Assisted Solubilization Strategy in Spiro‐OMeTAD for Thermally and Mechanically Stable Perovskite Solar Cells

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 3, 2025

The ions migration and de-doping reactions caused by conventional doping seriously jeopardizes the thermal stability of perovskite solar cells (PVSCs) based on spiro-OMeTAD as hole transport layer (HTL), which poses a significant challenge for subsequent commercialization. To address these issues, novel assisted solubilization strategy has been firstly developed using deep eutectic solvent (DES) synthesized from N-(cyanomethyl)acetamide (NCMA) lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). NCMA can form multiple strong interaction modes with LiTFSI through N-H⋅⋅⋅O hydrogen bonding Li-O/Li-N coordination, effectively inhibits Li+ at high temperature increases solubility in chlorobenzene without acetonitrile 4-tert-butylpyridine (tBP), fundamentally solving reaction. In addition, molecular network abundant functional groups DES improves fracture energy perovskite/spiro-OMeTAD interface enhances interfacial adhesion via chelation Ag electrode. Consequently, benefiting tBP removement inhibited migration, optimized PVSCs achieve power conversion efficiency (PCE) 25.02 %, unencapsulated device retains over 90 % initial PCE 85 °C, 40 RH 1200 h (ISOS-D-2 standard). This innovative represents critical step toward improving accelerating commercialization PVSCs.

Language: Английский

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Assisted Solubilization Strategy in Spiro‐OMeTAD for Thermally and Mechanically Stable Perovskite Solar Cells

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 3, 2025

Abstract The ions migration and de‐doping reactions caused by conventional doping seriously jeopardizes the thermal stability of perovskite solar cells (PVSCs) based on spiro‐OMeTAD as hole transport layer (HTL), which poses a significant challenge for subsequent commercialization. To address these issues, novel assisted solubilization strategy has been firstly developed using deep eutectic solvent (DES) synthesized from N‐(cyanomethyl)acetamide (NCMA) lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). NCMA can form multiple strong interaction modes with LiTFSI through N−H⋅⋅⋅O hydrogen bonding Li−O/Li−N coordination, effectively inhibits Li + at high temperature increases solubility in chlorobenzene without acetonitrile 4‐tert‐butylpyridine (tBP), fundamentally solving reaction. In addition, molecular network abundant functional groups DES improves fracture energy perovskite/spiro‐OMeTAD interface enhances interfacial adhesion via chelation Ag electrode. Consequently, benefiting tBP removement inhibited migration, optimized PVSCs achieve power conversion efficiency (PCE) 25.02 %, unencapsulated device retains over 90 % initial PCE 85 °C, 40 RH 1200 h (ISOS‐D‐2 standard). This innovative represents critical step toward improving accelerating commercialization PVSCs.

Language: Английский

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Accelerated discovery of high-performance small-molecule hole transport materials via molecular splicing, high-throughput screening, and machine learning

Journal of Materials Informatics, Journal Year: 2025, Volume and Issue: 5(3)

Published: April 15, 2025

As the most representative and widely utilized hole transport material (HTM), spiro-OMeTAD encounters challenges including limited mobility, high production costs, demanding synthesis conditions. These issues have a notable impact on overall performance of perovskite solar cells (PSCs) based hinder its large-scale commercial application. Consequently, there exists strong demand for high-throughput computational design novel small-molecule HTMs (SM-HTMs) that are cost-effective, easy to synthesize, offer excellent performance. In this study, systematic iterative development process SM-HTMs is proposed, aiming accelerate discovery application high-performance SM-HTMs. A custom-developed molecular splicing algorithm (MSA) generated sample space 200,000 intermediate molecules, culminating in creation comprehensive database over 7,000 potential SM-HTM candidates. total, six promising HTM candidates were identified through MSA, density functional theory calculations screening. Furthermore, three machine learning algorithms, namely random forest, gradient boosting decision tree, extreme (XGBoost), employed construct predictive models key properties, recombination energy, solvation free maximum absorption wavelength, hydrophobicity. Among these, XGBoost-based model demonstrated best The MSA methodology combining prediction models, as introduced offers powerful universal toolkit optimization next-generation SM-HTMs, thereby paving way future advancements PSCs.

Language: Английский

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Aggregation State Regulation of Molecular Hole Conductors for Light‐Stable Perovskite Photovoltaics

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: May 2, 2025

Abstract The molecular aggregation state of organic hole conductors greatly influences charge collection perovskite solar cells (PSCs). In this study, we optimize the core/periphery steric Cl‐substituent (W1, W2, W3) and regulate by packing interactions. It is demonstrated that W1 with Cl core‐substituent exhibits enhanced crystallization strong intermolecular interactions in contrast to W2 sidechain‐substituent. Conversely, W3 substituent at both core sidechain results most unfavorable stacking. high mobility reinforced interfacial bonding, achieving a remarkable photovoltaic efficiency 24.7%, outperforming other two (W2's 23.9% W3's 20.3%). Furthermore, W1‐ W2‐PSCs retain 95.3% 87.2% their initial after 1,000 hours maximum power point tracking (MPPT), respectively. This work provides fundamental insights into Cl‐substituent‐induced behavior offers delicate approach for designing high‐performance semiconductors.

Language: Английский

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Halide Perovskites Multifunctional Property: Coordination Engineering, Coordination Chemistry, Electronic Interactions and Energy Applications beyond Photovoltaic

Published: April 28, 2024

Halide perovskite materials gain enormous attention for their semiconducting properties, higher power conversion efficiency and potential applications in a wide range field of studies along with two key limitations: stability toxicity. In spite great progress made on the halide perovskites many promising research developments, overcoming these limitations is not realized yet. Therefore, coordination engineering new framework obtaining alternative fundamental understanding chemistry electronic interactions forming structure newly engineered might be one way order to overcome issues related both this review, current development families, lead free followed by frameworks engineer will reviewed comprehensively. Moreover, all concerns ideas that are keys structures discussed detail form main aim review. Interestingly, we also discuss recent energy beyond photovoltaic review has completed an essential open question: ‘what could happen future perovskites?’ excite commercial enterprises institutions again as well get motivating predictions continuity field.

Language: Английский

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Halide Perovskites’ Multifunctional Properties: Coordination Engineering, Coordination Chemistry, Electronic Interactions and Energy Applications beyond Photovoltaics

Inorganics, Journal Year: 2024, Volume and Issue: 12(7), P. 182 - 182

Published: June 28, 2024

Halide perovskite materials have gained enormous attention for their semiconducting properties, higher power conversion efficiency and potential applications in a wide range of fields study, along with two key limitations: stability toxicity. Despite great progress made on halide perovskites many promising research developments, the issues toxicity not been fully resolved. Therefore, coordination engineering new framework to obtain alternative fundamental understanding chemistry electronic interactions forming structure these newly engineered are possible ways overcome related both In this review, we comprehensively review current development families, lead lead-free perovskites, followed by frameworks engineer materials. All concerns regarding ideas vital structures thus form main aim review. We also discuss recent energy beyond photovoltaics answer an essential open question, ‘what could happen future perovskites?’ order excite commercial enterprises institutions again as well motivate predictions continuity field.

Language: Английский

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Tailoring Diversified Peripheral Anchor Groups in Spirofluorene‐Dithiolane‐Based Hole Transporting Materials for Efficient Organic and Perovskite Solar Cells from First‐Principle

Advanced Theory and Simulations, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 17, 2024

Abstract This quantum mechanical approach recommends push–pull molecular engineering to fabricate hole‐transporting materials (HTMs) for photovoltaic cells. It integrates acceptor moieties via thiophene fluorene core, resulting in five novel HTMs (SFD‐1 SFD‐5). The results exhibit that derivative show excellent coherence excitation, dispersion, and transportation of charge carriers, ensuring robust hole mobility. anchor functionalized unveil band alignment with perovskite fitting HOMO energy levels (−4.93–−5.35 eV), less optical absorption visible portion ( < 520). integration has improved the mobility derivatives, accredited smaller reorganization (0.14–0.68 greater transfer integral (0.22–0.33 eV). transition density matrix analysis exhibited electronic coupling, subtler carrier overlapping length (7.48–13.73 Å). resulted an upsurge intrinsic transference (70.75–92.70%) exciton binding energy, leading easier dissociation, fewer recombination fatalities. However, adequate variation dipole moment (4.04 D 16.34 D) Gibbs solvation‐free (−18.06 −21.89 kcal mol −1 ) ensures facile film formation processability. In conclusion, this these flourene‐based are highly desireable forthcoming solar cell technology.

Language: Английский

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Asymmetric Modification of Carbazole Based Self‐Assembled Monolayers by Hybrid Strategy for Inverted Perovskite Solar Cells

Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 5, 2024

Abstract Carbazole‐based self‐assembled molecules (SAMs) are widely applied in inverted perovskite solar cells (iPSCs) due to their unique molecular properties. However, the symmetrical structure of carbazole‐based SAMs makes it difficult finely regulate performance, which impedes further enhancement efficiency and stability iPSCs. This work demonstrates that by constructing an asymmetric carbazole core, 9H‐thieno[2′,3′ : 4,5]thieno[3,2‐b]indole) (TTID), key properties SAM can be effectively regulated. It has been confirmed hybrid thieno[2,3‐b]thiophene unit this core governs energy level, surface wettability, defect passivation capability SAMs, while substituent a greater impact on dipole device stability. The synergistic effects from fluorine lead KF‐derived iPSC demonstrating certified power conversion (PCE) 25.17 % excellent operational design concept offers promising approach for structural modification

Language: Английский

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Heterogeneous Amine with Polycyclic‐Aromatics‐Modified Hole Transport Material for Efficient and Operationally Durable Perovskite Solar Cells

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 10, 2024

Abstract Achieving efficient perovskite solar cells (PSCs) with high operational durability is a challenging task. Here, by exploiting the heterogeneous amine strategy at molecular level, novel spirobifluorene derivative bearing methoxynaphthalene and 9,9‐dimethylfluorene peripheral groups ( N 2 , 2′ 7 7′ ‐tetrakis(9,9‐dimethyl‐9 H ‐fluoren‐2‐yl)‐ ‐tetrakis(6‐methoxynaphthalen‐2‐yl)‐9,9′‐spirobi[fluorene]‐2,2′,7,7′‐tetraamine, denoted as Spiro‐NADF) hole transport material (HTM) developed to address efficiency issues of PSCs. Compared 2,2′,7,7′‐tetrakis( ‐di‐ p ‐methoxyphenyl)‐amine‐9,9′‐spirobifluorene, Spiro‐NADF exhibits not only favorable energy level alignment but also higher glass transition temperature strong adhesion perovskite. Moreover, Spiro‐NADF‐based layer shows excellent morphological stability in devices against damp heat stress. These advantages reduce voltage loss suppress decomposition ion migration. Consequently, PSCs based on exhibit champion 24.66% an open‐circuit 1.19 V. The corresponding show greatly enhanced harsh environments, retaining over 92% initial efficiencies for 500 h aging under test (85 °C 70–90% relative humidity) illumination maximum power point tracking, respectively. This work demonstrates that engineering HTMs using amines polycyclic aromatics leaves considerable room developing stable

Language: Английский

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Band edge engineering of lead halide perovskites using carboxylic‐based self‐assembled monolayer for efficient photovoltaics

EcoEnergy, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 7, 2024

Abstract Perovskite solar cells are promising candidates for low‐cost and efficient photovoltaic markets, but their efficiency is usually limited by the non‐radiative recombination losses at mismatched interface of perovskite transport layers. Herein, we show that band edges thin films can be on‐demand engineered a series carboxylic‐based self‐assembled monolayers. Experimental theoretical studies indicate functionalized inherits polarity monolayer with linear dependence work function on molecular dipole moments, which enables management interfacial charge process. Solar 4‐bromophenylacetic acid SAMs achieve about 6.48% enhancement in power conversion champion values over 23%.

Language: Английский

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