Fumarate, an unsaturated dicarboxylic acid, is an important material for producing unsaturated polyester resins and biodegradable plastics. Fumarate synthesis from petroleum-derived benzene and butane as starting materials is expected to be replaced by synthesis methods from renewable raw materials. In this work, fumarate synthesis from gaseous CO2 and pyruvate in an aqueous medium using a multi-biocatalytic system consisting of pyruvate carboxylase (PC), malate dehydrogenase (MDH) and fumarase (FUM) in the presence of ATP and NADH is accomplished. The conversion yield of fumarate from pyruvate using this system was estimated to be approximately 16% after 5 h of incubation.
不饱和二羧酸富马酸盐是生产不饱和聚酯树脂和生物降解塑料的重要原料。以源自石油的苯和丁烷为起始原料合成的富马酸有望被可再生原料合成法所取代。本研究利用由丙酮酸羧化酶(PC)、苹果酸脱氢酶(MDH)和富马酸酶(FUM)组成的多重生物催化系统,在 ATP 和 NADH 的存在下,在水介质中从气态 CO2 和丙酮酸合成富马酸。据估计,在培养 5 小时后,使用该系统将丙酮酸转化为富马酸的转化率约为 16%。
{"title":"A multi-biocatalytic system for effective fumarate synthesis from pyruvate and gaseous CO2†","authors":"Mika Takeuchi and Yutaka Amao","doi":"10.1039/D3SU00486D","DOIUrl":"10.1039/D3SU00486D","url":null,"abstract":"<p >Fumarate, an unsaturated dicarboxylic acid, is an important material for producing unsaturated polyester resins and biodegradable plastics. Fumarate synthesis from petroleum-derived benzene and butane as starting materials is expected to be replaced by synthesis methods from renewable raw materials. In this work, fumarate synthesis from gaseous CO<small><sub>2</sub></small> and pyruvate in an aqueous medium using a multi-biocatalytic system consisting of pyruvate carboxylase (PC), malate dehydrogenase (MDH) and fumarase (FUM) in the presence of ATP and NADH is accomplished. The conversion yield of fumarate from pyruvate using this system was estimated to be approximately 16% after 5 h of incubation.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d3su00486d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141743263","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Doubly decarboxylative coupling between two different carboxylic acids to form a new C–C bond is a powerful tool for the rapid assembly of complex compounds. Herein, we report a metal-free three-component decarboxylative strategy for the construction of diverse propargylamines in good yields with high chemoselectivity. This operationally simple method can be applied to various amino acids, α-keto acids, and terminal alkynes, providing a powerful new protocol for propargylamine synthesis. The reaction without the addition of metal catalysts has the advantages of broad scope and functional group compatibility, and environmental friendliness.
{"title":"Facile synthesis of propargylamines by metal-free doubly decarboxylative coupling†","authors":"Junduo Hu, Xiaofan Shi, Liliang Huang, Rongkang Zhang and Huangdi Feng","doi":"10.1039/D4SU00258J","DOIUrl":"10.1039/D4SU00258J","url":null,"abstract":"<p >Doubly decarboxylative coupling between two different carboxylic acids to form a new C–C bond is a powerful tool for the rapid assembly of complex compounds. Herein, we report a metal-free three-component decarboxylative strategy for the construction of diverse propargylamines in good yields with high chemoselectivity. This operationally simple method can be applied to various amino acids, α-keto acids, and terminal alkynes, providing a powerful new protocol for propargylamine synthesis. The reaction without the addition of metal catalysts has the advantages of broad scope and functional group compatibility, and environmental friendliness.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00258j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141743267","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jake G. Tillou, Joseph J. Kuchta, Nathan Thornburg, Santosh K. Balijepalli and Aaron K. Vannucci
The selective hydrodeoxygenation of lignin derived aromatics represents an important step towards the valorization of biomass. With this goal in mind, we synthesized a hybrid molecular/heterogeneous catalyst comprised of a (2,6-bis(1-methylbenzimidazolyl)pyridine-4′-aminopropyltrisiloxane)palladium(II) molecular catalyst covalently bound to a solid silica support through the siloxane functional group. A series of model complexes containing C–O bonds typically found in lignin biomass were explored and varying degrees of C–O bond hydrogenation were achieved. The stable covalent binding of the catalyst to the support was attributed to the observed long catalyst lifetimes which led to over 6000 catalytic turnovers without catalyst deactivation. Spectroscopic characterization of the catalyst pre- and post-catalytic reactions shows the catalyst maintains molecular integrity under the reaction conditions examined. The catalyst also exhibited complete selectivity for hydrodeoxygenation over ring hydrogenation of oxygenated aromatic molecules.
{"title":"Selective hydrodeoxygenation of oxygenated aromatic molecules using a molecular palladium catalyst covalently bound to a solid SiO2 support†","authors":"Jake G. Tillou, Joseph J. Kuchta, Nathan Thornburg, Santosh K. Balijepalli and Aaron K. Vannucci","doi":"10.1039/D4SU00333K","DOIUrl":"10.1039/D4SU00333K","url":null,"abstract":"<p >The selective hydrodeoxygenation of lignin derived aromatics represents an important step towards the valorization of biomass. With this goal in mind, we synthesized a hybrid molecular/heterogeneous catalyst comprised of a (2,6-bis(1-methylbenzimidazolyl)pyridine-4′-aminopropyltrisiloxane)palladium(<small>II</small>) molecular catalyst covalently bound to a solid silica support through the siloxane functional group. A series of model complexes containing C–O bonds typically found in lignin biomass were explored and varying degrees of C–O bond hydrogenation were achieved. The stable covalent binding of the catalyst to the support was attributed to the observed long catalyst lifetimes which led to over 6000 catalytic turnovers without catalyst deactivation. Spectroscopic characterization of the catalyst pre- and post-catalytic reactions shows the catalyst maintains molecular integrity under the reaction conditions examined. The catalyst also exhibited complete selectivity for hydrodeoxygenation over ring hydrogenation of oxygenated aromatic molecules.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00333k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141743261","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Carbanogels are carbon nanotube (CNT) lattices formed by carbon capture and utilization molten carbonate electrolysis of CO2. Higher tensile strength polymer composites with these CNTs from CO2 are prepared with epoxies and thermoplastics. The composites use less polymer to achieve strength, thereby lowering the polymer's carbon footprint.
{"title":"Polymer composites with carbon nanotubes made from CO2†","authors":"Gad Licht, Kyle Hofstetter and Stuart Licht","doi":"10.1039/D4SU00234B","DOIUrl":"10.1039/D4SU00234B","url":null,"abstract":"<p >Carbanogels are carbon nanotube (CNT) lattices formed by carbon capture and utilization molten carbonate electrolysis of CO<small><sub>2</sub></small>. Higher tensile strength polymer composites with these CNTs from CO<small><sub>2</sub></small> are prepared with epoxies and thermoplastics. The composites use less polymer to achieve strength, thereby lowering the polymer's carbon footprint.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00234b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141743262","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Aida Kiani, Marco Palumbo and Maria Rosaria Acocella
An unprecedented amidation of oxidized carbon black (oCB) by a mechanochemical approach is reported. The reaction proceeds in the presence of octadecylamine (ODA) in a short time, providing the corresponding adduct (oCB/ODA) with a high degree of functionalization. Hummers and ball milling procedures were used to obtain oxidized carbon black in solution and solvent-free conditions, respectively. Although the oxidation procedure used for oCB synthesis can deeply affect the degree of amidation because of the different nature of the functional groups on the carbon surface, the resulting powders were both functionalized with amine. The corresponding adducts showed a strong inversion of polarity, going from the high dispersibility in the water solution of the starting material to the high hydrophobic behaviour due to the alkyl chains bonded on the surface. Since the mechanochemical approach respects important green metrics, the procedure is highly sustainable.
{"title":"Eco-friendly amidation of oxidized carbon black by dry ball milling†","authors":"Aida Kiani, Marco Palumbo and Maria Rosaria Acocella","doi":"10.1039/D4SU00216D","DOIUrl":"10.1039/D4SU00216D","url":null,"abstract":"<p >An unprecedented amidation of oxidized carbon black (oCB) by a mechanochemical approach is reported. The reaction proceeds in the presence of octadecylamine (ODA) in a short time, providing the corresponding adduct (oCB/ODA) with a high degree of functionalization. Hummers and ball milling procedures were used to obtain oxidized carbon black in solution and solvent-free conditions, respectively. Although the oxidation procedure used for oCB synthesis can deeply affect the degree of amidation because of the different nature of the functional groups on the carbon surface, the resulting powders were both functionalized with amine. The corresponding adducts showed a strong inversion of polarity, going from the high dispersibility in the water solution of the starting material to the high hydrophobic behaviour due to the alkyl chains bonded on the surface. Since the mechanochemical approach respects important green metrics, the procedure is highly sustainable.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00216d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141743265","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yang Chen, Saleh Ibrahim, Sijia Zheng, Liam Wittenberg, Spencer Chapple, Griffin LaChapelle, Cheok Hang Iao, Adam Bourke and Michael A. Brook
Correction for ‘Cleaning steel by devulcanizing rubber from used automotive tires' by Yang Chen et al., RSC Sustain., 2023, 1, 2006–2013, https://doi.org/10.1039/D3SU00218G.
{"title":"Correction: Cleaning steel by devulcanizing rubber from used automotive tires","authors":"Yang Chen, Saleh Ibrahim, Sijia Zheng, Liam Wittenberg, Spencer Chapple, Griffin LaChapelle, Cheok Hang Iao, Adam Bourke and Michael A. Brook","doi":"10.1039/D4SU90030H","DOIUrl":"10.1039/D4SU90030H","url":null,"abstract":"<p >Correction for ‘Cleaning steel by devulcanizing rubber from used automotive tires' by Yang Chen <em>et al.</em>, <em>RSC Sustain.</em>, 2023, <strong>1</strong>, 2006–2013, https://doi.org/10.1039/D3SU00218G.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su90030h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141743266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lisa Eisele, Bletë Hulaj, Maximilian Podsednik, Francesco Laudani, Pablo Ayala, Alexey Cherevan, Annette Foelske, Andreas Limbeck, Dominik Eder and Katharina Bica-Schröder
Photocatalytic production of CO from CO2 has the potential for safe and atom-economic production of feedstock chemicals via in situ carbonylation chemistry. We developed novel ionic liquid-based polymeric materials through radical copolymerisation of 1-butyl-3-vinylimidazolium chloride and photocatalytically active Re- and Ru-complexes that serve as the CO2 reduction catalyst and photosensitiser, respectively. The crosslinked polymeric framework allows for the facile immobilisation of molecular organometallic complexes for use as heterogenised catalysts; moreover, the involved imidazolium core units co-catalyze the reduction of CO2via covalent interaction. The ratio of sensitiser and catalyst was analysed by laser ablation inductively coupled plasma mass spectroscopy (LA-ICP-MS) and set in relation to results from photocatalytic experiments. Ultimately, the heterogenous polymeric framework showed high selectivity for CO formation on photocatalytic CO2 reduction with improved stability to the corresponding homogenous system.
通过原位羰基化化学,光催化从 CO2 生成 CO 有可能实现安全、原子经济的原料化学品生产。我们通过 1-丁基-3-乙烯基氯化咪唑与光催化活性 Re- 和 Ru-复合物的自由基共聚,开发出了新型离子液体基聚合物材料,可分别用作二氧化碳还原催化剂和光敏剂。交联聚合物框架可以方便地固定分子有机金属复合物,用作异质催化剂;此外,其中的咪唑核心单元通过共价作用共同催化二氧化碳还原。通过激光烧蚀电感耦合等离子体质谱(LA-ICP-MS)分析了敏化剂和催化剂的比例,并根据光催化实验的结果进行了设定。最终,与相应的均质系统相比,异质聚合物框架在光催化二氧化碳还原过程中对一氧化碳的生成具有更高的选择性和更强的稳定性。
{"title":"Polymerized ionic liquid Co-catalysts driving photocatalytic CO2 transformation†","authors":"Lisa Eisele, Bletë Hulaj, Maximilian Podsednik, Francesco Laudani, Pablo Ayala, Alexey Cherevan, Annette Foelske, Andreas Limbeck, Dominik Eder and Katharina Bica-Schröder","doi":"10.1039/D4SU00194J","DOIUrl":"10.1039/D4SU00194J","url":null,"abstract":"<p >Photocatalytic production of CO from CO<small><sub>2</sub></small> has the potential for safe and atom-economic production of feedstock chemicals <em>via in situ</em> carbonylation chemistry. We developed novel ionic liquid-based polymeric materials through radical copolymerisation of 1-butyl-3-vinylimidazolium chloride and photocatalytically active Re- and Ru-complexes that serve as the CO<small><sub>2</sub></small> reduction catalyst and photosensitiser, respectively. The crosslinked polymeric framework allows for the facile immobilisation of molecular organometallic complexes for use as heterogenised catalysts; moreover, the involved imidazolium core units co-catalyze the reduction of CO<small><sub>2</sub></small><em>via</em> covalent interaction. The ratio of sensitiser and catalyst was analysed by laser ablation inductively coupled plasma mass spectroscopy (LA-ICP-MS) and set in relation to results from photocatalytic experiments. Ultimately, the heterogenous polymeric framework showed high selectivity for CO formation on photocatalytic CO<small><sub>2</sub></small> reduction with improved stability to the corresponding homogenous system.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00194j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141721042","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
This work utilizes an innovative microwave-visible irradiated continuous stirred slurry reactor (MWVIS-CSSR) for sustainable continuous production of a drop-in biofuel, namely, ethyl levulinate (EL), from pretreated sugarcane bagasse (PSCB). Besides, a novel realistic kinetic model, considering MWVIS intensified EL production through parallel non-catalytic and homogeneous–heterogeneous catalytic pathways in the presence of a magnetic Ni0.5Zn0.5Fe2O4 (NZF) photocatalyst in conjunction with an oxalic acid–choline chloride based acidic deep eutectic solvent (DES2), was also formulated and validated (R2 adj. ≥ 0.95). The 5 liter volume MWVIS-CSSR could render maximum 54.7 mol% EL yield (selectivity: 97.85%) at a feed flow rate of 35 ml min−1 under optimized conditions (temperature: 100 °C, NZF loading: 6 wt% PSCB, stirring speed: 500 rpm). Remarkably, the synergistic impact of MW and VIS irradiation substantially elevated the EL yield (54.7 mol%) compared to those of the individual MW (29.45 mol%) and VIS (20.1 mol%) systems. The optimally produced EL when blended at 5 vol% with B10 and B20 (10% and 20% biodiesel–diesel blends) could enhance the brake thermal efficiency (1–2%) besides mitigating 21–22% HC and 7.5–20% CO engine exhaust emissions in comparison with reference blends (B10 and B20). Notably, the reactor scale-up study based on the penetration depth of the MW and VIS energy of NZF and DES2 showcased the potential to upscale the 5 liter MWVIS-CSSR to a 1 m3 volume, allowing EL production to reach 689 kg h−1 with a sugarcane bagasse processing capacity of 2000 kg h−1. Moreover, the process simulation conducted in Aspen Plus software, utilizing COSMO-based property estimation with DFT calculations, alongside the techno-economic analysis, revealed a robust internal rate of return (IRR) of 54.25% and a net present value (NPV) of 8.22 × 105 US$ with a payback period of 4.91 years. Additionally, the environmental impact analysis study for the scaled-up EL production process in the MWVIS-CSSR revealed a reduction of 40–60% in marine ecotoxicity and 39–61% in human toxicity compared to the separate MW-CSSR and VIS-CSSR systems.
本研究利用创新的微波-可见光辐照连续搅拌淤浆反应器(MWVIS-CSSR),从预处理甘蔗渣(PSCB)中以生态友好和具有成本效益的方式连续生产滴入型生物燃料,即乙酰丙酸乙酯(EL)。此外,考虑到在磁性 Ni0.5Zn0.5Fe2O4(NZF)光催化剂与草酸-氯化胆碱基酸性深共晶溶剂(DES2)的作用下,MWVIS 可通过平行非催化和均相-异相催化途径强化 EL 的生产,该研究还制定并验证了一个新的现实动力学模型(R2 adj. ≥ 0.95)。在优化条件下(温度:100°C;NZF 负载:6 wt.% 的 PSCB;搅拌速度:500 rpm),进料流速为 35 ml/min,5 升体积的 MWVIS-CSSR 可产生最高 54.7 mol% 的 EL 收率(选择性:97.85%)。值得注意的是,与单独的 MW(29.45 摩尔%)和 VIS(20.1 摩尔%)体系相比,MW 和 VIS 辐照的协同作用大大提高了 EL 的产量(54.7 摩尔%)。与参考混合物(B10 和 B20)相比,优化生产的 EL 与 B10 和 B20(10% 和 20%的生物柴油-柴油混合物)混合 5 Vol%时,除了能减少 21-22% 的 HC 和 7.5-20% 的 CO 发动机废气排放外,还能提高断裂热效率(1-2%)。值得注意的是,基于 MW 的渗透深度以及 NZF 和 DES2 的 VIS 能量进行的反应器放大研究表明,5 升 MWVIS-CSSR 有可能放大到 1 立方米的容积,而甘蔗渣到 EL 的转化过程可放大到 2000 公斤/小时的处理能力。此外,在 Aspen Plus 软件中进行的工艺模拟,利用基于 COSMO 的属性估计和 DFT 计算,以及技术经济分析,显示出 54.25% 的稳健内部收益率和 8.22E+05 美元的净现值,投资回收期为 4.91 年。此外,对 MWVIS-CSSR 可持续电解质生产工艺的环境影响分析研究表明,与单独的 MW-CSSR 和 VIS-CSSR 反应器系统相比,海洋生态毒性降低了 40-60%,人体毒性降低了 39-61%。
{"title":"Continuous drop-in-biofuel production from pretreated sugarcane bagasse in a microwave-visible irradiated continuous stirred slurry reactor: reaction kinetics & techno-enviro-economic sustainability analyses†","authors":"Sourav Barman and Rajat Chakraborty","doi":"10.1039/D4SU00250D","DOIUrl":"10.1039/D4SU00250D","url":null,"abstract":"<p >This work utilizes an innovative microwave-visible irradiated continuous stirred slurry reactor (MWVIS-CSSR) for sustainable continuous production of a drop-in biofuel, namely, ethyl levulinate (EL), from pretreated sugarcane bagasse (PSCB). Besides, a novel realistic kinetic model, considering MWVIS intensified EL production through parallel non-catalytic and homogeneous–heterogeneous catalytic pathways in the presence of a magnetic Ni<small><sub>0.5</sub></small>Zn<small><sub>0.5</sub></small>Fe<small><sub>2</sub></small>O<small><sub>4</sub></small> (NZF) photocatalyst in conjunction with an oxalic acid–choline chloride based acidic deep eutectic solvent (DES2), was also formulated and validated (<em>R</em><small><sup>2</sup></small> adj. ≥ 0.95). The 5 liter volume MWVIS-CSSR could render maximum 54.7 mol% EL yield (selectivity: 97.85%) at a feed flow rate of 35 ml min<small><sup>−1</sup></small> under optimized conditions (temperature: 100 °C, NZF loading: 6 wt% PSCB, stirring speed: 500 rpm). Remarkably, the synergistic impact of MW and VIS irradiation substantially elevated the EL yield (54.7 mol%) compared to those of the individual MW (29.45 mol%) and VIS (20.1 mol%) systems. The optimally produced EL when blended at 5 vol% with B10 and B20 (10% and 20% biodiesel–diesel blends) could enhance the brake thermal efficiency (1–2%) besides mitigating 21–22% HC and 7.5–20% CO engine exhaust emissions in comparison with reference blends (B10 and B20). Notably, the reactor scale-up study based on the penetration depth of the MW and VIS energy of NZF and DES2 showcased the potential to upscale the 5 liter MWVIS-CSSR to a 1 m<small><sup>3</sup></small> volume, allowing EL production to reach 689 kg h<small><sup>−1</sup></small> with a sugarcane bagasse processing capacity of 2000 kg h<small><sup>−1</sup></small>. Moreover, the process simulation conducted in Aspen Plus software, utilizing COSMO-based property estimation with DFT calculations, alongside the techno-economic analysis, revealed a robust internal rate of return (IRR) of 54.25% and a net present value (NPV) of 8.22 × 10<small><sup>5</sup></small> US$ with a payback period of 4.91 years. Additionally, the environmental impact analysis study for the scaled-up EL production process in the MWVIS-CSSR revealed a reduction of 40–60% in marine ecotoxicity and 39–61% in human toxicity compared to the separate MW-CSSR and VIS-CSSR systems.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00250d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141721043","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A. Cornelio, A. Zanoletti, M. Scaglia, E. Galli, D. La Corte, G. Biava and E. Bontempi
During the energy transition, the demand for strategic metals has become a focal point due to their crucial roles in advancing cleaner energy technologies and sustainable practices. As a response to the potential supply vulnerabilities of critical raw materials, recycling has gained attention, despite some methods being more expensive than traditional mining. In this context, new technologies based on microwave radiation have been recently introduced to recover lithium from spent lithium-ion batteries. This study highlights the innovative results achieved through the application of microwave heating to lithium cobalt oxide (LCO) black mass, showing that mass increase can support the possibility of proposing the technology as a new sustainable approach. The possibility of coupling carbon materials with magnetic materials, available in the black mass (BM) results in a strategic approach to increasing the final temperature of microwave-absorbing materials. The process proves highly efficient in lithium recovery, with a treatment at 600 W for 5 minutes, reaching a value higher than 80%, while also eliminating some labour-intensive pre-treatment steps. The research sheds light on both the advantages and potential challenges associated with this ground-breaking technology.
{"title":"Thermal approaches based on microwaves to recover lithium from spent lithium-ion batteries†","authors":"A. Cornelio, A. Zanoletti, M. Scaglia, E. Galli, D. La Corte, G. Biava and E. Bontempi","doi":"10.1039/D4SU00202D","DOIUrl":"10.1039/D4SU00202D","url":null,"abstract":"<p >During the energy transition, the demand for strategic metals has become a focal point due to their crucial roles in advancing cleaner energy technologies and sustainable practices. As a response to the potential supply vulnerabilities of critical raw materials, recycling has gained attention, despite some methods being more expensive than traditional mining. In this context, new technologies based on microwave radiation have been recently introduced to recover lithium from spent lithium-ion batteries. This study highlights the innovative results achieved through the application of microwave heating to lithium cobalt oxide (LCO) black mass, showing that mass increase can support the possibility of proposing the technology as a new sustainable approach. The possibility of coupling carbon materials with magnetic materials, available in the black mass (BM) results in a strategic approach to increasing the final temperature of microwave-absorbing materials. The process proves highly efficient in lithium recovery, with a treatment at 600 W for 5 minutes, reaching a value higher than 80%, while also eliminating some labour-intensive pre-treatment steps. The research sheds light on both the advantages and potential challenges associated with this ground-breaking technology.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00202d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141721044","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lulu Wang, Hua Yuan, Xiaoli Ma, Zijin Li, Haowei Sun, Xiaoyan Zhang, Xiaoyu Huang, Qiaohong Peng and Yeqiang Tan
Ricinoleic acid, a natural hydroxy fatty acid, is a good candidate for preparing biodegradable polymer elastomers. Herein, high molecular weight poly(ricinoleic acid) (PRA) with a weight average molecular weight up to 122 kDa was successfully synthesized by solution polycondensation of methyl ricinoleate (MR) in hydrophobic ionic liquids, 1-alkyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide. The influence of monomer concentration, polymerization temperature and time, catalyst and properties of the ionic liquids on the polycondensation was comprehensively studied. Compared with the melt polycondensation, the solution polycondensation of MR in the ionic liquids can achieve much higher molecular weights. The PRA polymerized in ionic liquids shows a 100% cis structure like the natural monomer.
蓖麻油酸是一种天然羟基脂肪酸,是制备可生物降解聚合物弹性体的良好候选材料。在此,通过蓖麻油酸甲酯(MR)在疏水性离子液体、1-烷基-3-甲基咪唑鎓双(三氟甲磺酰)亚胺中的溶液缩聚,成功合成了重量平均分子量高达 122 kDa 的高分子量聚蓖麻油酸(PRA)。全面研究了单体浓度、聚合温度和时间、催化剂以及离子液体性质对缩聚反应的影响。与熔融缩聚相比,MR 在离子液体中的溶液缩聚可以获得更高的分子量。在离子液体中聚合的 PRA 与天然单体一样呈现 100% 顺式结构。
{"title":"Synthesis of high molecular weight poly(ricinoleic acid) via direct solution polycondensation in hydrophobic ionic liquids†","authors":"Lulu Wang, Hua Yuan, Xiaoli Ma, Zijin Li, Haowei Sun, Xiaoyan Zhang, Xiaoyu Huang, Qiaohong Peng and Yeqiang Tan","doi":"10.1039/D4SU00185K","DOIUrl":"10.1039/D4SU00185K","url":null,"abstract":"<p >Ricinoleic acid, a natural hydroxy fatty acid, is a good candidate for preparing biodegradable polymer elastomers. Herein, high molecular weight poly(ricinoleic acid) (PRA) with a weight average molecular weight up to 122 kDa was successfully synthesized by solution polycondensation of methyl ricinoleate (MR) in hydrophobic ionic liquids, 1-alkyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide. The influence of monomer concentration, polymerization temperature and time, catalyst and properties of the ionic liquids on the polycondensation was comprehensively studied. Compared with the melt polycondensation, the solution polycondensation of MR in the ionic liquids can achieve much higher molecular weights. The PRA polymerized in ionic liquids shows a 100% cis structure like the natural monomer.</p>","PeriodicalId":74745,"journal":{"name":"RSC sustainability","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/su/d4su00185k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141573503","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}