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green solvent-based approaches for synthesis of nanomaterials

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Science China Chemistry 2010年第2期53卷 372-382页

作者： LIU ZhiMin SUN ZhenYu Beijing National Laboratory for Molecular Sciences Center for Molecular ScienceInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

The use of green solvents (including supercritical fluids and ionic liquids) in the synthesis of nanomaterials is highlighted. The methods described can not only reduce or eliminate the use or generation of substances hazardous to health and the environment, but can also be used to efficiently prepare nanomaterials with high performances. The unique characteristics of green solvents are responsible for the green features and unusual advantages of these approaches.

关键词： green solvent supercritical fluid ionic liquid nanomaterial synthesis

Investigating TEP as a greener alternative to NMP in Ni-rich cathode fabrication

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Journal of Energy Chemistry 2023年第3期78卷 240-245,I0007页

作者： Changlong Chen Vignyatha Reddy Tatagari Hao Lin Leon Shaw Department of Mechanical Materials and Aerospace EngineeringIllinois Institute of TechnologyChicagoIL 60616United States Department of Chemistry Illinois Institute of TechnologyChicagoIL 60616United States

In the past decade,the surging demand for portable electronics,electric vehicles,and stationary energy storage grids has triggered a noticeable rise in the production of Li-ion batteries(LIBs).However,this swift rise is now hindered by relying on the use of N-methyl-2-pyrrolidone(NMP),a repro-toxic solvent,in the current cathode processing of LIBs.To overcome this challenge,here we have investigated triethyl phosphate(TEP) as a greener alternative to NMP.The compatibility with polyvinylidene fluoride(PVDF)binder,the slurry rheology,the electrode morphology and cell performance with Ni-rich cathodes are characterized.The results show that TEP-based samples possess indistinguishable characteristics in all as pects studied when compared with NMP,revealing that TEP is a promising substitute for NMP in processing Ni-rich cathodes.It is anticipated that this green solvent,TEP,will draw attention from industry in the real-world LIB application in the future.

关键词： Triethyl phosphate Li-ion batteries green solvent Electrode fabrication NMC622

Oriented Organization of Poly(3-Hexylthiophene)for Efficient and Stable Antimony Sulfide Solar Cells

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Energy & Environmental Materials 2023年第6期6卷 312-317页

作者： Jinxiang Gao Rongfeng Tang Huiling Cai Zhiyuan Cai Peng Xiao Gang Li Chenhui Jiang Changfei Zhu Tao Chen CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and EngineeringSchool of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei 230041China Institute of Energy Hefei Comprehensive National Science CenterHefei 230041China

Poly(3-hexylthiophene)(P3HT),as a traditional organic hole-transporting material(HTM),is widely used in thin-film solar cells due to its high charge mobility and good thermal stability.However,the P3HT films obtained by the traditional method are amorphous,which is unfavorable to hole extraction and transport.Here,a low-toxicity solvent 1,2,4-trimethylbenzene(TMB)was used as the solvent instead of the commonly used halogen solvent chlorobenzene(CB)to dissolve P3HT.Thus,the self-assembled nanofibrous P3HT film was prepared and applied as HTM in the newly emerged Sb_(2)S_(3)solar cells.According to the density functional theory calculations,the interface contact between TMB-P3HT and Sb_(2)S_(3)was enhanced via the bonding interaction of S in P3HT and Sb in Sb_(2)S_(3).Through transient absorption spectroscopy characterization,the enhanced interface contact improves the charge extraction ability of TMB-P3HT when compared to the CB-P3HT film.Thus,the TMB-P3HT-based Sb_(2)S_(3)solar cell delivers a power conversion efficiency of 6.21%,which is 9.7%higher than that of the CB-P3HT-based device.Furthermore,the dopant-free TMB-P3HT-based Sb_(2)S_(3)devices exhibit excellent environmental stability compared with Spiro-OMeTAD-based devices.This work demonstrates that the application of P3HT and the solvent engineering of HTM are applicable strategies for developing Sb_(2)S_(3)solar cells with high efficiency and stability.

关键词： green solvent P3HT Sb_(2)S_(3) self-assembled nanofibrous solar cell

3-Methylcyclohexanone Processed n-Channel Organic Thin-Film Transistors Based on a Conjugated Polymer Synthesized by Direct Arylation Polycondensation

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Chinese Journal of Polymer Science 2023年第5期41卷 824-831,I0012页

作者： Dong-Sheng Yan Xu-Wen Zhang Zhong-Li Wang Chen-Hui Xu Yi-Bo Shi Yun-Feng Deng Yang Han Yan-Hou Geng School of Materials Science and Engineering and Tianjin Key Laboratory of Molecular Optoelectronic Science Tianjin Universityand Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin 300072China State Key Laboratory of Separation Membranes and Membrane Processes Tianjin Key Laboratory of Advanced Fibers and Energy StorageSchool of Material Science and EngineeringTiangong UniversityTianjin 300387China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China

The solubility of a direct arylation polycondensation(DArP)synthesized conjugated polymer,i.e.,poly(3,6-bis(furan-2-yl)-2,5-bis(4-tetradecyloctadecyl)-pyrrolo[3,4-c]pyrrole-1,4(2H,5H)-dione-alt-1,2-bis(3,4-d ifl uorothien-2-yl)ethene)(PFuD PP-4FTVT),in variou s organic solvents was studied.The polymer is soluble in 3-methylcyclohexanone(3-MC),a green solvent from peppermint oil,besides other solvents such as anisole,cyclopentyl methyl ether(CPME)and o-dichlorobenzene(o-DCB),etc.Based on the Hansen solu bility parameters(HSP)analysis,3-MC is identified as a"marginal solvent"of PFuDPP-4FTVT.The morphology of the spin-coated films with 3-MC as the solvent strongly correlated with the solution preparation conditions.With a 3-MC solution aged for 3 h at 70℃,n-channel organic thin-film transistors(OTFTs)with electron mobility(μe)above 1 cm^(2)·V^(-1)·s^(-1) and current on/off ratio(Ion/Ioff)higher than 105 were fabricated by spin-coating.This is the first report on high mobility conjugated polymers for OTFTs processible with natu rally occurred green solvent.

关键词： Conjugated polymers Organic thin-film transistors Electron mobility green solvent Direct arylation polycondensation

Alkyl side chain engineering enables high performance as-cast organic solar cells of over 17%efficiency

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Fundamental Research 2023年第4期3卷 611-617页

作者： Xiang Xu Yazhou Qi Xiaoyan Luo Xinxin Xia Xinhui Lu Jun Yuan Yonghua Zhou Yingping Zou State Key Laboratory of Powder Metallurgy College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China Department of Physics The Chinese University of Hong KongNew TerritoriesHong Kong 999077China

Achieving high-performance as-cast OSCs is crucial for industrialization in the future,owing to the advantages of better stability,environmental-friendly,and decreasing production cost.In this regard,we synthesized an ADA′D-A type acceptor,Y6-eC6-BO,by shortening the straight alkyl side-chains on the thiophene position from C_(11) to C_(6) as well as lengthening the branched alkyl side-chains on the pyrrole position of Y6 to achieve a stronger crystallization and better miscibility than Y6.As a result,the corresponding chloroform-processed as-cast PM6:Y6-eC6-BO OSC showed a high PCE of 17.33%,which was one of the highest efficiencies of as-cast OSCs.And the as-cast PM6:Y6-eC6-BO OSCs processed from o-xylene displayed a PCE of 16.38%,as far as we know,this is among the highest efficiencies of non-halogenated-solvent processed as-cast OSCs.These results demonstrated tailoring the alkyl side-chain of NFAs is a feasible and simple approach to achieve high performance as-cast OSCs and provides guideline in molecular design in the future.

关键词： Organic solar cells Alkyl side chains As-cast green solvent Stability

green Anti-solvent Processed Efficient Flexible Perovskite Solar Cells

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Green Anti-solvent Processed Efficient Flexible Perovskite S...

High-gravity-assisted green synthesis of rare-earth doped calcium molybdate colloidal nanophosphors

第六届新型太阳能电池材料科学与技术学术研讨会

作者：辛德雨王增华张敏郑霄家秦勇朱建国张文华中国工程物理研究院化学材料研究所四川新材料研究中心四川大学材料科学系兰州大学物理科学与技术学院纳米科学与纳米技术研究所

Flexible perovskite solar cells(PSCs) possess compatible features with low-cost, high throughput production approaches, showing great potentials in wearable, portable, flyable, and deployable applications. However, flexible PSCs with superior efficiency are commonly fabricated with an anti-solvent assisted crystallization(ASAC) method, which uses highly toxic solvents as the processed solvents. In this work, we use environmentally benign anti-solvents for the fabrication of flexible PSCs.Benefiting from the low-temperature solution processability of a high quality SnO2 electron transport layer(ETL) with superior electron extraction and transfer features, flexible PSCs show an impressive PCE over 17% under reverse scan. This, to the best of our knowledge, is among the highest performances for flexible PSCs and is the first report for flexible PSCs fabricated by green anti-solvent processed techniques. These results provide new opportunities for environmental-friendly manufacturing of high performance flexible PSCs.

关键词： green solvent Flexible Perovskite solar cell Charge recombination tert-Butanol

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Chinese Journal of Chemical Engineering 2020年第6期28卷 1744-1751页

作者： Yuan Pu Lifeng Lin Jun Liu Jiexin Wang Dan Wang State Key Laboratory of Organic Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Research Center of the Ministry of Education for High Gravity Engineering and Technology Beijing University of Chemical TechnologyBeijing 100029China

In this work,we report an innovative route for the synthesis of rare-earth doped calcium molybdate(CaMoO4)nanophosphors by using high gravity rotating packed bed(RPB)technology and paraffin liquid as the solvent.The significant intensified mass transfer and micromixing of reactants in the RPB reactor are benefiting for homogeneous doping of rare-earth ions in the host materials,leading to nanophosphors with high quantum efficiency.The use of liquid paraffin as the solvent eliminates the safety risks associated with volatile organic compounds,increasing the potential for clean production of nanophosphors.Under excitation of deep ultraviolet(DUV)light,the CaMoO4:Na+,Eu3+nanophosphors exhibit red emission at peak wavelength of 615 nm and quantum yield of up to 35.01%.The CaMoO4:Na+,Tb3+nanophosphors exhibit green emission at peak wavelength of543 nm with quantum yield of up to 30.66%.The morphologies of the nanophosphors are tunable from nanofibers through nanorods to nanodots and the possible mechanism of controlling the formation of different nanostructures is proposed on the basis of experimental results and theoretical analysis of mesoscience.These nanophosphors are highly dispersible in organic solvents and utilized for fabricating fabrication of flexible,freestanding luminescent films based on silicone resin.We also demonstrate the red LEDs consisting of the hybrid films of CaMoO4:Na+,Eu3+nanoparticles as color-converting phosphors and DUV LEDs as illuminators,offering strong potential for future nanophosphors-basedsolid-state lighting systems.

关键词： Colloidal nanophosphors CaMoO4 Process intensification High gravity technology green solvent

The application of clean production in organic synthesis

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Chinese Chemical Letters 2021年第5期32卷 1637-1644页

作者： Jun Jiang Fang Xiao Wei-Min He Leyong Wang School of Chemistry and Chemical Engineering University of South ChinaHengyang 421001China Xiangya School of Public Health Central South UniversityChangsha 410078China Key Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Clean production,as an important part of green chemistry,has received great attention and considerable development in recent years.In this perspective article,we summarized some examples of(nearly)quantitative synthesis,clean separation and purification to emphasize clean production.These reactions were carried out by using eco-friendly solvents and the pure products could be easily obtained through clean procedures.

关键词： green chemistry green solvent Water solvent free Purification

Impact of solvents and surfactants on the self-assembly of nanostructured amine functionalized silica spheres for CO_(2) capture

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Journal of Energy Chemistry 2016年第2期25卷 325-333页

作者： Edith Berger Maximilian W.Hahn Thomas Przybilla Benjamin Winter Erdmann Spiecker Andreas Jentys Johannes A.Lercher Department of Chemistry and Catalysis Research Center Technische Universitat Munchen Lichtenbergstraβe 485747 GarchingGermany Center for Nanoanalysis and Electron Microscopy(CENEM)&Institute of Micro-and Nanostructure Research Friedrich-Alexander-Universitat Erlangen-NurnbergCauerstraβe 691058 ErlangenGermany

Macroscopic SiO2 spheres with a homogeneous amine distribution were synthesized by a one-step emulsion based synthesis approach in a flow column reactor. The CO2 adsorption capacity of the nanostructured amine-functionalized silica spheres was studied in absence and presence of H2O. The structural properties were adjusted by varying solvents and surfactants during the synthesis and, at constant amine loadings, were found to be the main factor for influencing the CO2 sorption capacities. Under water-free conditions CO2 is bound to the amino groups via the formation of carbamates, which require two neighboring amino groups to adsorb one CO2 molecule. At constant amine concentrations sorbents with lower surface area allow to establish a higher amine density on the surface, which enhances the CO2 uptake capacities under dry conditions. In presence of H2O the CO2 adsorption changes to 1：1 stoichiometry due to stabilization of carbamates by protonation of H2O and formation of further species such as bicarbonates, which should in principle double the adsorption capacities. Low concentrations of physisorbed H2O（0.3 mmol/g） did not impair the adsorption capacity of the adsorbents for CO2, while at higher water uptakes（0.6 and 1.1 mmol/g） the CO2 uptake is reduced, which could be attributed to capillary condensation of H2O or formation of bulky reaction products blocking inner pores and access to active sites.

关键词： Carbon dioxide Amines green solvent Surfactant Water(H2O) Carbamate Bicarbonate