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Ruddlesden-Popper 钙钛矿
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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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 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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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 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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ELECTROCHIMICA ACTA · 2022 · IF 7.336

In-situ construction of Ruddlesden-Popper/perovskite heterointerface induces efficient bifunctional oxygen electrocatalyst for rechargeable zinc-air batteries

Guohong Pan,Yanzhu Deng,Ling Zhao,Huanwen Wang,Rui Wang,Jun Jin,Yansheng Gong,Beibei He

Oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are the prerequisite reactions in rechargeable zinc-air batteries (ZABs), but their kinetics are usually slow. In order to develop energy-efficient ZABs, it is highly desirable to pursue bifunctional catalysts with the accelerated reaction kinetics and the reduced overpotentials. Transition metal oxides are expected as promising alternatives to replace noble metal-based catalysts, but their catalytic activities are still far from desirable. Herein, we propose a modified layer of Ruddlesden-Popper perovskite (Pr,Sr) 2 Ni 0.5 Co 0.5 O 4-δ (RP-PSNC) on the perovskite PrNi 0.5 Co 0.5 O 3-δ (P-PNC) nanofiber by a simple impregnation method, receiving a (Pr,Sr) 2 Ni 0.5 Co 0.5 O 4-δ / PrNi 0.5 Co 0.5 O 3-δ (RP-PSNC/P-PNC) heterostructured nanofibers. The RP-PSNC/P-PNC hybrid catalyst exhibits a small overpotential and an excellent stability due to the large number of vacancies in the two-phase interface. The RP-PSNC/P-PNC-based liquid rechargeable ZAB reaches a power density of 145 mW cm −2 , and 230 h of long-term cycle performance. When assembled into flexible ZABs, it can also reach a power density of 51 mW cm −2 and a stable open circuit voltage (∼1.35 V) for 44 h. These results indicate that the bifunctional electrocatalyst of heterostructured RP-PSNC/P-PNC provides a new path for the modification of perovskites through multi-phase catalysts system, and has great potential in rechargeable ZABs and other energy conversion devices.

研究领域: 材料科学 · 能源化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Enhancing oxygen evolution reaction performance of Ruddlesden–Popper perovskite oxide through heteroatom incorporation

Shu-Fang Li,Bao-Qin Zhang,Yu-Qing Wang,Dong Yan

Prior studies have demonstrated that Ruddlesden–Popper (RP) type perovskite oxides exhibit promising electrocatalytic properties for oxygen evolution reaction (OER). However, the limited electrocatalytic activity has impeded their widespread utilization. The incorporation of heteroatoms into the Ruddlesden–Popper type structure has been identified as an effective strategy to enhance the electrocatalytic performance. This research presents the systematic design and synthesis of RP type perovskite oxide LaSrFeO 4 (LSFO), followed by the optimization of electrocatalytic activity through Ni substitution at the Fe site of SLFO to create LaSrFe 1- x Ni x O 4 (LSFNO- x , x  = 0.2, 0.4, and 0.5). Therein, the LSFNO-0.4 sample achieved a current density of 10 mA·cm −2 with an overpotential of only 340 mV. Additionally, it displayed exceptional stability over 120 h in a 1.0 M KOH solution. Both experimental and theoretical studies suggest that the addition of Ni cation increases the Fe − O covalency, and impacts the morphology and surface electron density of LSFO. This substitution results in a greater electrochemically active surface area, improved electron transfer, and optimization of hydrogen/water absorption free energy. This study presents a successful approach for enhancing the OER performance of Ruddlesden–Popper LSFO through the deliberate control of Fe − O covalent bonding.

CAS / MDL: 10277-43-7
研究领域: 材料科学 · 电化学 · 催化
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EcoMat · 2024 ·Vol. 6 ·期 12 ·e12501 · IF 10.7

A universal reverse-cool annealing strategy makes two-dimensional Ruddlesden-popper perovskite solar cells stable and highly efficient with Voc exceeding 1.2 V

Zhongqi Xie,Huiming Luo,Qing-Song Jiang,Ya Zhao,Yong Peng,Ligang Yuan,Keyou Yan,Mojtaba Abdi-Jalebi

Two-dimensional Ruddlesden-Popper (2D RP) layered metal-halide perovskites have garnered increasing attention due to their favorable optoelectronic properties and enhanced stability in comparison to their three-dimensional counterparts. Nevertheless, precise control over the crystal orientation of 2D RP perovskite films remains challenging, primarily due to the intricacies associated with the solvent evaporation process. In this study, we introduce a novel approach known as reverse-cool annealing (RCA) for the fabrication of 2D RP perovskite films. This method involves a sequential annealing process at high and low temperatures for wet perovskite films. The resulting RCA-based perovskite films show the smallest root-mean-square value of 23.1 nm, indicating a minimal surface roughness and a notably compact and smooth surface morphology. The low defect density in these 2D RP perovskite films with exceptional crystallinity suppresses non-radiative recombination, leading to a minimal non-radiative open-circuit voltage loss of 149 mV. Moreover, the average charge lifetime in these films is extended to 56.3 ns, thanks to their preferential growth along the out-of-plane direction. Consequently, the leading 2D RP perovskite solar cell achieves an impressive power conversion efficiency of 17.8% and an open-circuit voltage of 1.21 V. Additionally, the stability of the 2D RP perovskite solar cell, even without encapsulation, exhibits substantial improvement, retaining 97.4% of its initial efficiency after 1000 hours under a nitrogen environment. The RCA strategy presents a promising avenue for advancing the commercial prospects of 2D RP perovskite solar cells.

研究领域: 材料科学 · 能源技术 · 纳米技术 · 固体物理学
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FUEL · 2024 · IF 6.7

Boosting the catalytic activity of high-order Ruddlesden–Popper perovskite SrEu2Fe2O7-δ air electrode by A-site La doping for CO2 electrolysis in solid oxide electrolysis cells

Pengkai Shan,Hui Ye,Bin Qian,Yifeng Zheng,Guoping Xiao

Ruddlesden–Popper (R-P) oxides (A n+1 B n O 3n+1 ) are potential air electrodes for solid oxide electrolysis cells (SOECs) because of their good electrochemical performance. Among them, SrEu 2 Fe 2 O 7-δ (SEF) with n = 2 has received extensive attention because of its special structure and promising ionic–electronic conductivity. However, the SEF material is prone to degradation at high temperatures (600 °C–800 °C), and its long-term stability is easily affected. In this study, R-P oxide Sr 1-x La x Eu 2 Fe 2 O 7-δ (SLEFx; x = 0, 0.05, 0.1) was successfully synthesized using the sol–gel method. XRD results showed that La-doped SEF displayed good chemical and thermal compatibility with the gadolinia-doped ceria electrolyte. The SLEF0.05 electrode exhibited a polarization resistance of 0.075 Ω cm 2 at 800 °C, which was 88.2 % lower than that of SEF. The half-cell based on the SLEF0.05 air electrode exhibited improved performance under the long-term stability test at a current density of − 0.5 A cm −2 for over 110 h at 800 °C, indicating excellent stability. Moreover, an electrolysis current density as high as 0.712 A cm −2 at 1.5 V was obtained for the full cell with the SLEF0.05 air electrode, which was 45.8 % higher than the SEF electrode when the temperature and feed gas were 800 °C and 50 % CO 2 –50 % CO, respectively. The XPS and cell testing results confirmed that La with high valance and small radius promoted the formation of oxygen vacancies and effectively enhanced the electrochemical performance and structural stability of the SEF material. Therefore, the R-P oxide SLEF0.05 is a promising air electrode material for SOECs.

研究领域: 材料科学 · 电化学 · 能源材料 · 催化
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Enhanced Performance in Quasi-Two-Dimensional Perovskite Photodetectors by Controlling the Formation of a Large N-Phase

Shun Xu,Huafang Zhang,Hong Cui,Haohao Tao,Lingying Cheng,Gencai Pan,Huiping Gao,Zhenlong Zhang,Yanli Mao

Quasi-two-dimensional (2D) Ruddlesden–Popper perovskites (general formula A2Bn–1PbnX3n+1) have received extensive attention in the field of photoelectric detection due to their tunable optical band gap and excellent stability. However, the prepared 2D perovskite films are generally composed of samples with different n values. With the increase of n, the photoelectric performance is improved due to the decreased binding energy, but the thermodynamic stability is decreased. Therefore, it is necessary to find a method that can simultaneously promote the formation of a large n-value perovskite and improve its stability. In this work, we fabricated a photodetector based on the typical quasi-2D perovskite BA2MAPb2I7 (n = 2) and promoted the formation of a large n-phase quasi-2D perovskite in BA2MAPb2I7 by slowing down its recrystallization rate of perovskite through adding a metal–organic framework (ZIF-8) solution on the top of the BA2MAPb2I7 layer. Concurrently, the organic ligands present in ZIF-8 effectively passivated the defects in BA2MAPb2I7 and enhanced its stability. The obtained photodetectors show a high detection rate of 1.03 × 1013 Jones, a high responsiveness of 0.925 A/W, a high switching ratio of 105, and excellent long-term operating stability, light stability, and environmental stability without packaging. This work provides a feasible way to further improve the photoelectric performance and stability of quasi-2D perovskites.

研究领域: 材料科学 · 光电子学 · 钙钛矿光电探测器 · 纳米材料 · 半导体器件
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Journal of Physical Chemistry Letters · 2020 · IF 6.71

Direct Observation of Competition between Amplified Spontaneous Emission and Auger Recombination in Quasi-Two-Dimensional Perovskites

Minghuan Cui,Chaochao Qin,Yuanzhi Jiang,Mingjian Yuan,Liuhong Xu,Didi Song,Yuhai Jiang,Yufang Liu

Quasi-two-dimensional (quasi-2D) Ruddlesden–Popper perovskites (RPPs) have been reported recently as laser media. The carrier dynamics of lasing in quasi-2D RPP films is still controversial. This work presents the amplified spontaneous emission (ASE) at room temperature based on the solution-processed quasi-2D (PEA)2Csn–1PbnBr3n+1 (⟨n⟩ = 3–5) thin films. Transient absorption spectroscopy was conducted to demonstrate the accumulation of excitons and population inversion for ASE caused by the energy transfer process along cascade quantum wells. The competition between the ASE and Auger recombination processes was observed via systematic and quantitative studies on the carrier dynamics. It is found that the contribution of Auger recombination is reduced by decreasing the temperature or adjusting the domain distribution of the quasi-2D RPP films, in order to achieve lower thresholds. This work re-emphasizes the importance of Auger recombination control for achieving low-threshold electrically or continuous-wave driven lasers and deepens the fundamental understanding of charge carrier dynamics of lasing in quasi-2D perovskite films.

研究领域: 材料科学 · 光电子学 · 光子学 · 凝聚态物理
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