During the last decade,perovskite solar technologies underwent an impressive development,with power conversion efficiencies reaching 25.5%for single-junction devices and 29.8%for Silicon-Perovskite tandem configuratio...During the last decade,perovskite solar technologies underwent an impressive development,with power conversion efficiencies reaching 25.5%for single-junction devices and 29.8%for Silicon-Perovskite tandem configurations.Even though research mainly focused on improving the efficiency of perovskite photovoltaics(PV),stability and scalability remain fundamental aspects of a mature photovoltaics technology.For n-i-p structure perovskite solar cells,using poly-triaryl(amine)(PTAA)as hole transport layer(HTL)allowed to achieve marked improvements in device stability compared with other common hole conductors.For p-i-n structure,poly-triaryl(amine)is also routinely used as dopant-free hole transport layer,but problems in perovskite film growth,and its limited resistance to stress and imperfect batch-to-batch reproducibility,hamper its use for device upscaling.Following previous computational investigations,in this work,we report the synthesis of two small-molecule organic hole transport layers(BPT-1,2),aiming to solve the above-mentioned issues and allow upscale to the module level.By using BPT-1 and methylammonium-free perovskite,max.Power conversion efficiencies of 17.26%and 15.42%on a small area(0.09 cm^(2))and mini-module size(2.25 cm^(2)),respectively,were obtained,with a better reproducibility than with poly-triaryl(amine).Moreover,BPT-1 was demonstrated to yield more stable devices compared with poly-triaryl(amine)under ISOS-D1,T1,and L1 accelerated life-test protocols,reaching maximum T_(90)values>1000 h on all tests.展开更多
The Buchwald-Hartwig coupling enables the grafting of nitrogen-containing functionalities onto molecules,facilitating the synthesis of a wide variety of molecular structures.However,several challenges impact the susta...The Buchwald-Hartwig coupling enables the grafting of nitrogen-containing functionalities onto molecules,facilitating the synthesis of a wide variety of molecular structures.However,several challenges impact the sustainability of this coupling.In our pursuit of a more sustainable Buchwald-Hartwig process,we report an optimized protocol that enhances energy efficiency and minimizes waste.Utilizing recoverable Pd/C as a catalyst,we performed the process in the bio-based solvent 2-MeTHF.To further boost energy efficiency,we employed microwave heating technology,resulting in improved overall process efficiency and reduced reaction times.This optimized approach allowed for the synthesis of a wide array of 17 variously functionalized arylamines.Thanks to the optimized workup procedure that facilitated the recovery and reuse of the catalyst,ligand,and 2-MeTHF,we achieved a reduced E-Factor ranging from 5.8 to 14.9,further contributing to the sustainability of the process.展开更多
The excellent ability of dye-sensitized solar cells(DSSCs)to capture ambient light and convert it into electric current makes them attractive power sources for indoor applications,including powering Internet of Things...The excellent ability of dye-sensitized solar cells(DSSCs)to capture ambient light and convert it into electric current makes them attractive power sources for indoor applications,including powering Internet of Things(IoT)devices.In this context,substantial research efforts have been devoted to the discovery of novel organic dyes able to harvest energy from a wide range of indoor light sources at different intensities.However,such activities are often based on trial-and-error procedures which are frequently expensive and time-consuming.Here,Machine Learning(ML)techniques and Density Functional Theory(DFT)methods have been combined in a two-stage approach,with the aim to accelerate the design of new,synthetically accessible organic dyes for indoor DSSC applications.By predicting the power conversion efficiency(PCE)under different indoor light sources and intensities,potentially high-performance organic dyes have been identified.展开更多
The self-assembling properties, stability, and dynamics of hybrid nanocarriers （gold nanoparticles （AuNPs） functionalized with cysteine-based peptides） in solution are studied through a series of classical molecul...The self-assembling properties, stability, and dynamics of hybrid nanocarriers （gold nanoparticles （AuNPs） functionalized with cysteine-based peptides） in solution are studied through a series of classical molecular dynamics simulations based on a recently parametrized reactive force field. The results reveal, at the atomic level, all the details regarding the peptide adsorption mechanisms, nanoparticle stabilization, aggregation, and sintering. The data confirm and explain the experimental findings and disclose aspects that cannot be scrutinized by experiments. The biomolecules are both chemisorbed and physisorbed; self-interactions of the adsorbates and formation of stable networks of inter- connected molecules on the AuNP surfaces limit substrate reconstructions, protect the AuNPs from the action of the solvent, and prevent direct interactions of the gold surfaces. The possibility of agglomeration of the functionalized nanoparticles, compared with the sintering of the bare supports in a water solution, is demonstrated through relatively long simulations and fast steered dynamics. The analysis of the trajectories reveals that the AuNPs were well stabilized by the peptides. This prevented particle sintering and kept the particles far apart; however, part of their chains could form interconnections （crosslinks） between neighboring gold vehicles. The excellent agreement of these results with the literature confirm the reliability of the method and its potential application to the modeling of more complex materials relevant to the biomedical sector.展开更多
基金funding from the Italian Ministry of Economic Development(MISE)in the framework of the Operating Agreement with ENEA for Research on the Electric Systemfrom the Italian Ministry of University and Research(MUR)in the framework of“BEST4U”Project,PON R&I 2014-2020.L.V.,M.S.+2 种基金A.D.C.were supported by the European Union's Horizon 2020 Framework Program for funding Research and Innovation under grant agreement no.764047(ESPResSo)no.691664(UNIQUE,Cofund ERANET Action,MUR GA 775970)no.826013(IMPRESSIVE).C.C.and A.S.acknowledge MIUR Grant—Department of Excellence 2018-2022 and the European Union's Horizon 2020 Framework Program for funding Research and Innovation under grant agreement no.764047(ESPResSo).
文摘During the last decade,perovskite solar technologies underwent an impressive development,with power conversion efficiencies reaching 25.5%for single-junction devices and 29.8%for Silicon-Perovskite tandem configurations.Even though research mainly focused on improving the efficiency of perovskite photovoltaics(PV),stability and scalability remain fundamental aspects of a mature photovoltaics technology.For n-i-p structure perovskite solar cells,using poly-triaryl(amine)(PTAA)as hole transport layer(HTL)allowed to achieve marked improvements in device stability compared with other common hole conductors.For p-i-n structure,poly-triaryl(amine)is also routinely used as dopant-free hole transport layer,but problems in perovskite film growth,and its limited resistance to stress and imperfect batch-to-batch reproducibility,hamper its use for device upscaling.Following previous computational investigations,in this work,we report the synthesis of two small-molecule organic hole transport layers(BPT-1,2),aiming to solve the above-mentioned issues and allow upscale to the module level.By using BPT-1 and methylammonium-free perovskite,max.Power conversion efficiencies of 17.26%and 15.42%on a small area(0.09 cm^(2))and mini-module size(2.25 cm^(2)),respectively,were obtained,with a better reproducibility than with poly-triaryl(amine).Moreover,BPT-1 was demonstrated to yield more stable devices compared with poly-triaryl(amine)under ISOS-D1,T1,and L1 accelerated life-test protocols,reaching maximum T_(90)values>1000 h on all tests.
基金funding by the European Union–NextGenerationEU under the Italian Ministry of University and Research(MUR)National Innovation Ecosystem grant ECS00000041–VITALITY.
文摘The Buchwald-Hartwig coupling enables the grafting of nitrogen-containing functionalities onto molecules,facilitating the synthesis of a wide variety of molecular structures.However,several challenges impact the sustainability of this coupling.In our pursuit of a more sustainable Buchwald-Hartwig process,we report an optimized protocol that enhances energy efficiency and minimizes waste.Utilizing recoverable Pd/C as a catalyst,we performed the process in the bio-based solvent 2-MeTHF.To further boost energy efficiency,we employed microwave heating technology,resulting in improved overall process efficiency and reduced reaction times.This optimized approach allowed for the synthesis of a wide array of 17 variously functionalized arylamines.Thanks to the optimized workup procedure that facilitated the recovery and reuse of the catalyst,ligand,and 2-MeTHF,we achieved a reduced E-Factor ranging from 5.8 to 14.9,further contributing to the sustainability of the process.
基金the hpc@dbcf for providing computational resources and Regione Toscana for granting the Project INSIEME(Approcci di INtelligenza artificiale,Sintesi Innovative e valutazione di sostenibilitàEconomico-ambientale per lo sviluppo di nuovi Materiali per la conversione e stoccaggio dell’Energia solare)-Progetti di alta formazione-Fondo Sociale Europeo+2021-207(FSE+2021-2027).
文摘The excellent ability of dye-sensitized solar cells(DSSCs)to capture ambient light and convert it into electric current makes them attractive power sources for indoor applications,including powering Internet of Things(IoT)devices.In this context,substantial research efforts have been devoted to the discovery of novel organic dyes able to harvest energy from a wide range of indoor light sources at different intensities.However,such activities are often based on trial-and-error procedures which are frequently expensive and time-consuming.Here,Machine Learning(ML)techniques and Density Functional Theory(DFT)methods have been combined in a two-stage approach,with the aim to accelerate the design of new,synthetically accessible organic dyes for indoor DSSC applications.By predicting the power conversion efficiency(PCE)under different indoor light sources and intensities,potentially high-performance organic dyes have been identified.
文摘The self-assembling properties, stability, and dynamics of hybrid nanocarriers （gold nanoparticles （AuNPs） functionalized with cysteine-based peptides） in solution are studied through a series of classical molecular dynamics simulations based on a recently parametrized reactive force field. The results reveal, at the atomic level, all the details regarding the peptide adsorption mechanisms, nanoparticle stabilization, aggregation, and sintering. The data confirm and explain the experimental findings and disclose aspects that cannot be scrutinized by experiments. The biomolecules are both chemisorbed and physisorbed; self-interactions of the adsorbates and formation of stable networks of inter- connected molecules on the AuNP surfaces limit substrate reconstructions, protect the AuNPs from the action of the solvent, and prevent direct interactions of the gold surfaces. The possibility of agglomeration of the functionalized nanoparticles, compared with the sintering of the bare supports in a water solution, is demonstrated through relatively long simulations and fast steered dynamics. The analysis of the trajectories reveals that the AuNPs were well stabilized by the peptides. This prevented particle sintering and kept the particles far apart; however, part of their chains could form interconnections （crosslinks） between neighboring gold vehicles. The excellent agreement of these results with the literature confirm the reliability of the method and its potential application to the modeling of more complex materials relevant to the biomedical sector.
