the pure 2D and 3D scenarios ( n = 1 and ∞). The potential gradient across phenethylammonium iodide ligands that significantly decreases surface work function, promotes separation of the photogenerated charge carriers with electron transferring from perovskite crystal to ligand at the interface, reducing charge recombination, which contributes to the smallest energy loss and the highest open-circuit voltage ( V oc ) in the perovskite solar cells (PSCs) based on the 2D RPP ( n = 5)/PCBM. The mechanism is further verified by inserting a thin 2D RPP capping layer between pure 3D perovskite and PCBM in PSCs, causing the V oc to evidently increase by 94 mV. Capacitance–voltage measurements with Mott–Schottky analysis demonstrate that such V oc improvement is attributed to the enhanced potential at the interface.

研究领域: 材料科学 · 能源工程
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Decoupling excitons behavior of two-dimensional Ruddlesden-Popper PEA2PbI4 nanosheets

Wen Li,Shiyu Yang,Bolin Guo,Xuehai Fu,Xiankan Zeng,Cheng Yan,Jingjing Cao,Qungui Wang,Weiqing Yang

Two-dimensional (2D) Ruddlesden-Popper hybrid organic-inorganic perovskites are the most promising candidates for highly efficient optoelectronic devices due to their remarkable exciton characteristics, adjustable band structure and long-term environmental stability. However, excitons emission behavior of 2D Ruddlesden-Popper perovskites is still unclear. Here we theoretically-experimentally decoupled the excitons behavior in 2D Ruddlesden-Popper PEA 2 PbI 4 nanosheets . Theoretically, the Elliott theory was used to separate exciton and band edge absorptions of PEA 2 PbI 4 nanosheets and determine an exciton binding energy of about 274 meV. Experimentally, spectral-dependent photoluminescence lifetime and excitation powder density-dependent photoluminescence spectra revealed that a distinct photoluminescence tail emission should be derived from localized excitons with lower emission energy than free excitons. Further, the luminescent component of the free excitons and localized excitons with their corresponding densities of states was theoretically decoupled by line-shape analysis of PEA 2 PbI 4 nanosheets photoluminescence spectra, which is consistent with the experimental results demonstrating the existence of localized excitons. Hence, our work provides understanding on the exciton behavior and luminescence mechanism of 2D Ruddlesden-Popper perovskites, which would benefit the prediction of high-performance excitonic devices based on 2D Ruddlesden-Popper perovskites.

研究领域: 材料科学 · 光学 · 物理化学
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ADVANCED MATERIALS · 2018 ·Vol. 30 ·期 21 ·1707166 · IF 21.95

Phase Transition Control for High Performance Ruddlesden–Popper Perovskite Solar Cells

Xu Zhang,Rahim Munir,Zhuo Xu,Yucheng Liu,Hsinhan Tsai,Wanyi Nie,Jianbo Li,Tianqi Niu,Detlef-M. Smilgies,Mercouri G. Kanatzidis,Aditya D. Mohite,Kui Zhao,Aram Amassian,Shengzhong (Frank) Liu

Ruddlesden–Popper reduced-dimensional hybrid perovskite (RDP) semiconductors have attracted significant attention recently due to their promising stability and excellent optoelectronic properties. Here, the RDP crystallization mechanism in real time from liquid precursors to the solid film is investigated, and how the phase transition kinetics influences phase purity, quantum well orientation, and photovoltaic performance is revealed. An important template-induced nucleation and growth of the desired (BA) 2 (MA) 3 Pb 4 I 13 phase, which is achieved only via direct crystallization without formation of intermediate phases, is observed. As such, the thermodynamically preferred perpendicular crystal orientation and high phase purity are obtained. At low temperature, the formation of intermediate phases, including PbI 2 crystals and solvate complexes, slows down intercalation of ions and increases nucleation barrier, leading to formation of multiple RDP phases and orientation randomness. These insights enable to obtain high quality (BA) 2 (MA) 3 Pb 4 I 13 films with preferentially perpendicular quantum well orientation, high phase purity, smooth film surface, and improved optoelectronic properties. The resulting devices exhibit high power conversion efficiency of 12.17%. This work should help guide the perovskite community to better control Ruddlesden–Popper perovskite structure and further improve optoelectronic and solar cell devices.

研究领域: 材料科学 · 光伏技术 · 半导体物理
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Nanomaterials · 2023 ·Vol. 13 ·期 3 ·571 · IF 5.3

Photoluminescence Modulation of Ruddlesden-Popper Perovskite via Phase Distribution Regulation

Xinwei Zhao,Ting Zheng,Weiwei Zhao,Yuanfang Yu,Wenhui Wang,Zhenhua Ni

The intrinsic chaotic phase distribution in Ruddlesden-Popper Perovskite (RPP) hinders its further improvement of photoluminescence (PL) emission and limits its application in optical devices. In this work, we achieve the phase distribution regulation of RPP by varying the composition ratio of organic bulky spacer cations 1-naphthylmethylamine (NMA) and phenylethyl-ammonium (PEA), which is controllable and nondestructive for structures of RPP. By suppressing the small n-phase, the PL intensity emission of RPP is further improved. Through the time-resolved PL (TRPL) measurements, we find the PL lifetime of the sample with 66% PEA concentration increases with the temperature initially and possesses the highest values ofτ1andτ2at ~255 K, indicating the immediate state assisting exciton radiative recombination, and it can be modulated by phase manipulation in RPP. The immediate state may outcompete other non-radiative decay channels for excited carriers, leading to the PL enhancement in RPP, and broadening its further application.

CAS / MDL: 68-12-2
研究领域: 材料科学 · 光学 · 物理化学
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Laurionite Competes with 2D Ruddlesden–Popper Perovskites During the Saturation Recrystallization Process

Jiahui Hou,Yangchun Yu,Sanam Attique,Bingqiang Cao,Shikuan Yang

The room-temperature saturation recrystallization (RTSR) method has been extensively used to prepare all-inorganic lead halide perovskite (e.g., CsPbBr3) nanocrystals. Here, we revealed that the composition of the products prepared by the seemingly simple RTSR method could be extremely complex under different experimental parameters. The pH value of the solution and the protonation tendency of the amines influenced by the amounts and types of introduced amines, oleic acid, and water from the environment determined the composition of the final products. PbBr2, 2D Ruddlesden–Popper perovskites (RPPs) formed by perovskite layers separated by intercalating cations, and laurionite Pb(OH)Br would form under acidic, mildly acidic, and alkaline conditions, respectively. Based on the understanding of the formation mechanism, Pb(OH)Br microparticles with well-defined morphologies were prepared, which could be transformed into highly luminescent CH3NH3PbBr3 with the morphology unchanged. The protonated amine behaves as an intercalating layer during the formation of 2D RPPs. Phenylethylamine (PEA) was proven to be an appropriate amine to prepare pure RPP microplates because of its weaker alkalinity compared to aliphatic amines. The prepared (PEA)2PbBr4 RPP microplates showed strong deep-blue light emission with a PL peak at 415 nm, which could be fine-tuned by changing amines. This study proved the complex reaction pathways of the seemingly simple RTSR method and extended the RTSR method into the fabrication of 2D RPPs and laurionite with promising applications in optoelectronic devices.

研究领域: 材料科学 · 化学 · 光学
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Journal of Physical Chemistry C · 2022 · IF 4.177

Efficient Self-Trapped Exciton Emission in Ruddlesden–Popper Sb-Doped Cs3Cd2Cl7 Perovskites

Yarui Dai,Qilin Wei,Tong Chang,Jialong Zhao,Sheng Cao,Bingsuo Zou,Ruosheng Zeng

Metal halide perovskites (MHPs) have attracted extensive attention due to their excellent optoelectronic properties. Among them, layered two-dimensional (2D) metal halide materials with special structures have attracted extensive attention due to their superior stability and optoelectronic properties. Here, we report the 2D Ruddlesden–Popper (RP) phase Cs3Cd2Cl7 synthesized by a solvothermal method, and the photoluminescence quantum yields (PLQYs) of the pristine Cs3Cd2Cl7 sample (PLQY ∼ 10%) can be increased to 68 ± 5% through appropriate Sb3+ doping. This should be the highest PLQY of all reported all-inorganic RP-phase Cd-based perovskites so far. Our results indicate that the highly efficient cyan emission can be attributed to the common self-trapped exciton (STE) emission of the triplet states of Cd2+ and Sb3+ induced by strong electron–phonon coupling, and Sb3+:Cs3Cd2Cl7 has excellent structural and spectral stability. This new material should be a promising candidate for optoelectronic applications in the future.

CAS / MDL: 1309-64-4
研究领域: 材料科学 · 光电 · 化学
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Advanced Energy Materials · 2022 ·Vol. 12 ·期 22 ·2200392 · IF 29.698

Protonic Conduction in La2NiO4+δ and La2-xAxNiO4+δ (A = Ca, Sr, Ba) Ruddlesden–Popper Type Oxides

Peng Zhong,Kazuaki Toyoura,Lulu Jiang,Lubing Chen,Sara Adeeba Ismail,Naoyuki Hatada,Truls Norby,Donglin Han

A significant hydration and protonic conduction in La 2 NiO 4+ δ -based Ruddlesden–Popper (RP) oxides will enable their use as positrode materials in proton ceramic electrochemical cells (PCECs). Unlike perovskite electrolytes and positrode materials, where protons reside and jump on regular oxide ions, RP oxides such as La 2 NiO 4+ δ may contain oxygen interstitials and offer the possibility that protons locate on and migrate by help of these, suggesting a mechanism by which positrodes may operate by triple conduction. Here, theoretical calculations that support proton migration between interstitial oxide ions in the rock-salt layer via unshared oxide ions in the perovskite layer are reported. Furthermore, water contents of pristine La 2 NiO 4+ δ and La 2- x A x NiO 4+ δ ( A = Ca, Sr, Ba) are reported, showing that hydration increases with the level and basicity of the dopant. Hebb-Wagner blocking electrode measurements show significant partial protonic conductivity in all samples. The effects of doping on hydration and of p H 2 O on the p-type conductivity suggest that protons reside primarily on structural oxide ion, but a role of interstitial oxide ions for dissolution and migration of protons cannot be ruled out in cases with oxygen excess. The results are instructive for further studies and optimization of RP oxides as potential positrode materials for PCECs.

研究领域: 材料科学 · 电化学
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JOURNAL OF SOLID STATE CHEMISTRY · 2024 · IF 3.2

Crystal field anisotropy correlated charge disproportionation in Ruddlesden-Popper Sr3-xCaxFe2O7-δ perovskites

Anli Zhang,Songbiao Cao,Jing Li,Na Lv,Pengchao Wei,Ning Zhu,Yijia Bai

A series of Ca 2+ -doped Ruddlesden-Popper phase perovskites Sr 3-x Ca x Fe 2 O 7-δ (x = 0∼0.4) were synthesized. Strong asymmetric FeO 6 octahedral distortion was confirmed at x  = 0.2 owing to the anisotropic chemical pressure applied from preferable occupation of Ca 2+ ion at Sr2 site. Unusual high-charged oxidation state of iron ion with enhanced p → d charge transfer was collectively evidenced by X-ray photoelectron spectroscopy and Mössbauer spectroscopy . Combined electron emission spectroscopy further revealed a narrowing of the surface band gap accompanied by an apparent lowering of the conduction band edge at x = 0.2. These observations can be explained by a nontrivial partial charge disproportionated (CD) regime: d 5 L  +  d 5 L → d 5 L 1− n  +  d 5 L 1+ n , which reflects a significant correlation between anisotropic chemical pressure and CD ground state . The d 5 L 1− n ground state, which dominates the conduction band , is largely stabilized by enhancing the d (Fe)- p (O) hybridization along the c -axis. In addition, abrupt changes in both magnetism and dc electrical properties were also observed at x  = 0.2. It is believed that the anisotropic crystal field correlated electronic state fluctuation of iron may facilitate magnetic phase competition and carrier transport. This work provides a comprehensive understanding of the crystallographic anisotropy and correlated valence electron behavior in Fe-base Ruddlesden-Popper perovskites , as well as quasi two-dimensional perovskite materials.

CAS / MDL: 471-34-1 1633-05-2
研究领域: 材料科学 · 凝聚态物理 · 表面科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Interface engineering of Ruddlesden–Popper perovskite/CeO2/carbon heterojunction for rechargeable zinc-air batteries

Yanzhu Deng,Juwei Du,Yan Zhu,Ling Zhao,Huanwen Wang,Yansheng Gong,Jun Jin,Beibei He,Rui Wang

The development of noble metal-based bifunctional electrocatalysts is the key to driving the sluggish oxygen reduction/evolution reaction (ORR/OER) for rechargeable zinc-air battery applications. There is an urgent need to design and construct robust and cost-efficient bifunctional electrocatalysts . Herein, an interface engineering strategy of Ruddlesden–Popper (RP) perovskite/CeO 2 /carbon heterojunction with core–shell nanostructures is described. Ce-based metal–organic framework derived CeO 2 -C nanosheets are decorated on the surface of RP type perovskite Pr 3 Sr(Ni 0.5 Co 0.5 ) 3 O 10−δ (PSNC) nanofibers . Benefiting from the favorable conductivity, abundant oxygen vacancies and strong interfacial coupling, the hierarchical CeO 2 -C/PSNC electrode delivers a half-wave potential of 0.78 V (ORR), and an OER overpotential of 370 mV at 10 mA cm −2 , respectively. A liquid rechargeable zinc-air battery (ZAB) assembled with CeO 2 -C/PSNC electrocatalysts as the air cathode exhibits a peak power density of 161 mW cm −2 and a long-term cycling life over 219 h. In addition, the CeO 2 -C/PSNC-based all-solid-state cable-type ZAB provides a high open-circuit voltage (∼1.44 V), good flexibility and durability. Our study opens a new insight into the design of efficient electrocatalysts for rechargeable ZABs by constructing hierarchical heterojunctions.

研究领域: 材料科学 · 电化学 · 能源存储与转换
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ENVIRONMENTAL RESEARCH · 2022 · IF 8.431

Copper-based Ruddlesden-Popper perovskite oxides activated hydrogen peroxide for coal pyrolysis wastewater (CPW) degradation: Performance and mechanism

Jinxin Li,Dan Zhong,Yiru Chen,Kefei Li,Wencheng Ma,Shaobo Zhang,Jingna Zhang,Aoshuang Sun,Haijiao Xie

Coal pyrolysis wastewater (CPW) contained all kinds of toxic and harmful components, which would seriously threaten the natural environment and human health. However, the traditional advanced oxidation processes frequently failed to remove phenolic substances. An A 2 BO 4 -type perovskite (La 2 CuO 4 ) was successfully synthesized through sol-gel process and first applied in the treatment of CPW. More than 90% of 3, 5-dimethylphenol (DMP) was removed within 200 min at neutral conditions. Moreover, La 2 CuO 4 also displayed excellent catalytic activity and stability in the actual CPW treatment process. Results demonstrated that DMP was removed through the attack of ∙OH, ∙O 2 − and 1 O 2 in La 2 CuO 4 /H 2 O 2 system. The La 2 CuO 4 were more favorable for H 2 O 2 activation and have a lower adsorption energy than LaFeO 3 . XPS of fresh and spent La 2 CuO 4 illustrated that the decomposition of hydrogen peroxide (H 2 O 2 ) was mainly due to the redox cycle between surface copper and oxygen species. Moreover, the possible degradation pathway of DMP was deduced by identifying degradation products and analyzing density functional theory (DFT) calculations. This research provided a novel strategy for the development of perovskite-based catalytic materials on the treatment of practical CPW.

研究领域: 环境科学 · 材料科学 · 化学工程
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