N. Goujon, Jérémy Demarteau, Xabier Lopez de Pariza, N. Casado, H. Sardón, D. Mecerreyes
Over 30 million ton of poly(ethylene terephthalate) (PET) is produced each year and no more than 60% of all PET bottles are reclaimed for recycling due to material property deteriorations during the mechanical recycling process. Herein, a sustainable approach is proposed to produce redox-active nanoparticles via the chemical upcycling of poly(ethylene terephthalate) (PET) waste for application in energy storage. Redox-active nanoparticles of sizes lower than 100 nm were prepared by emulsion polymerization of a methacrylic-terephthalate monomer obtained by a simple methacrylate functionalization of the depolymerization product of PET (i.e., bis-hydroxy(2-ethyl) terephthalate, BHET). The initial cyclic voltammetry results of the depolymerization product of PET used as a model compound show a reversible redox process, when using a 0.1 M tetrabutylammonium hexafluorophosphate/dimethyl sulfoxide electrolyte system, with a standard redox potential of −2.12 V vs. Fc/Fc+. Finally, the cycling performance of terephthalate nanoparticles was investigated using a 0.1 M TBAPF6 solution in acetonitrile as electrolyte in a three-electrode cell. The terephthalate anode electrode displays good cycling stability and performance at high C-rate (i.e., ≥5C), delivering a stable specific discharge capacity of 32.8 mAh.g−1 at a C-rate of 30 C, with a capacity retention of 94% after 100 cycles. However, a large hysteresis between the specific discharge and charge capacities and capacity fading are observed at lower C-rate (i.e., ≤2C), suggesting some irreversibility of redox reactions associated with the terephthalate moiety, in particular related to the oxidation process.
每年生产超过3000万吨的聚对苯二甲酸乙酯(PET)，由于机械回收过程中材料性能的恶化，所有PET瓶的回收利用率不超过60%。本文提出了一种可持续的方法，通过化学升级回收聚对苯二甲酸乙酯(PET)废物来生产具有氧化还原活性的纳米颗粒，用于储能。通过对PET解聚产物(即双羟基(2-乙基)对苯二甲酸乙酯，BHET)进行简单的甲基丙烯酸酯功能化得到的甲基丙烯酸酯-对苯二甲酸乙酯单体进行乳液聚合，制备了尺寸小于100 nm的氧化还原活性纳米颗粒。当使用0.1 M四丁基六氟磷酸铵/二甲亚砜电解质体系，标准氧化还原电位为- 2.12 V vs. Fc/Fc+时，作为模型化合物的PET解聚产物的初始循环伏安法结果表明，其氧化还原过程是可逆的。最后，以0.1 M TBAPF6溶液为电解液，在三电极电池中研究了对苯二甲酸盐纳米颗粒的循环性能。对苯二甲酸盐阳极电极在高倍率(即≥5C)下具有良好的循环稳定性和性能，稳定的比放电容量为32.8 mAh。g−1在C率为30℃时，循环100次后容量保持率为94%。然而，在较低的c速率(即≤2C)下，观察到比放电和充电容量之间的大滞后和容量衰减，这表明与对苯二甲酸酯部分相关的氧化还原反应存在一些不可逆性，特别是与氧化过程有关。
{"title":"Chemical Upcycling of PET Waste towards Terephthalate Redox Nanoparticles for Energy Storage","authors":"N. Goujon, Jérémy Demarteau, Xabier Lopez de Pariza, N. Casado, H. Sardón, D. Mecerreyes","doi":"10.3390/suschem2040034","DOIUrl":"https://doi.org/10.3390/suschem2040034","url":null,"abstract":"Over 30 million ton of poly(ethylene terephthalate) (PET) is produced each year and no more than 60% of all PET bottles are reclaimed for recycling due to material property deteriorations during the mechanical recycling process. Herein, a sustainable approach is proposed to produce redox-active nanoparticles via the chemical upcycling of poly(ethylene terephthalate) (PET) waste for application in energy storage. Redox-active nanoparticles of sizes lower than 100 nm were prepared by emulsion polymerization of a methacrylic-terephthalate monomer obtained by a simple methacrylate functionalization of the depolymerization product of PET (i.e., bis-hydroxy(2-ethyl) terephthalate, BHET). The initial cyclic voltammetry results of the depolymerization product of PET used as a model compound show a reversible redox process, when using a 0.1 M tetrabutylammonium hexafluorophosphate/dimethyl sulfoxide electrolyte system, with a standard redox potential of −2.12 V vs. Fc/Fc+. Finally, the cycling performance of terephthalate nanoparticles was investigated using a 0.1 M TBAPF6 solution in acetonitrile as electrolyte in a three-electrode cell. The terephthalate anode electrode displays good cycling stability and performance at high C-rate (i.e., ≥5C), delivering a stable specific discharge capacity of 32.8 mAh.g−1 at a C-rate of 30 C, with a capacity retention of 94% after 100 cycles. However, a large hysteresis between the specific discharge and charge capacities and capacity fading are observed at lower C-rate (i.e., ≤2C), suggesting some irreversibility of redox reactions associated with the terephthalate moiety, in particular related to the oxidation process.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2021-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"78548888","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Brown carbon is a type of carbonaceous aerosol with strong light absorption in the ultraviolet and visible wavelengths that leads to radiative forcing. However, it is difficult to correlate the chemical composition of brown carbon with its atmospheric light absorption properties, which translates into significant uncertainty. Thus, a time-dependent density functional theory (TD-DFT) approach was used to model the real-world absorption properties of 14 polycyclic aromatic hydrocarbons (PAHs) over three regions of the Basque Country (Spain): Bilbao, Urretxu, and Azpeitia. The data were corrected for atmospheric concentration. The results show that the absorption spectra over each region are qualitatively identical, with the absorption intensities being significantly higher over Bilbao than over Azpeitia and Urretxu. Furthermore, it was found that the light absorption by PAHs should be more relevant for radiative forcing when it occurs at UVA and (sub)visible wavelengths. Finally, among the 14 studied PAHs, benzo[b]fluoranthene, pyrene, fluoranthene, benzo[a]pyrene, and benzo[k]fluoranthene and benzoperylene were identified as the molecules with larger contributions to radiative forcing.
{"title":"TD-DFT Monitoring of the Absorption Spectra of Polycyclic Aromatic Hydrocarbons over the Basque Country, Spain","authors":"P. González-Berdullas, Luís Pinto da Silva","doi":"10.3390/suschem2040033","DOIUrl":"https://doi.org/10.3390/suschem2040033","url":null,"abstract":"Brown carbon is a type of carbonaceous aerosol with strong light absorption in the ultraviolet and visible wavelengths that leads to radiative forcing. However, it is difficult to correlate the chemical composition of brown carbon with its atmospheric light absorption properties, which translates into significant uncertainty. Thus, a time-dependent density functional theory (TD-DFT) approach was used to model the real-world absorption properties of 14 polycyclic aromatic hydrocarbons (PAHs) over three regions of the Basque Country (Spain): Bilbao, Urretxu, and Azpeitia. The data were corrected for atmospheric concentration. The results show that the absorption spectra over each region are qualitatively identical, with the absorption intensities being significantly higher over Bilbao than over Azpeitia and Urretxu. Furthermore, it was found that the light absorption by PAHs should be more relevant for radiative forcing when it occurs at UVA and (sub)visible wavelengths. Finally, among the 14 studied PAHs, benzo[b]fluoranthene, pyrene, fluoranthene, benzo[a]pyrene, and benzo[k]fluoranthene and benzoperylene were identified as the molecules with larger contributions to radiative forcing.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2021-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"81996626","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Andromachi Tzani, Styliani Kalafateli, Grigorios Tatsis, Maria Bairaktari, Ioanna Kostopoulou, A. Pontillo, A. Detsi
The extraction of valuable phytochemicals from natural sources is an important and constantly evolving research area. Zingiber officinale Roscoe (ginger) contains high amounts of bioactive phytochemicals, which are desirable due to their significant properties. In this work, the ability of different natural deep eutectic solvents (NaDESs) to serve as green solvents for the preparation of high added value extracts from ginger is explored, in combination with ultrasound assisted extraction. The method was optimized by applying a response surface methodology using the NaDES Bet/La/W (1:2:2.5). Three independent variables, namely the extraction time, ultrasound power and NaDES-to-dry-ginger ratio, were investigated by employing a 17-run three-level Box–Behnken Design (BBD) in order to study the correlation between the extraction conditions and the quality of the obtained extracts. The optimum conditions (in order to achieve simultaneously maximum total phenolic content and antioxidant activity), were found to be 23.8 min extraction time, 60 Watt and NaDES/ginger 25:1 w/w. In the optimum conditions the DPPH radical scavenging ability of the extracts was found to reach IC50 = 18.16 mg/mL after 120 min, whereas the TPC was 20.10 ± 0.26 mg GAE/g of dry ginger. The green methodology was also compared with the extraction using conventional solvents. All the obtained extracts were evaluated for their antioxidant activity and their total phenolic content, while the extract derived by the optimum extraction conditions was further investigated for its ability to bind to calf thymus DNA (ctDNA).
{"title":"Natural Deep Eutectic Solvents (NaDESs) as Alternative Green Extraction Media for Ginger (Zingiber officinale Roscoe)","authors":"Andromachi Tzani, Styliani Kalafateli, Grigorios Tatsis, Maria Bairaktari, Ioanna Kostopoulou, A. Pontillo, A. Detsi","doi":"10.3390/suschem2040032","DOIUrl":"https://doi.org/10.3390/suschem2040032","url":null,"abstract":"The extraction of valuable phytochemicals from natural sources is an important and constantly evolving research area. Zingiber officinale Roscoe (ginger) contains high amounts of bioactive phytochemicals, which are desirable due to their significant properties. In this work, the ability of different natural deep eutectic solvents (NaDESs) to serve as green solvents for the preparation of high added value extracts from ginger is explored, in combination with ultrasound assisted extraction. The method was optimized by applying a response surface methodology using the NaDES Bet/La/W (1:2:2.5). Three independent variables, namely the extraction time, ultrasound power and NaDES-to-dry-ginger ratio, were investigated by employing a 17-run three-level Box–Behnken Design (BBD) in order to study the correlation between the extraction conditions and the quality of the obtained extracts. The optimum conditions (in order to achieve simultaneously maximum total phenolic content and antioxidant activity), were found to be 23.8 min extraction time, 60 Watt and NaDES/ginger 25:1 w/w. In the optimum conditions the DPPH radical scavenging ability of the extracts was found to reach IC50 = 18.16 mg/mL after 120 min, whereas the TPC was 20.10 ± 0.26 mg GAE/g of dry ginger. The green methodology was also compared with the extraction using conventional solvents. All the obtained extracts were evaluated for their antioxidant activity and their total phenolic content, while the extract derived by the optimum extraction conditions was further investigated for its ability to bind to calf thymus DNA (ctDNA).","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2021-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"87813968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Amanda Jalihal, T. Le, Samantha Macchi, Hannah Krehbiel, Mujeebat Bashiru, Mavis Forson, Noureen Siraj
Herein, an ionic material (IM) with Förster Resonance Energy Transfer (FRET) characteristics is reported for the first time. The IM is designed by pairing a Nile Blue A cation (NBA+) with an anionic near-infrared (NIR) dye, IR820−, using a facile ion exchange reaction. These two dyes absorb at different wavelength regions. In addition, NBA+ fluorescence emission spectrum overlaps with IR820− absorption spectrum, which is one requirement for the occurrence of the FRET phenomenon. Therefore, the photophysical properties of the IM were studied in detail to investigate the FRET mechanism in IM for potential dye sensitized solar cell (DSSCs) application. Detailed examination of photophysical properties of parent compounds, a mixture of the parent compounds, and the IM revealed that the IM exhibits FRET characteristics, but not the mixture of two dyes. The presence of spectator counterion in the mixture hindered the FRET mechanism while in the IM, both dyes are in close proximity as an ion pair, thus exhibiting FRET. All FRET parameters such as spectral overlap integral, Förster distance, and FRET energy confirm the FRET characteristics of the IM. This article presents a simple synthesis of a compound with FRET properties which can be further used for a variety of applications.
{"title":"Understanding of Förster Resonance Energy Transfer (FRET) in Ionic Materials","authors":"Amanda Jalihal, T. Le, Samantha Macchi, Hannah Krehbiel, Mujeebat Bashiru, Mavis Forson, Noureen Siraj","doi":"10.3390/suschem2040031","DOIUrl":"https://doi.org/10.3390/suschem2040031","url":null,"abstract":"Herein, an ionic material (IM) with Förster Resonance Energy Transfer (FRET) characteristics is reported for the first time. The IM is designed by pairing a Nile Blue A cation (NBA+) with an anionic near-infrared (NIR) dye, IR820−, using a facile ion exchange reaction. These two dyes absorb at different wavelength regions. In addition, NBA+ fluorescence emission spectrum overlaps with IR820− absorption spectrum, which is one requirement for the occurrence of the FRET phenomenon. Therefore, the photophysical properties of the IM were studied in detail to investigate the FRET mechanism in IM for potential dye sensitized solar cell (DSSCs) application. Detailed examination of photophysical properties of parent compounds, a mixture of the parent compounds, and the IM revealed that the IM exhibits FRET characteristics, but not the mixture of two dyes. The presence of spectator counterion in the mixture hindered the FRET mechanism while in the IM, both dyes are in close proximity as an ion pair, thus exhibiting FRET. All FRET parameters such as spectral overlap integral, Förster distance, and FRET energy confirm the FRET characteristics of the IM. This article presents a simple synthesis of a compound with FRET properties which can be further used for a variety of applications.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2021-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"75200301","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kalani Periyapperuma, Laura Sanchez-Cupido, J. Pringle, C. Pozo‐Gonzalo
Neodymium (Nd) is one of the most essential rare-earth metals due to its outstanding properties and crucial role in green energy technologies such as wind turbines and electric vehicles. Some of the key uses includes permanent magnets present in technological applications such as mobile phones and hard disk drives, and in nickel metal hydride batteries. Nd demand is continually growing, but reserves are severely limited, which has put its continued availability at risk. Nd recovery from end-of-life products is one of the most interesting ways to tackle the availability challenge. This perspective concentrates on the different methods to recover Nd from permanent magnets and rechargeable batteries, covering the most developed processes, hydrometallurgy and pyrometallurgy, and with a special focus on electrodeposition using highly electrochemical stable media (e.g., ionic liquids). Among all the ionic liquid chemistries, only phosphonium ionic liquids have been studied in-depth, exploring the impact of temperature, electrodeposition potential, salt concentration, additives (e.g., water) and solvation on the electrodeposition quality and quantity. Finally, the importance of investigating new ionic liquid chemistries, as well as the effect of other metal impurities in the ionic liquid on the deposit composition or the stability of the ionic liquids are discussed. This points to important directions for future work in the field to achieve the important goal of efficient and selective Nd recovery to overcome the increasingly critical supply problems.
{"title":"Analysis of Sustainable Methods to Recover Neodymium","authors":"Kalani Periyapperuma, Laura Sanchez-Cupido, J. Pringle, C. Pozo‐Gonzalo","doi":"10.3390/suschem2030030","DOIUrl":"https://doi.org/10.3390/suschem2030030","url":null,"abstract":"Neodymium (Nd) is one of the most essential rare-earth metals due to its outstanding properties and crucial role in green energy technologies such as wind turbines and electric vehicles. Some of the key uses includes permanent magnets present in technological applications such as mobile phones and hard disk drives, and in nickel metal hydride batteries. Nd demand is continually growing, but reserves are severely limited, which has put its continued availability at risk. Nd recovery from end-of-life products is one of the most interesting ways to tackle the availability challenge. This perspective concentrates on the different methods to recover Nd from permanent magnets and rechargeable batteries, covering the most developed processes, hydrometallurgy and pyrometallurgy, and with a special focus on electrodeposition using highly electrochemical stable media (e.g., ionic liquids). Among all the ionic liquid chemistries, only phosphonium ionic liquids have been studied in-depth, exploring the impact of temperature, electrodeposition potential, salt concentration, additives (e.g., water) and solvation on the electrodeposition quality and quantity. Finally, the importance of investigating new ionic liquid chemistries, as well as the effect of other metal impurities in the ionic liquid on the deposit composition or the stability of the ionic liquids are discussed. This points to important directions for future work in the field to achieve the important goal of efficient and selective Nd recovery to overcome the increasingly critical supply problems.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2021-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"77314075","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The concomitant hydrolysis and dehydration of biomass-derived cellulose and hemicellulose to furfural (FUR) and 5-(hydroxymethyl)furfural (HMF) under acid catalysis allows a dramatic reduction in the oxygen content of the parent sugar molecules with a 100% carbon economy. However, most applications of FUR or HMF necessitate synthetic modifications. Catalytic hydrogenation and hydrogenolysis have been recognized as efficient strategies for the selective deoxygenation and energy densification of biomass-derived furfurals generating water as the sole byproduct. Efficient and eco-friendly catalysts have been developed for the selective hydrogenation of furfurals affording renewable furanic compounds such as 2-methylfuran, 2,5-dimethylfuran and 2-methyltetrahydrofuran with potential applications as biofuel, solvent and chemical feedstock. Hydrogen gas or hydrogen donor molecules, required for the above processes, can also be renewably obtained from biomass using catalytic processes, enabling a circular economy. In this review, the recent developments in the energy densification of furfurals to furanic compounds of commercial significance are elaborated, emphasizing the role of catalyst and the reaction parameters employed. Critical discussion on sourcing hydrogen gas required for the processes, using hydrogen donor solvents, catalyst design and the potential markets of furanic intermediates have been made. Critical evaluations of the accomplishments and challenges in this field are also provided.
{"title":"Energy Densification of Biomass-Derived Furfurals to Furanic Biofuels by Catalytic Hydrogenation and Hydrodeoxygenation Reactions","authors":"Nivedha Vinod, S. Dutta","doi":"10.3390/suschem2030029","DOIUrl":"https://doi.org/10.3390/suschem2030029","url":null,"abstract":"The concomitant hydrolysis and dehydration of biomass-derived cellulose and hemicellulose to furfural (FUR) and 5-(hydroxymethyl)furfural (HMF) under acid catalysis allows a dramatic reduction in the oxygen content of the parent sugar molecules with a 100% carbon economy. However, most applications of FUR or HMF necessitate synthetic modifications. Catalytic hydrogenation and hydrogenolysis have been recognized as efficient strategies for the selective deoxygenation and energy densification of biomass-derived furfurals generating water as the sole byproduct. Efficient and eco-friendly catalysts have been developed for the selective hydrogenation of furfurals affording renewable furanic compounds such as 2-methylfuran, 2,5-dimethylfuran and 2-methyltetrahydrofuran with potential applications as biofuel, solvent and chemical feedstock. Hydrogen gas or hydrogen donor molecules, required for the above processes, can also be renewably obtained from biomass using catalytic processes, enabling a circular economy. In this review, the recent developments in the energy densification of furfurals to furanic compounds of commercial significance are elaborated, emphasizing the role of catalyst and the reaction parameters employed. Critical discussion on sourcing hydrogen gas required for the processes, using hydrogen donor solvents, catalyst design and the potential markets of furanic intermediates have been made. Critical evaluations of the accomplishments and challenges in this field are also provided.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2021-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"86411950","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Thuy Le, Y. Khan, N. Speller, Mujeebat Bashiru, Samantha Macchi, I. Warner, Noureen Siraj
Herein, an inexpensive commercially available sensor is presented for the detection of 4-nitrophenol (4NP) pollutant. Sodium fluorescein (NaFl) is used as a sensor to detect trace amounts of 4NP in acetonitrile (MeCN). The photophysical properties of NaFl were studied in two different solvents, MeCN (aprotic) and water (protic), with varying concentrations of different nitroaromatics using UV-visible absorption and fluorescence spectrophotometry. In an aqueous medium, photophysical properties of NaFl did not change in the presence of nitroaromatics. However, examination of the photodynamics in MeCN demonstrated that NaFl is extremely sensitive to 4NP (limit of detection: 0.29 µg/mL). This extreme specificity of NaFl towards 4NP when dissolved in MeCN, as compared to other nitroaromatics, is attributed to hydrogen bonding of 4NP with NaFl in the absence of water, resulting in both static and dynamic quenching processes. Thus, NaFl is demonstrated as a simple, inexpensive, sensitive, and robust optical turn off sensor for 4NP.
{"title":"A Highly Selective Economical Sensor for 4-Nitrophenol","authors":"Thuy Le, Y. Khan, N. Speller, Mujeebat Bashiru, Samantha Macchi, I. Warner, Noureen Siraj","doi":"10.3390/suschem2030028","DOIUrl":"https://doi.org/10.3390/suschem2030028","url":null,"abstract":"Herein, an inexpensive commercially available sensor is presented for the detection of 4-nitrophenol (4NP) pollutant. Sodium fluorescein (NaFl) is used as a sensor to detect trace amounts of 4NP in acetonitrile (MeCN). The photophysical properties of NaFl were studied in two different solvents, MeCN (aprotic) and water (protic), with varying concentrations of different nitroaromatics using UV-visible absorption and fluorescence spectrophotometry. In an aqueous medium, photophysical properties of NaFl did not change in the presence of nitroaromatics. However, examination of the photodynamics in MeCN demonstrated that NaFl is extremely sensitive to 4NP (limit of detection: 0.29 µg/mL). This extreme specificity of NaFl towards 4NP when dissolved in MeCN, as compared to other nitroaromatics, is attributed to hydrogen bonding of 4NP with NaFl in the absence of water, resulting in both static and dynamic quenching processes. Thus, NaFl is demonstrated as a simple, inexpensive, sensitive, and robust optical turn off sensor for 4NP.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2021-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"81018301","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mattia Annatelli, Giacomo Trapasso, Lucrezia Lena, F. Aricò
Commercially available Purolite CT151 demonstrated to be an efficient acid catalyst for the synthesis of alkyl levulinates via alcoholysis of furfuryl alcohol (FA) at mild temperatures (80–120 °C) and short reaction time (5 h). Reaction conditions were first optimized for the synthesis of ethyl levulinate and then tested for the preparation of methyl-, propyl-, isopropyl-, butyl, sec-butyl- and allyl levulinate. Preliminary scale-up tests were carried out for most of the alkyl levulinates (starting from 5.0 g of FA) and the resulting products were isolated as pure by distillation in good yields (up to 63%). Furthermore, recycling experiments, conducted for the preparation of ethyl levulinate, showed that both the Purolite CT151 and the exceeding ethanol can be recovered and reused for four consecutive runs without any noticeable loss in the catalyst activity.
市购Purolite CT151是糠醛醇醇解合成乙酰丙酸烷基酯的高效酸催化剂，反应温度较低(80-120℃)，反应时间较短(5 h)。首先优化了乙酰丙酸乙酯的合成条件，然后测试了甲基-、丙基-、异丙基-、丁基、中丁基-和乙酰丙酸烯丙酯的制备条件。对大多数乙酰丙酸烷基酯(从5.0 g FA开始)进行了初步的放大试验，所得产品通过蒸馏分离为纯产品，收率很高(高达63%)。此外，对制备乙酰丙酸乙酯的回收实验表明，Purolite CT151和多余的乙醇都可以连续四次回收再利用，而催化剂活性没有明显损失。
{"title":"Alkyl Levulinates from Furfuryl Alcohol Using CT151 Purolite as Heterogenous Catalyst: Optimization, Purification, and Recycling","authors":"Mattia Annatelli, Giacomo Trapasso, Lucrezia Lena, F. Aricò","doi":"10.3390/suschem2030027","DOIUrl":"https://doi.org/10.3390/suschem2030027","url":null,"abstract":"Commercially available Purolite CT151 demonstrated to be an efficient acid catalyst for the synthesis of alkyl levulinates via alcoholysis of furfuryl alcohol (FA) at mild temperatures (80–120 °C) and short reaction time (5 h). Reaction conditions were first optimized for the synthesis of ethyl levulinate and then tested for the preparation of methyl-, propyl-, isopropyl-, butyl, sec-butyl- and allyl levulinate. Preliminary scale-up tests were carried out for most of the alkyl levulinates (starting from 5.0 g of FA) and the resulting products were isolated as pure by distillation in good yields (up to 63%). Furthermore, recycling experiments, conducted for the preparation of ethyl levulinate, showed that both the Purolite CT151 and the exceeding ethanol can be recovered and reused for four consecutive runs without any noticeable loss in the catalyst activity.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2021-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"79710449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Marta E. G. Mosquera, Gerardo Jiménez, Vanessa Tabernero, Joan Vinueza-Vaca, C. García-Estrada, K. Kosalková, Alberto Sola-Landa, Belén Monje, C. Acosta, Rafael Alonso, Miguel Ángel Valera
Polymers are essential materials in our daily life. The synthesis of value-added polymers is mainly performed from fossil fuel-derived monomers. However, the adoption of the circular economy model based on the bioeconomy will reduce the dependence on fossil fuels. In this context, biorefineries have emerged to convert biomass into bioenergy and produce high value-added products, including molecules that can be further used as building blocks for the synthesis of biopolymers and bioplastics. The achievement of catalytic systems able to polymerize the natural monomer counterparts, such as terpenes or terpenoids, is still a challenge in the development of polymers with good mechanical, thermal, and chemical properties. This review describes the most common types of bioplastics and biopolymers and focuses specifically on the polymerization of terpenes and terpenoids, which represent a source of promising monomers to create bio-based polymers and copolymers.
{"title":"Terpenes and Terpenoids: Building Blocks to Produce Biopolymers","authors":"Marta E. G. Mosquera, Gerardo Jiménez, Vanessa Tabernero, Joan Vinueza-Vaca, C. García-Estrada, K. Kosalková, Alberto Sola-Landa, Belén Monje, C. Acosta, Rafael Alonso, Miguel Ángel Valera","doi":"10.3390/suschem2030026","DOIUrl":"https://doi.org/10.3390/suschem2030026","url":null,"abstract":"Polymers are essential materials in our daily life. The synthesis of value-added polymers is mainly performed from fossil fuel-derived monomers. However, the adoption of the circular economy model based on the bioeconomy will reduce the dependence on fossil fuels. In this context, biorefineries have emerged to convert biomass into bioenergy and produce high value-added products, including molecules that can be further used as building blocks for the synthesis of biopolymers and bioplastics. The achievement of catalytic systems able to polymerize the natural monomer counterparts, such as terpenes or terpenoids, is still a challenge in the development of polymers with good mechanical, thermal, and chemical properties. This review describes the most common types of bioplastics and biopolymers and focuses specifically on the polymerization of terpenes and terpenoids, which represent a source of promising monomers to create bio-based polymers and copolymers.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2021-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"77476475","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
By tradition, herbal infusions have been mainly consumed for their pleasant taste, but, nowadays, the consumer, along with the pleasantness of drinking a savory beverage, also looks for their health benefits. Grapes and grape/wine by-products are a rich source of health-promoting compounds, presenting great potential for the development of new beverages. Moreover, grape-infusion preparation is no more than a sustainable or green way of extracting polyphenols and other nutraceutical compounds from grapes and grape leaves. In this review, we summarize the benefits of drinking grape infusions and discuss the sustainable processes of extracting potential nutraceutical compounds from grapes and grape by-products, which are often considered fermentation waste and are discarded to the environment without proper treatment.
{"title":"Grape Infusions: Between Nutraceutical and Green Chemistry","authors":"A. Vilela, T. Pinto","doi":"10.3390/suschem2030025","DOIUrl":"https://doi.org/10.3390/suschem2030025","url":null,"abstract":"By tradition, herbal infusions have been mainly consumed for their pleasant taste, but, nowadays, the consumer, along with the pleasantness of drinking a savory beverage, also looks for their health benefits. Grapes and grape/wine by-products are a rich source of health-promoting compounds, presenting great potential for the development of new beverages. Moreover, grape-infusion preparation is no more than a sustainable or green way of extracting polyphenols and other nutraceutical compounds from grapes and grape leaves. In this review, we summarize the benefits of drinking grape infusions and discuss the sustainable processes of extracting potential nutraceutical compounds from grapes and grape by-products, which are often considered fermentation waste and are discarded to the environment without proper treatment.","PeriodicalId":22103,"journal":{"name":"Sustainable Chemistry","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2021-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"84027818","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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