Buried‐Interface Engineering Enables Efficient and 1960‐Hour ISOS‐L‐2I Stable Inverted Perovskite Solar Cells

Advanced Materials

Published On 2024/3

High‐performance perovskite solar cells (PSCs) typically require interfacial passivation, yet this is challenging for the buried interface, owing to the dissolution of passivation agents during the deposition of perovskites. Here, this limitation is overcome with in situ buried‐interface passivation—achieved via directly adding a cyanoacrylic‐acid‐based molecular additive, namely BT‐T, into the perovskite precursor solution. Classical and ab initio molecular dynamics simulations reveal that BT‐T spontaneously may self‐assemble at the buried interface during the formation of the perovskite layer on a nickel oxide hole‐transporting layer. The preferential buried‐interface passivation results in facilitated hole transfer and suppressed charge recombination. In addition, residual BT‐T molecules in the perovskite layer enhance its stability and homogeneity. A power‐conversion efficiency (PCE) of 23.48% for 1.0 cm2 inverted …

Journal

Advanced Materials

Published On

2024/3

Volume

36

Issue

13

Page

2303869

Authors

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Position

Professor

H-Index(all)

299

H-Index(since 2020)

170

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Solar energy conversion

Yaoguang Rong

Yaoguang Rong

Huazhong University of Science and Technology

Position

H-Index(all)

48

H-Index(since 2020)

43

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Photovoltaics

perovskite solar cells

nano-materials

Felix Thomas Eickemeyer

Felix Thomas Eickemeyer

École Polytechnique Fédérale de Lausanne

Position

Senior scientist (EPFL)

H-Index(all)

35

H-Index(since 2020)

29

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Ursula Rothlisberger

Ursula Rothlisberger

École Polytechnique Fédérale de Lausanne

Position

EPFL Switzerland

H-Index(all)

31

H-Index(since 2020)

13

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Nikolaos Lempesis

Nikolaos Lempesis

École Polytechnique Fédérale de Lausanne

Position

Research Associate @

H-Index(all)

12

H-Index(since 2020)

7

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Chemical Engineering

Materials Science

Molecular Simulation

Physical Chemistry

Lorenzo Agosta

Lorenzo Agosta

Stockholms universitet

Position

H-Index(all)

9

H-Index(since 2020)

8

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

University Profile Page

Virginia Carnevali

Virginia Carnevali

Central Michigan University

Position

Postdoctoral fellow

H-Index(all)

8

H-Index(since 2020)

8

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Material science

Photovoltaics

Graphene

Thermoelectrics

University Profile Page

Other Articles from authors

Virginia Carnevali

Virginia Carnevali

Central Michigan University

Journal of the American Chemical Society

Three-Fold Coordination of Copper in Sulfides: A Blockade for Hole Carrier Delocalization but a Driving Force for Ultralow Thermal Conductivity

Copper-rich sulfides are very promising for energy conversion applications due to their environmental compatibility, cost effectiveness, and earth abundance. Based on a comparative analysis of the structural and transport properties of Cu3BiS3 with those of tetrahedrite (Cu12Sb4S13) and other Cu-rich sulfides, we highlight the role of the cationic coordination types and networks on the electrical and thermal properties. By precession-assisted 3D electron diffraction analysis, we find very high anisotropic thermal vibration of copper attributed to its 3-fold coordination, with an anisotropic atomic displacement parameter up to 0.09 Å2. Density functional theory calculations reveal that these Cu atoms are weakly bonded and give rise to low-energy Einstein-like vibrational modes that strongly scatter heat-carrying acoustic phonons, leading to ultralow thermal conductivity. Importantly, we demonstrate that the 3-fold …

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Nature

High carrier mobility along the [111] orientation in Cu2O photoelectrodes

Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight,. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials, –. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance. Here we demonstrate performance of Cu2O photocathodes beyond the state-of-the-art by exploiting a new conceptual understanding of carrier recombination and transport in single-crystal Cu2O thin films. Using ambient liquid-phase epitaxy, we present a new method to grow single-crystal Cu2O samples with three crystal orientations. Broadband femtosecond transient reflection spectroscopy measurements were used to quantify anisotropic optoelectronic properties, through which the carrier mobility along the [111 …

Felix Thomas Eickemeyer

Felix Thomas Eickemeyer

École Polytechnique Fédérale de Lausanne

Advanced Functional Materials

Interfacial Modulation through Mixed‐Dimensional Heterostructures for Efficient and Hole Conductor‐Free Perovskite Solar Cells

Perovskite solar cells have led the new surge of solar energy research. However, their instability is a pressing issue mostly attributed to the perovskite interface with charge‐selective transport layers. In this work, diethylammonium iodide (DEAI) surface treatment is used to mitigate interfacial non‐radiative recombination losses by forming a mixed phase of layered perovskite on the surface. This results in enhanced device performance with the power conversion efficiency of 23.3% and improved operational stability under thermal stress. Moreover, the DEAI treatment facilitates interfacial hole transfer, enabling a carbon‐based hole transport layer‐free perovskite solar cell with a power conversion efficiency of 15.6%.

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Advanced Functional Materials

Interfacial Modulation through Mixed‐Dimensional Heterostructures for Efficient and Hole Conductor‐Free Perovskite Solar Cells

Perovskite solar cells have led the new surge of solar energy research. However, their instability is a pressing issue mostly attributed to the perovskite interface with charge‐selective transport layers. In this work, diethylammonium iodide (DEAI) surface treatment is used to mitigate interfacial non‐radiative recombination losses by forming a mixed phase of layered perovskite on the surface. This results in enhanced device performance with the power conversion efficiency of 23.3% and improved operational stability under thermal stress. Moreover, the DEAI treatment facilitates interfacial hole transfer, enabling a carbon‐based hole transport layer‐free perovskite solar cell with a power conversion efficiency of 15.6%.

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Advanced Materials

Durable Perovskite Solar Cells with 24.5% Average Efficiency: the Role of Rigid Conjugated Core in Molecular Semiconductors

Efficient and robust n‐i‐p perovskite solar cells necessitate superior organic hole‐transport materials with both mechanical and electronic prowess. Deciphering the structure−property relationship of these materials is crucial for practical perovskite solar cell applications. Through direct arylation, we synthesized two high glass transition temperature molecular semiconductors, DBC‐ETPA (202 °C) and TPE‐ETPA (180 °C), using dibenzo[g,p]chrysene (DBC) and 1,1,2,2‐tetraphenylethene (TPE) tetrabromides with triphenylene–ethylenedioxythiophene‐dimethoxytriphenylamine (ETPA). In comparison to spiro‐OMeTAD, both semiconductors exhibit shallower HOMO energy levels, resulting in increased hole densities (generated by air oxidation doping) and accelerated hole extraction from photoexcited perovskite. Experimental and theoretical studies highlight the more rigid DBC core, enhancing hole mobility due to …

Felix Thomas Eickemeyer

Felix Thomas Eickemeyer

École Polytechnique Fédérale de Lausanne

Advanced Materials

Indoor Self‐Powered Perovskite Optoelectronics with Ultraflexible Monochromatic Light Source

Self‐powered skin optoelectronics fabricated on ultrathin polymer films is emerging as one of the most promising components for the next‐generation Internet of Things (IoT) technology. However, a longstanding challenge is the device underperformance owing to the low process temperature of polymer substrates. In addition, broadband electroluminescence (EL) based on organic or polymer semiconductors inevitably suffers from periodic spectral distortion due to Fabry–Pérot (FP) interference upon substrate bending, preventing advanced applications. Here, ultraflexible skin optoelectronics integrating high‐performance solar cells and monochromatic light‐emitting diodes using solution‐processed perovskite semiconductors is presented. n–i–p perovskite solar cells and perovskite nanocrystal light‐emitting diodes (PNC‐LEDs), with power‐conversion and current efficiencies of 18.2% and 15.2 cd A−1 …

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Scientific Reports

Infrared-reflective ultrathin-metal-film-based transparent electrode with ultralow optical loss for high efficiency in solar cells

In this work we study in-depth the antireflection and filtering properties of ultrathin-metal-film-based transparent electrodes (MTEs) integrated in thin-film solar cells. Based on numerical optimization of the MTE design and the experimental characterization of thin-film perovskite solar cell (PSC) samples, we show that reflection in the visible spectrum can be strongly suppressed, in contrast to common belief (due to the compact metal layer). The optical loss of the optimized electrode (~ 2.9%), composed of a low-resistivity metal and an insulator, is significantly lower than that of a conventional transparent conductive oxide (TCO ~ 6.3%), thanks to the very high transmission of visible light within the cell (> 91%) and low thickness (< 70 nm), whereas the reflection of infrared light (~ 70%) improves by > 370%. To assess the application potentials, integrated current density > 25 mA/cm2, power conversion …

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Joule

Photo-doping of spiro-OMeTAD for highly stable and efficient perovskite solar cells

A widely used component of high-efficiency perovskite solar cells (PSCs) is the molecular hole-transport material (HTM) spiro-OMeTAD. This organic solid needs to be p-doped to acquire sufficient hole conductivity. However, the conventional doping method using LiTFSI in the air is slow, sensitive to the environment, and may lead to the deterioration of the PSCs by unintended oxidation or dopant migration. It is thus highly desirable to develop fast doping approaches that avoid exposing the PSC to ambient air and easy-to-move dopant ions. We report here that light absorption by spiro-OMeTAD itself triggers redox photochemistry that has so far been ignored. Strikingly, we found that Y(III) or La(III)-tBP complexes catalyze the symmetry-breaking charge separation of photo-excited spiro-OMeTAD, resulting in the efficient p-doping of the HTM. Using this photo-redox process, we realize PSCs with superior stability over …

Felix Thomas Eickemeyer

Felix Thomas Eickemeyer

École Polytechnique Fédérale de Lausanne

Advanced Materials

Durable Perovskite Solar Cells with 24.5% Average Efficiency: the Role of Rigid Conjugated Core in Molecular Semiconductors

Efficient and robust n‐i‐p perovskite solar cells necessitate superior organic hole‐transport materials with both mechanical and electronic prowess. Deciphering the structure−property relationship of these materials is crucial for practical perovskite solar cell applications. Through direct arylation, we synthesized two high glass transition temperature molecular semiconductors, DBC‐ETPA (202 °C) and TPE‐ETPA (180 °C), using dibenzo[g,p]chrysene (DBC) and 1,1,2,2‐tetraphenylethene (TPE) tetrabromides with triphenylene–ethylenedioxythiophene‐dimethoxytriphenylamine (ETPA). In comparison to spiro‐OMeTAD, both semiconductors exhibit shallower HOMO energy levels, resulting in increased hole densities (generated by air oxidation doping) and accelerated hole extraction from photoexcited perovskite. Experimental and theoretical studies highlight the more rigid DBC core, enhancing hole mobility due to …

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Advanced Materials Interfaces

Modulation of Ionically Generated Space Charge Effects at Hybrid Perovskite and Oxide Interfaces via Surface Modification

Interfacial space charges significantly influence transport and recombination of charge carriers in optoelectronic devices. Due to the mixed ionic‐electronic conducting properties of halide perovskites, not only electronic effects, but also ionic interactions at their interfaces need to be considered in the analysis of space charges. Understanding of these interactions and their control is currently missing. This study elucidates the ionic effects on space charge formation at the interface between methylammonium lead iodide (MAPI) and alumina, and its modulation through surface modification using organic molecules. Embedding insulating alumina nanoparticles within MAPI films leads to enhancement of the electronic conductivity. This effect is consistent with the formation of an interfacial inversion layer in MAPI and can only be explained on the basis of ionic interactions. Such an effect is attenuated by surface …

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Research data supporting" High carrier mobility along the [111] orientation in Cu2O photoelectrodes"

Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance. Here we demonstrate performance of Cu2O photocathodes beyond the state-of-the-art by exploiting a new conceptual understanding of carrier recombination and transport in single-crystal Cu2O thin films. Using ambient liquid-phase epitaxy, we present a new method to grow single-crystal Cu2O samples with three crystal orientations. Broadband femtosecond transient reflection spectroscopy measurements were used to quantify anisotropic optoelectronic properties, through which the carrier mobility along the [111] orientation was found to be an order of magnitude higher than those along other orientations. Driven by these findings, we developed a polycrystalline Cu2O photocathode with an extraordinarily pure (111) orientation and (111) terminating facets using a simple and low-cost method, which delivers 7 mA cm− 2 current density (more than 70% improvement compared to that of state-of-the-art electrodeposited devices) at 0.5 V versus a reversible hydrogen electrode under air mass 1.5 G illumination, and stable operation over at least 120 h.

Felix Thomas Eickemeyer

Felix Thomas Eickemeyer

École Polytechnique Fédérale de Lausanne

Energy & Environmental Materials

High‐Performance Perovskite Solar Cells with Zwitterion‐Capped‐ZnO Quantum Dots as Electron Transport Layer and NH4X (X = F, Cl, Br) Assisted Interfacial …

The systematic advances in the power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs) have been driven by the developments of perovskite materials, electron transport layer (ETL) materials, and interfacial passivation between the relevant layers. While zinc oxide (ZnO) is a promising ETL in thin film photovoltaics, it is still highly desirable to develop novel synthetic methods that allow both fine‐tuning the versatility of ZnO nanomaterials and improving the ZnO/perovskite interface. Among various inorganic and organic additives, zwitterions have been effectively utilized to passivate the perovskite films. In this vein, we develop novel, well‐characterized betaine‐coated ZnO QDs and use them as an ETL in the planar n‐i‐p PSC architecture, combining the ZnO QDs‐based ETL with the ZnO/perovskite interface passivation by a series of ammonium halides (NH4X, where X = F, Cl, Br). The …

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Energy & Environmental Science

Understanding and decoupling the role of wavelength and defects in light-induced degradation of metal-halide perovskites

Light-induced degradation in metal halide perovskites is a major concern that can potentially hamper the commercialization of perovskite optoelectronic devices. The phenomena viz. ion migration, phase segregation, and defect intolerance are believed to be the factors behind the degradation. However, a detailed mechanistic understanding of how and why light reduces the long-term stability of perovskites is still lacking. Here, by combining multiscale characterization techniques and computational studies, we uncover the role of white light in the surface degradation of state-of-the-art FAPbI3-rich perovskite absorbers (reaching up to 22% PCE in solar cells). We unravel the degradation kinetics and found that white light triggers the chemical degradation of perovskite into secondary phases with higher work function and metallic I–V characteristics. Furthermore, we demonstrate that perovskite degradation is triggered …

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Energy & Environmental Materials

High‐Performance Perovskite Solar Cells with Zwitterion‐Capped‐ZnO Quantum Dots as Electron Transport Layer and NH4X (X = F, Cl, Br) Assisted Interfacial …

The systematic advances in the power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs) have been driven by the developments of perovskite materials, electron transport layer (ETL) materials, and interfacial passivation between the relevant layers. While zinc oxide (ZnO) is a promising ETL in thin film photovoltaics, it is still highly desirable to develop novel synthetic methods that allow both fine‐tuning the versatility of ZnO nanomaterials and improving the ZnO/perovskite interface. Among various inorganic and organic additives, zwitterions have been effectively utilized to passivate the perovskite films. In this vein, we develop novel, well‐characterized betaine‐coated ZnO QDs and use them as an ETL in the planar n‐i‐p PSC architecture, combining the ZnO QDs‐based ETL with the ZnO/perovskite interface passivation by a series of ammonium halides (NH4X, where X = F, Cl, Br). The …

Other articles from Advanced Materials journal

So Min Park

So Min Park

University of Toronto

Advanced Materials

Sub‐Second Long Lifetime Triplet Exciton Reservoir for Highly Efficient and Stable Organic Light‐Emitting Diode

In organic light‐emitting diode (OLED), achieving high efficiency requires effective triplet exciton confinement by carrier‐transporting materials, which typically have higher triplet energy (ET) than the emitter, leading to poor stability. Here, an electron‐transporting material (ETM), whose ET is 0.32 eV lower than that of the emitter is reported. In devices, it surprisingly exhibits strong confinement effect and generates excellent efficiency. Additionally, the device operational lifetime is 4.9 times longer than the device with a standard ETM, 1,3,5‐tri(1‐phenyl‐1H‐benzo[d]imidazol‐2‐yl) phenyl (whose ET 0.36 eV is higher than the emitter). This anomalous finding is ascribed to the exceptionally long triplet state lifetime (≈0.2 s) of the ETM. It is named as long‐lifetime triplet exciton reservoir effect. The systematic analysis reveals that the long triplet lifetime of ETM can compensate the requirement for high ET with the help of …

Jingrui Li

Jingrui Li

Xi'an Jiaotong University

Advanced Materials

Optimizing the Buried Interface in Flexible Perovskite Solar Cells to Achieve Over 24% Efficiency and Long‐Term Stability

The buried interface of the perovskite layer has a profound influence on its film morphology, defect formation, and aging resistance from the outset, therefore, significantly affects the film quality and device performance of derived perovskite solar cells. Especially for FAPbI3, although it has excellent optoelectronic properties, the spontaneous transition from the black perovskite phase to nonperovskite phase tends to start from the buried interface at the early stage of film formation then further propagate to degrade the whole perovskite. In this work, by introducing ─NH3+ rich proline hydrochloride (PF) with a conjugated rigid structure as a versatile medium for buried interface, it not only provides a solid α‐phase FAPbI3 template, but also prevents the phase transition induced degradation. PF also acts as an effective interfacial stress reliever to enhance both efficiency and stability of flexible solar cells. Consequently, a …

Claudia Robertson

Claudia Robertson

Baylor College of Medicine

Advanced Materials

Oxidized activated charcoal nanozymes: Synthesis, and optimization for in vitro and in vivo bioactivity for traumatic brain injury

Carbon‐based superoxide dismutase (SOD) mimetic nanozymes have recently been employed as promising antioxidant nanotherapeutics due to their distinct properties. The structural features responsible for the efficacy of these nanomaterials as antioxidants are, however, poorly understood. Here, the process–structure–property–performance properties of coconut‐derived oxidized activated charcoal (cOAC) nano‐SOD mimetics are studied by analyzing how modifications to the nanomaterial's synthesis impact the size, as well as the elemental and electrochemical properties of the particles. These properties are then correlated to the in vitro antioxidant bioactivity of poly(ethylene glycol)‐functionalized cOACs (PEG‐cOAC). Chemical oxidative treatment methods that afford smaller, more homogeneous cOAC nanoparticles with higher levels of quinone functionalization show enhanced protection against oxidative …

Xumin Ding

Xumin Ding

Harbin Institute of Technology

Advanced Materials

Metasurface‐Based Optical Logic Operators Driven by Diffractive Neural Networks (Adv. Mater. 9/2024)

In article number 2308993, Xumin Ding, Shah Nawaz Burokur, Guangwei Hu, and co-workers report an optical quantum logic operator with high fidelity. The device is driven by an all-optical diffractive neural network, while combining polarization-and spatial-multiplexing strategies to achieve four classical quantum gates. This work substantially improves the integration and flexibility of quantum computing systems.

q. jiang

q. jiang

Jilin University

Advanced Materials

Lamellar Nanoporous Metal/Intermetallic Compound Heterostructure Regulating Dendrite‐Free Zinc Electrodeposition for Wide‐Temperature Aqueous Zinc‐Ion Battery

Aqueous zinc‐ion batteries are attractive post‐lithium battery technologies for grid‐scale energy storage because of their inherent safety, low cost and high theoretical capacity. However, their practical implementation in wide‐temperature surroundings persistently confronts irregular zinc electrodeposits and parasitic side reactions on metal anode, which leads to poor rechargeability, low Coulombic efficiency and short lifespan. Here, this work reports lamellar nanoporous Cu/Al2Cu heterostructure electrode as a promising anode host material to regulate high‐efficiency and dendrite‐free zinc electrodeposition and stripping for wide‐temperatures aqueous zinc‐ion batteries. In this unique electrode, the interconnective Cu/Al2Cu heterostructure ligaments not only facilitate fast electron transfer but work as highly zincophilic sites for zinc nucleation and deposition by virtue of local galvanic couples while the …

Sung-Hong Park

Sung-Hong Park

KAIST

Advanced Materials

Longitudinal Magnetic Resonance Imaging with ROS‐Responsive Bilirubin Nanoparticles Enables Monitoring of Nonalcoholic Steatohepatitis Progression to Cirrhosis

Despite the vital importance of monitoring the progression of nonalcoholic fatty liver disease (NAFLD) and its progressive form, nonalcoholic steatohepatitis (NASH), an efficient imaging modality that is readily available at hospitals is currently lacking. Here, a new magnetic‐resonance‐imaging (MRI)‐based imaging modality is presented that allows for efficient and longitudinal monitoring of NAFLD and NASH progression. The imaging modality uses manganese‐ion (Mn2+)‐chelated bilirubin nanoparticles (Mn@BRNPs) as a reactive‐oxygen‐species (ROS)‐responsive MRI imaging probe. Longitudinal T1‐weighted MR imaging of NASH model mice is performed after injecting Mn@BRNPs intravenously. The MR signal enhancement in the liver relative to muscle gradually increases up to 8 weeks of NASH progression, but decreases significantly as NASH progresses to the cirrhosis‐like stage at weeks 10 and 12. A …

Myeong Je Jang

Myeong Je Jang

University of Waterloo

Advanced Materials

Longevous Cycling of Rechargeable Zn‐Air Battery Enabled by “Raisin‐Bread” Cobalt Oxynitride/Porous Carbon Hybrid Electrocatalysts

Developing commercially viable electrocatalyst lies at the research hotspot of rechargeable Zn‐air batteries, but it is still challenging to meet the requirements of energy efficiency and durability in realistic applications. Strategic material design is critical to addressing its drawbacks in terms of sluggish kinetics of oxygen reactions and limited battery lifespan. Herein, a “raisin‐bread” architecture is designed for a hybrid catalyst constituting cobalt nitride as the core nanoparticle with thin oxidized coverings, which is further deposited within porous carbon aerogel. Based on synchrotron‐based characterizations, this hybrid provides oxygen vacancies and Co‐Nx‐C sites as the active sites, resulting from a strong coupling between CoOxNy nanoparticles and 3D conductive carbon scaffolds. Compared to the oxide reference, it performs enhanced stability in harsh electrocatalytic environments, highlighting the benefits of the …

Ruiqin ZHANG

Ruiqin ZHANG

City University of Hong Kong

Advanced Materials

Decoupling Activation and Transport by Electron‐Regulated Atomic‐Bi Harnessed Surface‐to‐Pore Interface for Vanadium Redox Flow Battery

In article number 2305415, Xiangyang Zhang, Walid A. Daoud, and co-workers report a surface-to-pore catalytic interface structured electrode that is designed and implemented in vanadium redox flow battery (VRFB), therein lies the concept of decoupling the activation and transport processes. This study addresses a critical challenge in conventional catalyst designs, aiming to substantially upgrade VRFB performance while sustaining remarkable durability for encouraging widespread adoption.

Neil R. Champness

Neil R. Champness

University of Birmingham

Advanced Materials

How reproducible is the synthesis of Zr–porphyrin metal–organic frameworks? An interlaboratory study

Metal–organic frameworks (MOFs) are a rapidly growing class of materials that offer great promise in various applications. However, the synthesis remains challenging: for example, a range of crystal structures can often be accessed from the same building blocks, which complicates the phase selectivity. Likewise, the high sensitivity to slight changes in synthesis conditions may cause reproducibility issues. This is crucial, as it hampers the research and commercialization of affected MOFs. Here, it presents the first‐ever interlaboratory study of the synthetic reproducibility of two Zr–porphyrin MOFs, PCN‐222 and PCN‐224, to investigate the scope of this problem. For PCN‐222, only one sample out of ten was phase pure and of the correct symmetry, while for PCN‐224, three are phase pure, although none of these show the spatial linker order characteristic of PCN‐224. Instead, these samples resemble dPCN‐224 …

Lingling Huang

Lingling Huang

Beijing Institute of Technology

Advanced Materials

Multi‐dimensional Multiplexed Metasurface Holography by Inverse Design

Multi‐dimensional multiplexed metasurface holography extends holographic information capacity, promises revolutionary advancements for vivid imaging, information storage and encryption. However, achieving multifunctional metasurface holography by forward design method is still difficult since it relies heavily on Jones matrix engineering, which places high demands on physical knowledge and processing technology. To break these limitations and simplify the design process, here we propose an end‐to‐end inverse design framework. By directly linking the metasurface to the reconstructed images and employing a loss function to guide the update of metasurface, the calculation of hologram can be omitted, thus greatly simplifying the design process. In addition, the requirements on the completeness of meta‐library can also be significantly reduced, allowing multi‐channel hologram to be achieved using meta …

Lingling Huang

Lingling Huang

Beijing Institute of Technology

Advanced Materials

Meta‐Attention Network based Spectral Reconstruction with Snapshot Near‐Infrared Metasurface

Near‐infrared (NIR) spectral information is important for detecting and analyzing material compositions. However, snapshot NIR spectral imaging systems still pose significant challenges owing to the lack of high‐performance NIR filters and bulky setups, preventing effective encoding and integration with mobile devices. In this study, we introduce a snapshot spectral imaging system that employs a compact NIR metasurface featuring 25 distinct C4 symmetry structures. Benefitting from the sufficient spectral variety and low correlation coefficient among these structures, center‐wavelength accuracy of 0.05 nm and full width at half maximum (FWHM) accuracy of 0.13 nm are realized. The system maintains good performance within an incident angle of 1°. A novel meta‐attention network prior iterative denoising reconstruction (MAN‐IDR) algorithm guided by both meta‐attention and spatial‐spectral attention is …

Bo Zou (邹勃)

Bo Zou (邹勃)

Jilin University

Advanced Materials

Harvesting Multi‐Color Photoluminescence in Non‐Aromatic Interpenetrated Metal‐Organic Framework Nanocrystals via Pressure‐Modulated Carbonyls Aggregation

Interpenetrated metal‐organic frameworks (MOFs) with non‐aromatic ligands provide a unique platform for adsorption, catalysis, and sensing applications. However, non‐emission and the lack of optical property tailoring make it challenging to fabricate smart responsive devices with non‐aromatic interpenetrated MOFs based on ligand‐centered emission. In this paper, we introduce the pressure‐induced aggregation effect in non‐aromatic interpenetrated Zn4O(ADC)4(Et3N)6 (IRMOF‐0) nanocrystals (NCs), where carbonyl groups aggregation results in O‐O distances smaller than the sum of the van der Waals radii (3.04 Å), triggering the photoluminescence turn‐on behavior. It is noteworthy that the IRMOF‐0 NCs display an ultra‐broad emission tunability of 130 nm from deep blue (440 nm) to yellow (570 nm) upon release to ambient conditions at different pressures. The eventual retention of through‐space n‐π …

Lian Duan 段炼

Lian Duan 段炼

Tsinghua University

Advanced Materials

B‐N Covalent Bond Embedded Double Hetero‐[n] helicenes for Pure Red Narrowband Circularly Polarized Electroluminescence with High Efficiency and Stability

Chiral B/N embedded multi‐resonance (MR) emitters open a new paradigm of circularly polarized (CP) organic light‐emitting diodes (OLEDs) owing to their unique narrowband spectra. However, pure‐red CP‐MR emitters and devices remain exclusive in literature. Herein, by introducing a B‐N covalent bond to lower the electron‐withdrawing ability of the para‐positioned B‐π‐B motif, the first pair of pure‐red double hetero‐[n]helicenes (n = 6 and 7) CP‐MR emitter peaking 617 nm with a small full‐width at half‐maximum of 38 nm and a high photoluminescence quantum yield of ≈100% in toluene is developed. The intense mirror‐image CP light produced by the enantiomers is characterized by high photoluminescence dissymmetry factors (gPL) of +1.40/−1.41 × 10−3 from their stable helicenes configuration. The corresponding devices using these enantiomers afford impressive CP electroluminescence …

Lian Duan 段炼

Lian Duan 段炼

Tsinghua University

Advanced Materials

Colour‐Tunable Organic Light‐Emitting Diodes with Single Pt (O^ N^ C^ N)‐dibenzofuran Emitter Exhibiting High External Quantum Efficiency of∼ 30% and Superior Operational Lifetime

Colour‐tunable organic light‐emitting diodes (CT‐OLEDs) have a large colour‐tuning range, high efficiency and operational stability at practical luminance, making them ideal for human‐machine interactive terminals of wearable biomedical devices. However, the device operational lifetime of CT‐OLEDs is currently far from reaching practical requirements. To address this problem, we designed a tetradentate Pt(II) complex named tetra‐Pt‐dbf, which can emit efficiently in both monomer and aggregation states. This emitter has a high Td of 508°C and a large intermolecular bonding energy of ‐52.0 kcal/mol, which improve its thermal/chemical stability. Our unique single‐emitter CT‐OLED essentially avoids the “colour‐ageing issue” and achieves a large colour‐tuning span (red to yellowish green) and a high EQE of ∼30% at 1000 cd m−2 as well as an EQE of above 25% at 10000 cd m−2. We estimated a superior …

JaeHong Park

JaeHong Park

Ewha Womans University

Advanced Materials

Self‐Powering Sensory Device with Multi‐Spectrum Image Realization for Smart Indoor Environments

The development of organic‐based optoelectronic technologies for the indoor Internet of Things market, which relies on ambient energy sources, has increased, with organic photovoltaics (OPVs) and photodetectors (OPDs) considered promising candidates for sustainable indoor electronic devices. However, the manufacturing processes of standalone OPVs and OPDs can be complex and costly, resulting in high production costs and limited scalability, thus limiting their use in a wide range of indoor applications. This study uses a multi‐component photoactive structure to develop a self‐powering dual‐functional sensory device with effective energy harvesting and sensing capabilities. The optimized device demonstrates improved free‐charge generation yield by quantifying charge carrier dynamics, with a high output power density of over 81 and 76 µW cm−2 for rigid and flexible OPVs under indoor conditions (LED …

Shuqiang Jiao

Shuqiang Jiao

University of Science and Technology Beijing

Advanced Materials

Weak Electrostatic Force on K+ in Gel Polymer Electrolyte Realizes High Ion Transference Number for Quasi Solid‐State Potassium Ion Batteries

Quasi‐solid‐state potassium‐ion batteries (SSPIBs) are of great potential for commercial use due to the abundant reserves and cost‐effectiveness of resources, as well as high safety. Gel polymer electrolytes (GPEs) with high ionic conductivity and fast interfacial charge transport are necessary for SSPIBs. Here, the weak electrostatic force between K+ and electronegative functional groups in the ethoxylated trimethylolpropane triacrylate (ETPTA) polymer chains, which can promote fast migration of free K+, is revealed. To further enhance the interfacial reaction kinetics, a multilayered GPE by in situ growth of poly(vinylidenefluoride‐co‐hexafluoropropylene) (PVDF‐HFP) on ETPTA (PVDF‐HFP|ETPTA|PVDF‐HFP) is constructed to improve the interface contact and provide sufficient K+ concentration in PVDF‐HFP. A high ion transference number (0.92) and a superior ionic conductivity (5.15 × 10−3 S cm−1) are …

Albert Fan Yee

Albert Fan Yee

University of California, Irvine

Advanced Materials

Selective Induction of Molecular Assembly to Tissue‐Level Anisotropy on Peptide‐Based Optoelectronic Cardiac Biointerfaces

The conduction efficiency of ions in excitable tissues and of charged species in organic conjugated materials both benefit from having ordered domains and anisotropic pathways. In this study, a photocurrent‐generating cardiac biointerface is presented, particularly for investigating the sensitivity of cardiomyocytes to geometrically comply to biomacromolecular cues differentially assembled on a conductive nanogrooved substrate. Through a polymeric surface‐templated approach, photoconductive substrates with symmetric peptide‐quaterthiophene (4T)‐peptide units assembled as 1D nanostructures on nanoimprinted polyalkylthiophene (P3HT) surface are developed. The 4T‐based peptides studied here can form 1D nanostructures on prepatterned polyalkylthiophene substrates, as directed by hydrogen bonding, aromatic interactions between 4T and P3HT, and physical confinement on the nanogrooves. It is …

Weilin Zhang

Weilin Zhang

Georgia Institute of Technology

Advanced Materials

Harnessing High‐Throughput Computational Methods to Accelerate the Discovery of Optimal Proton Conductors for High‐Performance and Durable Protonic Ceramic Electrochemical Cells

The pursuit of high‐performance and long‐lasting protonic ceramic electrochemical cells (PCECs) has been impeded by the lack of efficient and enduring proton conductors. Conventional research approaches, predominantly based on a trial‐and‐error methodology, have proven to be demanding of resources and time‐consuming. Here we report our findings in harnessing high‐throughput computational methods to expedite the discovery of optimal electrolytes for PCECs. We methodically computed the oxygen vacancy formation energy (EV), hydration energy (EH), and the adsorption energies of H2O and CO2 for a set of 932 oxide candidates. Notably, our findings highlight BaSnxCe0.8‐xYb0.2O3‐δ (BSCYb) as a prospective game‐changing contender, displaying superior proton conductivity and chemical resilience when compared to the well‐regarded BaZrxCe0.8‐xY0.1Yb0.1O3‐δ (BZCYYb) series …

Hyun Kyu Song

Hyun Kyu Song

Korea University

Advanced Materials

Polymorphic Self‐Assembly with Procedural Flexibility for Monodisperse Quaternary Protein Structures of DegQ Enzymes

As large molecular tertiary structures, some proteins can act as small robots that find, bind, and chaperone target protein clients, showing the potential to serve as smart building blocks in self‐assembly fields. Instead of using such intrinsic functions, most self‐assembly methodologies for proteins aim for de novo‐designed structures with accurate geometric assemblies, which could limit procedural flexibility. Here, we present a strategy enabling polymorphic clustering of quaternary proteins, exhibiting simplicity and flexibility of self‐assembling paths for proteins in forming monodisperse quaternary cage particles. We propose that the enzyme protomer DegQ, previously solved at low resolution, may potentially be usable as a threefold symmetric building block, which can form polyhedral cages incorporated by the chaperone action of DegQ in the presence of protein clients. To obtain highly monodisperse cage …

Stephanie Law

Stephanie Law

University of Delaware

Advanced Materials

The Role of Optical Phonon Confinement in the Infrared Dielectric Response of III–V Superlattices

Polar dielectrics are key materials of interest for infrared (IR) nanophotonic applications due to their ability to host phonon‐polaritons that allow for low‐loss, subdiffractional control of light. The properties of phonon‐polaritons are limited by the characteristics of optical phonons, which are nominally fixed for most “bulk” materials. Superlattices composed of alternating atomically thin materials offer control over crystal anisotropy through changes in composition, optical phonon confinement, and the emergence of new modes. In particular, the modified optical phonons in superlattices offer the potential for so‐called crystalline hybrids whose IR properties cannot be described as a simple mixture of the bulk constituents. To date, however, studies have primarily focused on identifying the presence of new or modified optical phonon modes rather than assessing their impact on the IR response. This study focuses on …