ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Guofeng You,Kunpeng Du,Yiran Zheng,Hongkai Chen,Yibo Xu,Weifei Fu,Hongzheng Chen
Interfacial defects remain a major bottleneck to simultaneously achieve high efficiency and long-term stability in inverted perovskite solar cells (PVSCs). While recent studies have highlighted the importance of the orientation of passivators at the perovskite surface, the systematic control and quantification of orientation preference have received far less attention. Here, we present an orientation-tuned molecular design strategy using piperazinium derivatives in which substituent engineering modulates steric hindrance to favor face-on alignment at the perovskite surface. Among the series, N-formylpiperazinium iodide (NFPI) exhibits the strongest face-on preference, enabling dual-site anchoring to undercoordinated Pb2+ and FA+ vacancies. Density functional theory and spectroscopy confirm that NFPI delivers the highest binding energy, reduced trap density, prolonged carrier lifetimes, and enhanced interfacial band bending. Consequently, NFPI-passivated PVSCs achieve a champion power conversion efficiency (PCE) of 25.82% with a high open-circuit voltage of 1.182 V and minimal hysteresis. Moreover, devices retain 90% of the initial PCE after 1500 h of thermal aging at 65 °C (ISOS-D-2), and encapsulated devices reach a T80 of 477 h under continuous operation (ISOS-L-1). This work establishes adsorption orientation control as a key design principle for efficient and durable PVSCs.
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Kaiyu Wang,Xiuhong Sun,Cheng Peng,Qiangqiang Zhao,Bingqian Zhang,Tianci Wu,Xiaoxu Zhang,Shenglai Wang,Xiao Wang,Shuping Pang
While 2D/3D heterostructures are widely employed to improve the stability of perovskite optoelectronic devices, their effectiveness is fundamentally governed by the crystallinity of the interfacial structure—a factor often overlooked. Disordered interfaces exhibit thermodynamic metastability, where ion diffusion induces sequential phase transitions from low-n to high-n phases. Here, we construct atomically ordered 2D/3D interfaces using phase-pure 2D perovskite capping layers, which reduce the interfacial phase transition rate by 95% and effectively suppress ion migration. As a result, devices exhibit outstanding operational stability, retaining over 99% of their initial power conversion efficiency after 1500 h of continuous operation, along with excellent thermal durability at 85 °C. These findings identify interfacial order as a critical parameter for regulating ion dynamics and phase behavior, providing a robust design principle for achieving high-efficiency, long-lifetime perovskite technologies.
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ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Xin Song,Lijie Wang,Jiayi Wang,Yafeng Xu,Renqian Zhou,Shulin Chen,Partha Maity,Peng Yuan,Yongcao Zhang,Bingyao Shao,Jian-Xin Wang,Jun Yin,Ren-Wu Huang,Youyou Yuan,Taimoor Ahmad,Osman M. Bakr,Omar F. Mohammed
Traditional 0D Bi-based perovskites suffer from inherently poor charge transport, limiting their application in X-ray detection. Here, we report a molecularly engineered 0D compound, Dpy 3 Bi 2 I 12 , featuring conjugated dipyridine cations at the A-site that enhance hydrogen bonding within [BiI 6 ] 3− octahedra and promote the formation of a quasi-2D framework. Compared to conventional MA 3 Bi 2 I 9 , this design shifts the Fermi level closer to the conduction band (CB), enabling more efficient electron injection, as evidenced by ultrafast transient absorption spectroscopy and partial density of states calculations that reveal efficient carrier generation and delocalization between iodide octahedra and conjugated ligands, thereby overcoming the intrinsic confinement of 0D lattices. As a result, Dpy 3 Bi 2 I 12 achieves an ultralow detection limit of 4.4 nGy s −1 , a high sensitivity of 10,600µC·Gy −1 cm −2 at a low operating bias of −5 V·mm −1 . These findings demonstrate an effective strategy for unlocking efficient charge transport in 0D perovskites, advancing their prospects for low-dose, high-resolution X-ray imaging.
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Nanoscale
·
2026
·
IF 5.1
Haoqiu Ding,Zhanpo Han,Hang Li,Chang Shu,Jiahao Lu,Yue Gao,Xin Ming,Kaiwen Li,Yiwei Zhang,Dan Chang,Chao Gao,Zheng Li,Senping Liu,Zhen Xu
The rapid advancement of wearable healthcare monitoring and athletic performance tracking devices has intensified the demand for high-conductivity flexible sensors with high sensing performance. Despite their excellent electrical conductivity, graphene fibers exhibit limited flexibility, constraining their applications in flexible sensors. Here, we produced ultrafine graphene nanofibers via electrospinning of nano-sized graphene oxide sheets, significantly improving the flexibility of graphene fibers and corresponding non-woven fabrics. With a diameter of 66 nm, which is two orders of magnitude thinner than common graphene fibers, the non-woven fabrics made of randomly distributed graphene nanofibers exhibited exceptional flexibility,obtaining the sensors with bending flexibility, wide strain range, low detection limit and good cycling stability. By capturing resistance signals from sensors located at the throat, finger joints, knees, and other sites, we achieved effective word recognition and human motion monitoring. This work establishes a method for fabricating ultrafine fibers from two-dimensional materials, greatly advancing the development of wearable devices
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ACS Photonics
·
2026
·
IF 6.7
Yan Yang,Haiqiang Huang,Lei Liu,Qiuhong Tan,Yifei Huang,Lujun Yang,Hui Zhang,Xuejin Zhang,Feng Song,Yingkai Liu
Two-dimensional (2D) Ruddlesden–Popper perovskite phenylethylammonium lead iodide ((PEA)2PbI4) possesses potential photoelectronic properties and is considered to be an ideal material for photodetectors. However, single devices commonly suffer from low responsivity, slow response speed, and narrow detection range, which hinder their applications in imaging, communications, and artificial intelligence (AI). In this work, high-quality 2D (PEA)2PbI4 tetragons (TTs) were synthesized via a unique liquid–air interface floating method and integrated with cadmium selenide (CdSe) nanobelts (NBs) to construct a novel hybrid heterojunction photodetector. It confirms that the formation of type-II band alignment at the heterointerface enables efficient interfacial charge transfer. Notably, the (PEA)2PbI4/CdSe heterojunction hybrid device exhibits exceptional performance under 450 and 682 nm monochromatic illumination: extremely high responsivity (R) (2.80 × 103 and 6.39 × 103 A/W), excellent detectivity (D*) (4.09 × 1013 and 9.32 × 1013 Jones), large external quantum efficiency (EQE) (7.74 × 105% and 1.16 × 106%), and remarkable Ion/Ioff ratio (3.60 × 105 and 8.66 × 105), as well as fast response speeds (rise/decay time: 108/265 μs and 86/196 μs). Furthermore, the hybrid device overcomes the intrinsic bandgap limitation of (PEA)2PbI4, extending its photoresponse to cover nearly the entire visible spectrum and demonstrating reliable imaging capability. This study provides an innovative strategy for developing high-performance photodetectors with significant practical application potential.
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CHEMISTRY OF MATERIALS
·
2026
·
IF 7
Fuwei Shang,Youkui Xu,Feifei Chai,Xiushan Wang,Xingxuan Zuo,Mengge Zhao,Lin Zheng,ZhenHua Li,Zhun Yao
Two-dimensional (2D) CsPbI3 perovskite shows excellent prospects in the optoelectronics field, attributed to the superior phase stability compared to its 3D counterpart. However, it inherently faces quantum and dielectric confinement effects of the insulating bulky organic cations, leading to poor carrier transport kinetics. Here, we developed diamine cations [OEA, 2,2-oxybis(ethylamine)] and [EDBE, 2,2-(ethylenedioxy)bis(ethylamine)] with extended C–O chains for 2D Dion–Jacobson (DJ) CsPbI3 perovskites, aiming to avoid the undesirable charge tunneling barrier across the organic interlayer. Detailed characterization reveals that EDBE eliminates electron adsorption during interlayer transport, optimizing band alignment and enhancing the Pb-s orbital contribution at the valence band maximum (VBM), which leads to improved carrier lifetime. Through strategic molecular design, the extended dual-functional groups in EDBE strengthen hydrogen bonding and reduce interlayer distance, resulting in compact films with an enhanced carrier lifetime. More importantly, the EDBE spacer induces perovskite crystalline growth with a preferred vertical orientation and forms a multiphase distribution to facilitate carrier transport. Owing to these advantages, the optimized 2D DJ EDBECs4Pb5I16 solar cells deliver a champion power conversion efficiency (PCE) of up to 11.21%. Importantly, the devices exhibit exceptional stability, retaining 90% of their initial PCE after 720 h at 85 °C. It is believed that extended C–O chain engineering paves an effective route for solving carrier transport problems in 2D CsPbI3.
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
·
2026
·
IF 8.2
Feng Li,ZeZhou He,JiaHao Li,SiChao Zhang,Jun Xia,Liu Wang,HengAn Wu,YinBo Zhu
Layered graphene oxide (GO) films are promising structural materials, but their strength and ductility are limited by weak, porous interfaces that lose load transfer during interlayer sliding. Here we report a nacre-like reduced graphene oxide/melamine (rGO/Mel) film coupling dense lamellar stacking with strong, constrained yet dynamically reconfigurable noncovalent interactions. Melamine is introduced between GO sheets and retained after hydroiodic acid reduction, while the reduced sheets form flatter, more compact stacks with smaller interlayer spacing. Melamine’s triazine rings interact with graphitic domains through π–π stacking, and its amine groups form reversible hydrogen bonds with residual oxygen-containing groups, sustaining shear transfer while allowing controlled sliding. Under tensile loading, rGO/Mel exhibits pronounced post-yield strain hardening associated with nanosheet straightening, interfacial reorientation and continued molecular bridging. The optimized film reaches a tensile strength of 262.7 MPa, a strain at break of 5.0 % and a toughness of 6.0 MJ m⁻ 3 . These values represent increases of 538 %, 317 % and 2900 % over pure GO, respectively. Molecular dynamics simulations support this picture by showing more stable interlayer contact and melamine-assisted shear transfer in rGO/Mel. This work shows that constrained noncovalent interfaces can turn interlayer sliding from a failure pathway into a source of strain hardening in layered nanocomposites.
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Materials
·
2026
·Vol. 19
·期 14
·3038
·
IF 3.7
Xiaoting Liu,Jingjing Liu,Caiting Ji,Yanan Qiao,Chunqing Hou,Xiaoxu Bo
HighlightsDiiodine-induced host-guest assembly drives a 1D-to-0D evolution in antimony(III) halides.This structural transformation narrows the optical bandgap to an optimal 1.46 eV, approaching the Shockley-Queisser limit.Strong sp-orbital hybridization ensures robust visible-light harvesting, with absorption coefficients exceeding 104cm−1.The resulting 0D complex exhibits high intrinsic thermal stability and remains structurally intact after a 6-month ambient exposure.Developing lead-free organic-inorganic hybrid metal halides with strong light-harvesting capabilities and superior stability, while precisely tuning their crystalline phases and electronic structures, remains a key challenge in optoelectronics. Herein, we report a neutral iodine-induced structural transition from a 1D chain-like (C6H11NH3)2SbI5architecture to a 0D dimeric (C6H11NH3)3[Sb2I9]·I2supramolecular host-guest complex. This transformation is achieved via a controlled solution-cooling crystallization process, yielding high-quality bulk single crystals. Crystallographic analysis reveals that N–H···I hydrogen-bonding networks stabilize the organic cations, while halogen bonding interactions anchor the I2guests within the lattice cavities of the [Sb2I9]3−dimeric host. Experimental characterizations, including XRD, TGA, and XPS, confirm the high phase purity and thermal stability of the (C6H11NH3)3[Sb2I9]·I2hybrid and determine its electronic band structure. To further elucidate the underlying mechanisms, theoretical calculations were performed, revealing that strong sp-orbital hybridization yields a high absorption coefficient. The associated dimensional transition narrows the direct optical bandgap to 1.46 eV, approaching the Shockley-Queisser limit and demonstrating strong potential for visible-light harvesting. This work elucidates the role of supramolecular host-guest interactions in modulating the lattice evolution of lead-free antimony-based materials, presenting halogen guest engineering as an effective approach for optoelectronic material design.
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Energy & Environmental Materials
·
2026
·
IF 13.8
Yifan Shen,Yanfeng Chen,Quan Chen,Jinyu Wu,Jian Yang,Erdong Zhang,Wei Wang,Ningyi Xu,Wei Shen,Junmin Xia,Shufen Chen,Wei Huang
The advancement of quasi-two-dimensional (quasi-2D) tin-based perovskite solar cells (TPSCs) is severely hampered by challenges including Sn 2+ oxidation, rapid crystallization, and uncontrollable phase distribution. Currently, no one effective approach has been developed to address all these issues simultaneously. Herein, a facile strategy is proposed involving organic spacers that resolves all three problems at once. On the one hand, the introduction of H + suppresses the conversion of Sn 2+ to Sn 4+ in precursor solutions. On the other hand, leveraging the in situ generation and decomposition of DMASnI 3 within the precursor delays the crystallization of quasi-2D tin-based perovskite. Concurrently, the regulation of the crystallization process helps to form the more uniform distribution of quasi-2D phases, significantly improving carrier mobility. The optimized Dion-Jacobson type (DJ) TPSC achieves a champion power conversion efficiency (PCE) of 7.39%, winning a new record, while demonstrating exceptional stability. The successful implementation of this strategy in both quasi-2D Ruddlesden-Popper (RP) and DJ TPSCs demonstrates its universal applicability for enhancing performance across low-dimensional optoelectronic devices.
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Advanced Optical Materials
·
2026
·Vol. 14
·期 13
·e71145
·
IF 7.2
Binbin Su,Chenning Sun,Jiahui Wei,Zhichao Chang,Yayun Zhou,Guojun Zhou,Huidong Xie,Zhiguo Xia
The development of high-performance scintillators is crucial for advancing radiation detection and X-ray imaging technologies. Herein, we report the rational design and synthesis of a 0D hybrid copper iodide scintillator (CyclamH 4 )Cu 2 I 6 , which exhibits intense radioluminescence centered at 450 nm. This blue emission demonstrates excellent spectral match with the peak photon detection efficiency of modern silicon photomultipliers, thereby facilitating efficient photodetection. The (CyclamH 4 )Cu 2 I 6 scintillator achieves a high light yield of 42 720 photons/MeV, a detection limit of 83.5 nGy air s −1 , and notable radiation resistance stability. Accordingly, the inch-size flexible (CyclamH 4 )Cu 2 I 6 @PDMS scintillator film achieves superior performance in X-ray imaging, as evidenced by a high spatial resolution of 13.6 lp/mm. This work validates copper halides as a tunable platform for the design of scintillators, thereby opening new avenues for the innovation of X-ray imaging technology.
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Matter
·
2026
·
IF 15.7
Yu-Chuang Fang,Yu-Hua Huang,Wei Wei,Su-Yan Zou,Cong-Yi Sheng,Xu-Dong Wang,Dai-Bin Kuang
Large-area halide perovskite thick films offer significant potential for next-generation X-ray detectors. However, bias-induced ion migration at buried interfaces significantly degrades device performance. Here, we introduce an innovative buried interface engineering strategy by incorporating a low-polarity solution (ethyl acetate)-processable 1D perovskite (PBL 4 PbI 6 , PBL = pregabalin) as bottom contact layer, which simultaneously addresses three critical issues: (1) low-polarity ethyl acetate eliminates solvent residue, improving device repeatability and stability; (2) low lattice mismatch (≈1.3%) of underlying 1D layer enables high-quality crystalline growth of top 3D layer; (3) a built-in reverse electric field at 1D/3D heterostructure, enables efficient carrier extraction, while suppressing excessive field-induced ion migration. As a result, ion migration activation energy increases from 149 to 182 meV. The optimized detectors achieve a high sensitivity of 76,553 μC Gy air −1 cm −2 and a low detection limit of 9.5 nGy air s −1 , outperforming most reported perovskite thick-film X-ray detectors based on interface engineering.
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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 33
·45388-45398
·
IF 7.8
Su Ju-Wen,Wang Xing-Qi,Zhu Bo-Yuan,Yang Wei-Wei,Qu Zhi-Guo,Tao Yu-Bing
High-power operation of vanadium redox flow batteries (VRFBs) is still limited by sluggish interfacial charge transfer, insufficient electrolyte wettability, and concentration polarization within porous carbon electrodes. Herein, an iodine-functionalized reduced graphene oxide/graphite felt electrode (GF@rGO-V) was prepared through hydroiodic acid vapor treatment to regulate the solid–liquid interface of graphite felt while retaining its three-dimensional porous framework. Structural and surface analyses indicate that HI vapor treatment produces a less compact iodine-containing rGO interface with improved electrolyte accessibility. Electrochemical measurements further reveal enhanced apparent ion transport and reduced charge-transfer resistance toward both VO 2+ /VO 2 + and V 2+ /V 3+ redox couples. Temperature-dependent impedance analysis shows that the apparent activation energy for the positive reaction decreases from 40.2 kJ mol –1 on pristine graphite felt to 23.7 kJ mol –1 on GF@rGO-V, suggesting a more favorable interfacial kinetic environment. As a result, the assembled VRFB delivers an energy efficiency of 82.2% at 400 mA cm –2 , a peak power density of 1257.6 mW cm –2 , and stable cycling over 1500 cycles at 400 mA cm –2 . This work demonstrates an iodine-assisted interfacial engineering strategy for improving mass transport and charge-transfer kinetics in high-power aqueous flow batteries.
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