ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Kegui Li,Xiaoyan Gan,Ruojin Zheng,Haoran Zhang,Maling Xiang,Siqi Dai,Dingjin Du,Feng Zhang,Liling Guo,Hanxing Liu
2D Ruddlesden–Popper (RP) perovskites have appeared as a promising prospective material owing to their tunable optoelectronic peculiarities and structural stability. The choice of interlayer cations greatly influences the performance of the 2D RP perovskites. In this study, through theoretical calculations and experimental investigation, we demonstrate the intrinsic and device performance differences between two perovskites based on cations of thiophenemethylamine (TMA) and thiopheneethylamine (TEA). Using density functional theory (DFT) calculations, it exposes that as compared to (TMA)2PbI4, (TEA)2PbI4 exhibits more pronounced distortion of [PbI6]4– units and possesses a wider band gap and larger effective mass. The experimental results on the TMA- and TEA-based 2D perovskites further show that when TEA is used as the interlayer cation, the crystallization process tends to form more low-n phases, which hinder charge transfer and decrease light harvesting. On the other hand, when TMA is used as the interlayer cation, excessive low-n phases are not observed, and the thin film exhibits excellent quality with significantly improved electron mobility. The (TMA)2(FA)n−1PbnI3n+1 (n = 5) perovskite device shows a remarkable conversion efficiency of 16.56%, much higher than that of TEA-based devices (PCE = 2.58%). Moreover, the unencapsulated devices based on TMA were able to maintain 88% of their initial efficiency even after being exposed to the environment (RT, RH = 30 ± 5%) for a duration of 1080 h. These findings provide important insights into the differences between thiophene-based cations and the selection of organic interlayer cations for 2D RP perovskite solar cells.
研究领域:
材料科学
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太阳能电池
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理论计算
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Chao Huang,Yingnan Dou,Liping Sun,Lihua Huo,Qiang Li,Hui Zhao
The mechanism by which the multicomponent systems in high-entropy perovskites regulate catalytic sites remains unclear, especially how the introduction of A-site elements with different radii influences the B-site catalytic centers. This study designed medium-entropy perovskite oxides, (La 0.2 Pr 0.2 Nd 0.2 Sm 0.2 M 0.2 ) 2 NiO 4 (M = Ca, Sr, Ba), by leveraging the differential ionic potentials of strategically selected alkaline earth metals, with the aim of elucidating how systematic modifications of the local polar environment influence the bonding state of catalytic sites and their electrocatalytic behavior. The differing ionic potentials of the A-site cations (Ca, Sr, Ba) modulate the bond strength and electron cloud overlap of the B-site transition metal‑oxygen bonds. This modulation, primarily through coulombic interactions with the B-site metal ions, induces significant electron transfer and consequently adjusts the energy of the d-band center. This weakened interaction facilitates the generation and migration of active oxygen species by lowering the metal‑oxygen bond strength. Electrochemical results indicate that (La 0.2 Pr 0.2 Nd 0.2 Sm 0.2 Ba 0.2 ) 2 NiO 4 (LPNSBNO) exhibits a low polarization resistance of 0.29 Ω cm 2 at 700 °C. The single cell of LPNSBNO achieved a maximum power density of 0.82 W cm −2 in fuel cell mode. A current density of 0.58 A cm −2 was achieved in electrolyzer mode at 1.3 V and 700 °C. Furthermore, compared to Nd 1.6 Ba 0.4 NiO 4 , the entropy-enhanced LPNSBNO exhibits weaker Ba 2+ surface segregation energy, thereby demonstrating more robust Cr/CO 2 resistance. These results establish LPNSBNO as a catalyst with significant potential for bi-functional applications.
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Zhenfei Li,Haoteng Yuan,Chenzhao Liu,Anas Mousa,Liyuan Fan,Dong Yan,Bin Hua,Lichao Jia
The practical deployment of reversible protonic ceramic cells requires oxygen electrodes that can operate efficiently and reversibly without relying on cobalt- and strontium-containing perovskites, that often suffer from thermal mismatch, surface segregation, and durability degradation. Here, we report a Sr/Co-free Ba/Fe co-doped Ruddlesden–Popper nickelate, Pr 1.8 Ba 0.2 Ni 0.9 Fe 0.1 O 4+δ (PBNF0.1), as an efficient and stable oxygen electrode. Ba incorporation stabilizes the layered Pr 2 NiO 4+δ framework, while Fe substitution regulates the Ni valence state, promotes oxygen-vacancy formation, and enhances hydration capability, thereby improving oxygen-electrode kinetics. Consequently, PBNF0.1 exhibits reduced polarization resistance compared with Pr 1.8 Ba 0.2 NiO 4+δ (PBN) and delivers excellent reversiblecell performance, achieving 1.28 W cm −2 in fuel-cell mode and −2.47 A cm −2 at 1.3 V in electrolysis mode at 700 °C. Stable operation under fuel-cell, electrolysis, and reversible cycling conditions further highlights Ba/Fe co-doping as an effective strategy for durable Sr/Co-free oxygen electrodes.
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高影响因子
Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 12
·4645-4657
·
IF 6.482
Xiangxin Tian,Zhaoxing Hu,Zeliang Gao,Yongzhuan Zhang,Chuanming Li,Hongwei Qi,Xiuping Liu,Rongkun Zheng,Jiangtao Xu,Jingquan Liu
The quasi two-dimensional Ruddlesden–Popper perovskites (RPPs) have drawn unprecedented research attention due to their superior long-term environmental stability, abundant structural diversity, and favorable performance in energy-related application scenarios. Rational molecular design strategies, especially proper selections and modifications on the bulky organic spacer cations, play a vital role in obtaining RPPs with desired properties. Recently, employing fluorinated organic cations for further improving the stability and artificial tuning of the performance of RPP based devices has become a promising strategy. However, the mechanism of how fluorination affects the orientation of the spacer cations and the interactions between the organic slabs and the inorganic frameworks is still controversial and needs further investigations, especially on the structure–property relationship based on well-developed single crystals. Herein, we adopted meta-fluorophenethylamine (3-FPEA) as the spacer cation and successfully synthesized a RPP, (3-FPEA)2PbI4. Centimeter-sized single crystals of this material were grown through the bottom-seeded solution growth (BSSD) method by using hydroiodic acid as the self-solvent. (3-FPEA)2PbI4 exhibits superior thermal stability (from −175 °C to 281 °C), while a reversible phase transition occurs at 212 °C and it remains stable for at least 90 days when exposed to RH 80% at room temperature. Structural refinement and optical characterization indicate that the meta-substitution of fluorine breaks its original symmetry from monoclinic Cc to triclinic P space group accompanying a certain degree of disorder of the Pb2+ ions as well as the equatorial bridging I− ions and leads to a smaller band gap (2.20 eV), blue-shifted photoluminescence peak (516 nm), and longer decay time (τave = 1.36 ns). This work offers further insights into the structure–property relationships of the fluorinated RPPs and provides an effective strategy for designing novel RPPs with superior photoelectric properties.
研究领域:
材料科学
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化学
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物理学
·
光电学
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DOI
高影响因子
ADVANCED MATERIALS
·
2019
·Vol. 31
·期 37
·1901673
·
IF 25.809
Jishan Shi,Yerun Gao,Xiang Gao,Yun Zhang,Junjie Zhang,Xin Jing,Ming Shao
Low-dimensional Ruddlesden–Popper perovskites (RPPs) exhibit excellent stability in comparison with 3D perovskites; however, the relatively low power conversion efficiency (PCE) limits their future application. In this work, a new fluorine-substituted phenylethlammonium (PEA) cation is developed as a spacer to fabricate quasi-2D (4FPEA) 2 (MA) 4 Pb 5 I 16 ( n = 5) perovskite solar cells. The champion device exhibits a remarkable PCE of 17.3% with a J sc of 19.00 mA cm −2 , a V oc of 1.16 V, and a fill factor (FF) of 79%, which are among the best results for low-dimensional RPP solar cells ( n ≤ 5). The enhanced device performance can be attributed as follows: first, the strong dipole field induced by the 4-fluoro-phenethylammonium (4FPEA) organic spacer facilitates charge dissociation. Second, fluorinated RPP crystals preferentially grow along the vertical direction, and form a phase distribution with the increasing n number from bottom to the top surface, resulting in efficient charge transport. Third, 4FPEA-based RPP films exhibit higher film crystallinity, enlarged grain size, and reduced trap-state density. Lastly, the unsealed fluorinated RPP devices demonstrate superior humidity and thermal stability. Therefore, the fluorination of the long-chain organic cations provides a feasible approach for simultaneously improving the efficiency and stability of low-dimensional RPP solar cells.
研究领域:
材料科学
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能源科学
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DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2023
·
IF 6.4
Qing Dai,Qin Ling,Like Huang,Xiaohui Liu,Houcheng Zhang,Jing Zhang,Yuejin Zhu,Ziyang Hu
Two-dimensional (2D) perovskites have attracted significant attention in recent years due to their promising light harvesting and emissive properties. However, the realization of 2D perovskite crystallization with sufficient coverage and reliable reproducibility remains difficult. In this study, controlling the solvent volatilization to achieve high-quality crystallization with full coverage and lateral homogeneity of 2D Ruddlesden–Popper phase perovskite was effectively achieved. It is found that variations in the solvent evaporation rate give rise to lateral film coverage gradients with the degree of grain fusion during the process of hot-casting. As a result, the obtained photovoltaic efficiency varies due to the growth inhomogeneity across hot-casting thin films from center to edge. By adjusting the temperature of the casting perovskite precursor, film inhomogeneity and device performance variation can be alleviated. Regulating radial morphology across hot-casting thin films will enable coating techniques amenable to the solution process for robust reproducibility.
研究领域:
材料科学
·
光伏技术
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DOI
高影响因子
Chemistry-An Asian Journal
·
2021
·Vol. 16
·期 21
·3437-3443
·
IF 4.568
Ke Liu,Chen Li,Ting Wen,Dequan Jiang,Zimin Jiang,Yingying Ma,Yonggang Wang
Transition-metal containing halides with Ruddlesden-Popper (RP) perovskite structures have received extensive attention owing to their emerging and anisotropic photoelectric functionalities. Among them, A 2 Cu X 4 ( A =alkali metal or organic cations, X =Cl, Br, I) series are particular, because of the Jahn-Teller distortion of Cu 2+ sensitive to external stimuli such as temperature and pressure. In this article, we report the structure evolution and physical property responses of RP perovskites Rb 2 CuCl 4- x Br x ( x =1, 2) to external pressure. Dramatic structural phase transitions from orthorhombic to monoclinic occur around 3.0 GPa in both materials regardless of their distinct compositions. Structure analyses reveal the suppression and final vanishing of the Jahn-Teller distortion of Cu 2+ cations under compression and crossing the phase transition, respectively. Rb 2 CuCl 4- x Br x perovskites exhibit abrupt bandgap narrowing (from reddish-brown to black) along with the structural phase transition, and an overall bandgap narrowing of 75% up to ∼27 GPa but still keeping semiconductive. During the compression processes, the resistances of Rb 2 CuCl 4- x Br x have been greatly reduced by 5-orders of magnitude. Moreover, all of the pressure-induced phenomena in Rb 2 CuCl 4- x Br x perovskites are reversible upon decompression and no obvious difference is observed for the pressure responses between [CuCl 4 Br 2 ] and [CuCl 4 (Cl,Br) 2 ] coordination environments. The impact of pressure on the structural and physical properties in two-dimensional Rb 2 CuCl 4- x Br x provides in-depth understanding on the structure design of functional halide perovskites at ambient conditions.
研究领域:
材料科学
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凝聚态物理
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无机化学
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高压研究
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光电子学
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DOI
高影响因子
CERAMICS INTERNATIONAL
·
2026
·
IF 5.6
Jiahui Zhu,Huifang Gong,Jiaqi Zhu,Xiaofei Zhu,Shangyu Li,Defeng Zhou,Jinghe Bai
Ruddlesden-Popper phase perovskites, a class of traditional SOFC cathode materials, are limited by inadequate ORR activity under intermediate temperatures. This research proposes fabricating composite cathodes by blending La 2 Ni 0.9 Sc 0.1 O 4+δ (LNSO) with Pr 6 O 11 (PO), which is a promising oxygen catalyst, at varying concentrations.The impacts of composite electrodes on the material’s thermal stability, electrochemical performance, and structural properties were explored using XRD, FE-SEM, and an electrochemical workstation. Experimental results demonstrate that 30% PO content notably boosts the surface oxygen content of the cathode material and improves its ORR catalytic activity. Relaxation time distribution results indicate that LNSO-30PO speeds up the oxygen adsorption and dissociation processes. At 700 °C, the symmetric cell with LNSO-30PO as the electrode exhibits a polarization resistance as low as 0.063 Ω·cm 2 , representing a 51.5% decrease relative to pure LNSO. When integrated into a single-cell SOFC as the cathode, LNSO-30PO enables the device to reach a PPD of 0.96 W cm -2 (1.28 times that of the LNSO-based counterpart) while maintaining excellent long-term stability. These findings suggest that LNSO-30PO is a viable candidate for IT-SOFC cathodes.
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高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Keke Hou,Chenjie Lou,Mingxue Tang,Hujun Cao,Laijun Liu,Jungu Xu
Ruddlesden–Popper (RP)-structured materials based on transition metals with a variable valence, such as Fe, Mn, Ni, and so on, have been well documented for their potential of being used as electrodes in solid-oxide fuel cells. However, RP materials with pure or dominant ionic conduction are rare. Here, a series of Zr-based RP materials Sr3Zr2–xMxO7–0.5x (M = Ga, Y, In) with electrical conductivity as high as 3.25 × 10–3 S cm–1 at 900 °C in air was reported, which represents the highest conductivity for the Zr-based RP materials and is comparable to that of the recently reported In-based RP oxide-ion conductors, such as NdBaInO4-based and La2BaIn2O7-based materials. Under low oxygen partial pressure (pO2), the doped samples show pure ionic conducting behaviors without n-type electronic conductivity. The defect formation energies, local structure around the oxygen vacancies, and oxide-ion-conducting mechanism of the acceptor-doped Sr3Zr2O7-based materials were studied for the first time. The results revealed a two-dimensional oxide ion migration characteristic within the perovskite slabs. This work therefore provides a good reference for developing new oxide-ion conductors in the Zr-based RP-structured materials.
研究领域:
材料科学
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固体离子学
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能源材料
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陶瓷材料
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燃料电池
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DOI
高影响因子
Solar RRL
·
2021
·Vol. 5
·期 10
·2100495
·
IF 8.582
Chang Liu,Rui Liu,Zhuoneng Bi,Yue Yu,Gang Xu,Hongming Hou,Qiaofeng Wu,Hua Yu,Xueqing Xu
2D Ruddlesden–Popper (2DRP) perovskites with hydrophobic bulky cations are proven to improve the environmental stability in photovoltaic devices significantly. However, these spacer cations lead to a weak interplay in the 2DRP perovskites, severely impacting the charge carrier transport and require a systematic understanding of the interaction between spacer cations and inorganic slabs. Herein, a series of novel perovskites (BA 1− x NMA x ) 2 MA 3 Pb 4 I 13 (NMA = 1-naphthalenemethylammonium, BA = n -butylammonium) are successfully fabricated to reveal the interaction of mixed spacers and inorganic slabs. Incorporating NMA cations enhances the N H⋯I − hydrogen-bonding interaction between the spacer cations and [PbI 6 ] 4− slabs, resulting in a preferentially crystal vertical orientation of smoothed perovskite films with larger crystal grains. Thus, a significant reduction in the density of trap states of the resulting 2DRP perovskites is achieved which leads to highly efficient charge carrier transport. Consequently, the champion (BA 0.9 NMA 0.1 ) 2 MA 3 Pb 4 I 13 device yields a power conversion efficiency (PCE) of 14.21%, along with the unencapsulated devices that can retain 85% of their initial PCE for 1200 h under 35–65% relative humidity conditions. This work provides a simple and original method to modulate the interlayer interplay in 2DRP perovskites for highly efficient and air-stable perovskite solar cells.
研究领域:
材料科学
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光伏技术
·
化学
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DOI
高影响因子
Energy & Environmental Materials
·
2024
·Vol. 7
·期 5
·e12717
·
IF 13
Dongliang Liu,Hang Shang,Chuan Zhou,Jie Miao,Daxiang Xue,Zeping Chen,Meijuan Fei,Fengli Liang,Qiang Niu,Ran Ran,Wei Zhou,Zongping Shao
Solid oxide electrolysis cells (SOECs), displaying high current density and energy efficiency, have been proven to be an effective technique to electrochemically reduce CO 2 into CO. However, the insufficiency of cathode activity and stability is a tricky problem to be addressed for SOECs. Hence, it is urgent to develop suitable cathode materials with excellent catalytic activity and stability for further practical application of SOECs. Herein, a reduced perovskite oxide, Pr 0.35 Sr 0.6 Fe 0.7 Cu 0.2 Mo 0.1 O 3-δ (PSFCM0.35), is developed as SOECs cathode to electrolyze CO 2 . After reduction in 10% H 2 /Ar, Cu and Fe nanoparticles are exsolved from the PSFCM0.35 lattice, resulting in a phase transformation from cubic perovskite to Ruddlesden–Popper (RP) perovskite with more oxygen vacancies. The exsolved metal nanoparticles are tightly attached to the perovskite substrate and afford more active sites to accelerate CO 2 adsorption and dissociation on the cathode surface. The significantly strengthened CO 2 adsorption capacity obtained after reduction is demonstrated by in situ Fourier transform-infrared (FT-IR) spectra. Symmetric cells with the reduced PSFCM0.35 (R-PSFCM0.35) electrode exhibit a low polarization resistance of 0.43 Ω cm 2 at 850 °C. Single electrolysis cells with the R-PSFCM0.35 cathode display an outstanding current density of 2947 mA cm −2 at 850 °C and 1.6 V. In addition, the catalytic stability of the R-PSFCM0.35 cathode is also proved by operating at 800 °C with an applied constant current density of 600 mA cm −2 for 100 h.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
JOURNAL OF PHYSICS D-APPLIED PHYSICS
·
2022
·Vol. 55
·期 35
·354004
·
IF 3.409
Chun-Liang Zhou,Wen-Bo Ma,Zhen-Long Zhang,Yan-Li Mao
The anti-solvent method is one of the main methods used to prepare two-dimensional (2D) Ruddlesden–Popper (RP)-phase perovskite (PVK) films. To investigate the effect of anti-solvent type on the performance of solar cells based on RP-phase PVK films, three kinds of solvents, toluene (TL), ethyl acetate (EA) and chlorobenzene (CB), were used to prepare 2D RP-phase PVK of GA2MA4Pb5I16. The results display that solar cells based on a 2D PVK layer formed with CB present better performance than those with TL and EA. The results of several investigations show that PVK films formed with CB present lower trap density, longer lifetime, no pinholes and smoother surfaces compared with those formed with TL and EA. This demonstrates that CB is the optimal anti-solvent for the preparation of 2D RP PVK solar cells.
研究领域:
材料科学
·
能源科学
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DOI
高影响因子
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