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1.
ACS Nano ; 18(20): 13061-13072, 2024 May 21.
Artículo en Inglés | MEDLINE | ID: mdl-38721824

RESUMEN

Various strain isolation strategies that combine rigid and stretchable regions for stretchable electronics were recently proposed, but the vulnerability of inorganic materials to mechanical stress has emerged as a major impediment to their performance. We report a strain-isolation system that combines heteropolymers with different elastic moduli (i.e., hybrid stretchable polymers) and utilize it to construct a rugged island-bridge inorganic electronics system. Two types of prepolymers were simultaneously cross-linked to form an interpenetrating polymer network at the rigid-stretchable interface, resulting in a hybrid stretchable polymer that exhibited efficient strain isolation and mechanical stability. The system, including stretchable micro-LEDs and microheaters, demonstrated consistent operation under external strain, suggesting that the rugged island-bridge inorganic electronics mounted on a locally strain-isolated substrate offer a promising solution for replacing conventional stretchable electronics, enabling devices with a variety of form factors.

2.
Small ; : e2400031, 2024 Mar 18.
Artículo en Inglés | MEDLINE | ID: mdl-38497894

RESUMEN

Improving the hydroxide conductivity and dimensional stability of anion exchange membranes (AEMs) while retaining their high alkaline stability is necessary to realize the commercialization of AEM water electrolysis (AEMWE). A strategy for improving the hydroxide conductivity and dimensional stability of AEMs by inserting fluorine atoms in the core structure of the backbone is reported, which not only reduces the glass transition temperature of the polymer due to steric strain, but also induces distinct phase separation by inducing polarity discrimination to facilitate the formation of ion transport channels. The resulting PFPFTP-QA AEM with fluorine into the core structure shows high hydroxide conductivity (>159 mS cm-1 at 80 °C), favorable dimensional stability (>25% at 80 °C), and excellent alkaline stability for 1000 h in 2 m KOH solution at 80 °C. Moreover, the PFPFTP-QA is used to construct an AEMWE cell with a platinum group metal (PGM)-free NiFe anode, which exhibits the current density of 6.86 A cm-2 at 1.9 V at 80 °C, the highest performance in Pt/C cathode and PGM-free anode reports so far and operates stably for over 100 h at a constant current of 0.5 A cm-2 .

3.
Small Methods ; 8(2): e2300238, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-37322273

RESUMEN

Recently, multijunction tandem solar cells (TSCs) have presented high power conversion efficiency and revealed their immense potential in photovoltaic evolution. It is demonstrated that multiple light absorbers with various bandgap energies overcome the Shockley-Queisser limit of single-junction solar cells by absorbing the wide-range wavelength photons. Here, the main key challenges are reviewed, especially the charge carrier dynamics in perovskite-based 2-terminal (2-T) TSCs in terms of current matching, and how to manage these issues from a vantage point of characterization. To do this, the effect of recombination layers, optical and fabrication hurdles, and the impact of wide bandgap perovskite solar cells are discussed extensively. Afterward, this review focuses on various optoelectronics, spectroscopic, and theoretical (optical simulation) characterizations to figure out those issues, especially current-matching issues faced by the photovoltaic society. This review comprehensively provides deep insights into the relationship between the current-matching problems and the photovoltaic performance of TSCs through a variety of perspectives. Consequently, it is believed that this review is essential to address the main problems of 2-T TSCs, and the suggestions to elucidate the charge carrier dynamics and its characterization may pave the way to overcome such obstacles to further improve the development of 2-T TSCs in relation to the current-matching problems.

4.
Small ; 19(50): e2304274, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37626461

RESUMEN

To achieve the global goal of carbon neutrality, recently, emphasis has been placed on developing green ammonia production method to replace the Haber-Bosch process. Nitrate reduction reaction (NO3 RR) has received considerable attention, especially for electrochemically producing ammonia from nitrate and simultaneously purifying wastewater. This study first demonstrates that the combination of NO3 RR with hydrazine oxidation reaction (HzOR) is an energy efficient green ammonia production method, which overcomes the sluggish water oxidation limitation. Tungsten phosphide (WP) nanowires (NWs) are prepared as cathode NO3 RR electrocatalysts, which exhibit a high Faradaic efficiency in both neutral (≈93%) and alkaline (≈85%) media. Furthermore, they show a high bifunctional activity in anodic reactions and exhibit a low potential 0.024 V for generating a current density of 10 mA cm-2 in HzOR. The overall NO3 RR-HzOR required an impressively low potential of 0.24 V for generating a current density of 10 mA cm-2 ; this potential is much lower than those required for NO3 RR-OER (1.53 V) and NO3 RR-UOR (1.31 V). A self-powered ammonia production system, prepared by assembling an NO3 RR-HzOR with a perovskite solar cell, displays a high ammonia production rate of 1.44 mg cm-2  h-1 . A single PV cell provides enough driving voltage in the PV-EC due to low required potential. This system facilitates unassisted green ammonia synthesis with a low energy consumption and also allows upcycling of wastewater to produce useful fuel.

5.
Adv Sci (Weinh) ; 10(24): e2302376, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-37357145

RESUMEN

The advancement of non-fullerene acceptors with crescent-shaped geometry has led to the need for polymer donor improvements. Additionally, there is potential to enhance the photovoltaic parameters in high-efficiency organic solar cells (OSCs). The random copolymerization method is a straightforward and effective strategy to further optimize photoactive morphology and enhance device performance. However, finding a suitable third component in terpolymers remains a crucial challenge. In this study, a series of terpolymer donors (PTF3, PTF5, PTF10, PTF20, and PTF50) is synthesized by introducing varying amounts of the trifluoromethyl-substituted unit (CF3) into the PM6 polymer backbone. Even subtle changes in the CF3 content can significantly enhance all the photovoltaic parameters due to the optimized energy levels, molecular aggregation/miscibility, and bulk-heterojunction morphology of the photoactive materials. Thus, the best binary OSC based on the PTF5:Y6-BO achieves an outstanding power conversion efficiency (PCE) of 18.2% in the unit cell and a PCE of 11.6% in the sub-module device (aperture size: 54.45 cm2 ), when using halogen-free solvent o-xylene. This work showcases the remarkable potential of the easily accessible CF3 unit as a key constituent in the construction of terpolymer donors in high-performance OSCs.

6.
ACS Appl Mater Interfaces ; 15(22): 27026-27033, 2023 Jun 07.
Artículo en Inglés | MEDLINE | ID: mdl-37220162

RESUMEN

High thermal stability is crucial for the commercialization of organic solar cells (OSCs). The thermal stability of OSCs has been improved using the tailoring blend morphology of bulk heterojunctions (BHJs). Herein, we demonstrated thermally stable OSCs in a ternary blended system containing low-crystalline semiconducting polymers (asy-PNDI1FTVT and PTB7-Th) and a non-fullerene acceptor (Y6). The asymmetric n-type semiconducting polymer (asy-PNDI1FTVT) differed from general symmetric semiconducting polymers as it randomly substituted fluorine atoms at the donor moiety (TVT), resulting in significantly lower crystallinity. asy-PNDI1FTVT in PTB7-Th:Y6 exhibited a well-mixed morphology at the BHJ and efficiently facilitated the charge dissociation process with an enhanced fill factor and power conversion efficiency. Furthermore, the ternary system of PTB7-Th:Y6:asy-PNDI1FTVT suppressed phase separation with negligible burn-in loss and performance degradation under thermal stress. The experiments showed that our devices without encapsulation retained over 90% of their initial efficiencies after 100 h at 65 °C. These results show significant potential for the development of thermally stable OSCs with reasonable efficiency.

7.
Nat Commun ; 14(1): 1990, 2023 Apr 08.
Artículo en Inglés | MEDLINE | ID: mdl-37031201

RESUMEN

Electroadhesion provides a promising route to augment robotic functionalities with continuous, astrictive, and reversible adhesion force. However, the lack of suitable conductive/dielectric materials and processing capabilities have impeded the integration of electroadhesive modules into soft robots requiring both mechanical compliance and robustness. We present herein an iontronic adhesive based on a dynamically crosslinked gel-elastomer system, including an ionic organohydrogel as adhesive electrodes and a resilient polyurethane with high electrostatic energy density as dielectric layers. Through supramolecular design and synthesis, the dual-material system exhibits cohesive heterolayer bonding and autonomous self-healing from damages. Iontronic soft grippers that seamlessly integrate actuation, adhesive prehension, and exteroceptive sensation are devised via additive manufacturing. The grippers can capture soft and deformable items, bear high payload under reduced voltage input, and rapidly release foreign objects in contrast to electroadhesives. Our materials and iontronic mechanisms pave the way for future advancement in adhesive-enhanced multifunctional soft devices.

8.
Adv Mater ; 35(4): e2203430, 2023 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-35700966

RESUMEN

The power conversion efficiency of CsPbI3 perovskite quantum dot (PQD) solar cells shows increase from 10.77% to 16.2% in a short period owing to advances in material and device design for solar cells. However, the device stability of CsPbI3 PQD solar cells remains poor in ambient conditions, which requires an in-depth understanding of the degradation mechanisms of CsPbI3 PQDs solar cells in terms of both inherent material properties and device characteristics. Along with this analysis, advanced strategies to overcome poor device stability must be conceived. In this review, fundamental mechanisms that cause the degradation of CsPbI3 PQD solar cells are discussed from the material property and device viewpoints. In addition, based on detailed insights into degradation mechanisms in CsPbI3 PQD solar cells, various strategies are introduced to improve the stability of CsPbI3 PQD solar cells. Finally, future perspectives and challenges are presented to achieve highly durable CsPbI3 PQD solar cells. The investigation of the degradation mechanisms and the stability enhancement strategies can pave the way for the commercialization of CsPbI3 PQD solar cells.

9.
Inorg Chem ; 62(1): 43-55, 2023 Jan 09.
Artículo en Inglés | MEDLINE | ID: mdl-36547377

RESUMEN

Three new cationic cyclometalated iridium(III) complexes equipped with differently substituted benzo[b]thiophen-2-ylquinoline cyclometalating ligands and with a sterically demanding tert-butyl-substituted 2,2'-bipyridine ancillary ligand were synthesized and structurally characterized by NMR and X-ray diffraction techniques. To tune the electronic properties of such complexes, the quinoline moiety of the cyclometalating ligands was kept pristine or equipped with electron-withdrawing phenyl and -CF3 substituents, leading to complexes 1, 2, and 3, respectively. A complete electrochemical and photophysical investigation, supported by density functional theory calculations, permits a deep understanding of their electronic properties. The emission of all complexes arises from ligand-centered triplet states in the spectral range between 625 and 950 nm, with excited-state lifetimes between 2.10 and 6.32 µs at 298 K. The unsubstituted complex (1) exhibits the most blue-shifted emission in polymeric matrix at 298 K (λmax = 667 nm, photoluminescence quantum yield (PLQY) = 0.25 and τ = 5.32 µs). The phenyl-substituted complex (2) displays the highest photoluminescent quantum yields (up to 0.30 in polymeric matrix), while the CF3-substituted counterpart (3) shows the most red-shifted emission, peaking at approx. 720 nm, but with lower quantum yields (e.g., 0.10 in polymeric matrix at 298 K). Complexes 1 and 2 were tested in single-layer nondoped light-emitting electrochemical cells (LEECs), using a nozzle-printing technique; both devices display deep-red electroluminescence with an external quantum efficiency close to 20%.

10.
Nanomicro Lett ; 14(1): 204, 2022 Oct 17.
Artículo en Inglés | MEDLINE | ID: mdl-36251125

RESUMEN

Perovskite quantum dots (PQDs) have been considered promising and effective photovoltaic absorber due to their superior optoelectronic properties and inherent material merits combining perovskites and QDs. However, they exhibit low moisture stability at room humidity (20-30%) owing to many surface defect sites generated by inefficient ligand exchange process. These surface traps must be re-passivated to improve both charge transport ability and moisture stability. To address this issue, PQD-organic semiconductor hybrid solar cells with suitable electrical properties and functional groups might dramatically improve the charge extraction and defect passivation. Conventional organic semiconductors are typically low-dimensional (1D and 2D) and prone to excessive self-aggregation, which limits chemical interaction with PQDs. In this work, we designed a new 3D star-shaped semiconducting material (Star-TrCN) to enhance the compatibility with PQDs. The robust bonding with Star-TrCN and PQDs is demonstrated by theoretical modeling and experimental validation. The Star-TrCN-PQD hybrid films show improved cubic-phase stability of CsPbI3-PQDs via reduced surface trap states and suppressed moisture penetration. As a result, the resultant devices not only achieve remarkable device stability over 1000 h at 20-30% relative humidity, but also boost power conversion efficiency up to 16.0% via forming a cascade energy band structure.

11.
ACS Appl Mater Interfaces ; 14(18): 20848-20855, 2022 May 11.
Artículo en Inglés | MEDLINE | ID: mdl-35476422

RESUMEN

Defect passivation has become essential in improving efficiency and stability in perovskite solar cells. Here, we report the use of (α-methylguanido)acetic acid, also known as creatine, as a passivation molecule. It is employed both as an additive and as a surface passivation layer of perovskite thin films, given its multiple functional groups, which could address different defect sites, and its size, which could inherently affect the material structure. We prove that the surface passivation is more efficiently working by removing vulnerable defects on the surface. Hole and electron defect densities were reduced, leading to the highest power conversion efficiency of 22.6%. In addition, it can effectively protect the perovskite thin film and improve the operational stabilities in high thermal (85 °C) and humid conditions (50% relative humidity), suggesting a strong stability of the surface passivation layer.

12.
Angew Chem Int Ed Engl ; 61(11): e202117303, 2022 Mar 07.
Artículo en Inglés | MEDLINE | ID: mdl-35060264

RESUMEN

Defects and energy offsets at the bulk and heterojunction interfaces of perovskite are detrimental to the efficiency and stability of perovskite solar cells (PSCs). Herein, we designed an amphiphilic π-conjugated ionic compound (QAPyBF4 ), implementing simultaneous defects passivation and interface energy level alignments. The p-type conjugated cations passivated the surface trap states and optimized energy alignment at the perovskite/hole transport layer. The highly electronegative [BF4 ]- enriched at the SnO2 interface featured desired band alignment due to the dipole moment of this interlayer. The planar n-i-p PSC had an efficiency of 23.1 % with Voc of 1.2 V. Notably, the synergy effect elevated the intrinsic endothermic decomposition temperature of the perovskite. The modified devices showed excellent long-term thermal (85 °C) and operational stability at the maximum power point for 1000 h at 45 °C under continuous one-sun illumination with no appreciable efficiency loss.

13.
Chem Sci ; 12(42): 14004-14023, 2021 Nov 03.
Artículo en Inglés | MEDLINE | ID: mdl-34760184

RESUMEN

Organic photovoltaics (OPVs) have emerged as a promising next-generation technology with great potential for portable, wearable, and transparent photovoltaic applications. Over the past few decades, remarkable advances have been made in non-fullerene acceptor (NFA)-based OPVs, with their power conversion efficiency exceeding 18%, which is close to the requirements for commercial realization. Novel molecular NFA designs have emerged and evolved in the progress of understanding the physical features of NFA-based OPVs in relation to their high performance, while there is room for further improvement. In this review, the molecular design of representative NFAs is described, and their blend characteristics are assessed via statistical comparisons. Meanwhile, the current understanding of photocurrent generation is reviewed along with the significant physical features observed in high-performance NFA-based OPVs, while the challenging issues and the strategic perspectives for the commercialization of OPV technology are also discussed.

14.
ChemSusChem ; 14(17): 3475-3487, 2021 Sep 06.
Artículo en Inglés | MEDLINE | ID: mdl-34164933

RESUMEN

Organic photovoltaics (OPVs) are a promising next-generation photovoltaic technology with great potential for wearable and transparent device applications. Over the past decades, remarkable advances in device efficiency close to 20 % have been made for bulk heterojunction (BHJ)-based OPV devices with long-term stability, and room for further improvements still exists. In recent years, ancillary components have been demonstrated as effective in improving the photovoltaic performance of OPVs by controlling the optoelectronic and morphological properties of BHJ blends. Herein, an updated understanding of polymer-based blend OPVs is provided, and the role and impact of ancillary components in various blend systems are categorized and discussed. Lastly, a strategic perspective on the ancillary components of blend-based OPVs for commercialization is provided.

15.
ACS Appl Mater Interfaces ; 13(14): 16722-16731, 2021 Apr 14.
Artículo en Inglés | MEDLINE | ID: mdl-33543611

RESUMEN

The effects of the microstructure of conjugated polymer thin films on charge trapping and operational stability of organic field-effect transistors (OFETs) are investigated. Device characteristics of OFETs based on two model conjugated polymers, poly(3-hexylthiophene) (P3HT) and a random 3-hexylthiophene-thiophene copolymer (RP33), are compared. P3HT films have high crystallinity and long-range molecular order, whereas RP33 films have low crystallinity and short-range molecular order as well as enhanced polymer backbone planarity. Experimental evidence shows that although the microstructure of the RP33 film provides efficient charge transport pathways, its high degree of structural disorder causes severe shallow trapping of charge carriers, which results in its inferior stability under bias stress. This study demonstrates that low-crystalline conjugated polymers with short-range order can provide a high charge-carrier mobility but at the same time be inappropriate for practical OFETs because of their poor intrinsic operational stability.

16.
Small ; 16(45): e2002460, 2020 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-33079485

RESUMEN

Quantum dots (QDs) are emerging photovoltaic materials that display exclusive characteristics that can be adjusted through modification of their size and surface chemistry. However, designing a QD-based optoelectronic device requires specialized approaches compared with designing conventional bulk-based solar cells. In this paper, design considerations for QD thin-film solar cells are introduced from two different viewpoints: optics and electrics. The confined energy level of QDs contributes to the adjustment of their band alignment, enabling their absorption characteristics to be adapted to a specific device purpose. However, the materials selected for this energy adjustment can increase the light loss induced by interface reflection. Thus, management of the light path is important for optical QD solar cell design, whereas surface modification is a crucial issue for the electrical design of QD solar cells. QD thin-film solar cell architectures are fabricated as a heterojunction today, and ligand exchange provides suitable doping states and enhanced carrier transfer for the junction. Lastly, the stability issues and methods on QD thin-film solar cells are surveyed. Through these strategies, a QD solar cell study can provide valuable insights for future-oriented solar cell technology.

17.
Adv Mater ; 32(48): e2004985, 2020 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-33118229

RESUMEN

The need for optoelectronic and chemical compatibility between the layers in colloidal quantum dot (CQD) photovoltaic devices remains a bottleneck in further increasing performance. Conjugated polymers are promising candidates as new hole-transport layer (HTL) materials in CQD solar cells (CQD-SCs) owing to the highly tunable optoelectronic properties and compatible chemistries. A diketopyrrolopyrrole-based polymer with benzothiadiazole derivatives (PD2FCT-29DPP) as an HTL in these devices is reported. The energy level, molecular orientation, and hole mobility of this HTL are manipulated through molecular engineering. By levering the polymer's optical absorption spectrum complementary to that of the CQD active layer, EQE across the visible and near-infrared regions is maximized. As a result, a PD2FCT-29DPP-based device exhibits a fill factor of 70% and approximately 35% efficiency enhancement compared to a PTB7-based device.

18.
Adv Mater ; 32(42): e2004657, 2020 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-32939875

RESUMEN

Monolithically integrated hybrid tandem solar cells (TSCs) that combine solution-processed colloidal quantum dot (CQD) and organic molecules are a promising device architecture, able to complement the absorption across the visible to the infrared. However, the performance of organic/CQD hybrid TSCs has not yet surpassed that of single-junction CQD solar cells. Here, a strategic optical structure is devised to overcome the prior performance limit of hybrid TSCs by employing a multibuffer layer and a dual near-infrared (NIR) absorber. In particular, a multibuffer layer is introduced to solve the problem of the CQD solvent penetrating the underlying organic layer. In addition, the matching current of monolithic TSCs is significantly improved to 15.2 mA cm-2 by using a dual NIR organic absorber that complements the absorption of CQD. The hybrid TSCs reach a power conversion efficiency (PCE) of 13.7%, higher than that of the corresponding individual single-junction cells, representing the highest efficiency reported to date for CQD-based hybrid TSCs.

19.
Adv Mater ; 32(7): e1906679, 2020 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-31858638

RESUMEN

For emerging biocompatible, wearable, and stretchable epidermal electronic devices, it is essential to realize novel stretchable conductors with the attributes of transparency, low-cost and nontoxic components, green-solvent processbility, self-healing, and thermal stabililty. Although conducting materials-rubber composites, ionic hydrogels, organogels have been developed, no stretchable material system that meets all the outlined requirements has been reported. Here, a series of P(SPMA-r-MMA) polymers with different ratios of ionic side chains is designed and synthesized, and it is demonstrated that the resulting stretchable ionic conductors with glycerol are transparent, water processable, self-healable, and thermally stable due to the chemically linked ionic side chain, satisfying all of the aforementioned requirements. Among the series of polymer gels, the P(SPMA0.75 -r-MMA0.25 ) gel shows optimum conductivity (6.7 × 10-4 S cm-1 ), stretchability (2636% of break at elongation), and self-healing (98.3% in 3 h) properties. Accordingly, the transparent and self-healable P(SPMA0.75 -r-MMA0.25 ) gels are used to realize thermally robust actuators up to 100 °C and deformable and self-healable thermal sensors.

20.
Small ; 15(49): e1905501, 2019 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-31682059

RESUMEN

Complementary water splitting electrocatalysts used simultaneously in the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) can simplify water splitting systems. Herein, earth-abundant NiMoFe (NMF) and phosphorized NiMoFeP (NMFP) are synthesized as complementary overall water splitting (OWS) catalysts. First, NMF is tested as both the HER and OER promoter, which exhibits low overpotentials of 68 (HER) and 337 mV (OER). A quaternary NMFP is then prepared by simple phosphorization of NMF, which shows a much lower OER overpotential of 286 mV. The enhanced OER activity is attributed to the unique surface/core structure of NMFP. The surface phosphate acts as a proton transport mediator and expedites the rate-determining step. With the application of OER potential, the NMFP surface is composed of Ni(OH)2 and FeOOH, active sites for OER, but the inner core consists of Ni, Mo, and Fe metals, serving as a conductive electron pathway. OWS with NMF-NMFP requires an applied voltage of 1.452 V to generate 10 mA cm-2 , which is one of the lowest values among OWS results with transition-metal-based electrocatalysts. Furthermore, the catalysts are combined with tandem perovskite solar cells for photovoltaic (PV)-electrolysis, producing a high solar-to-hydrogen (STH) conversion efficiency of 12.3%.

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