Pub Date : 2024-08-13DOI: 10.1016/j.xcrp.2024.102146
Innovative approaches on clean alternative energy sources are important for future decarbonization. Electrification and hydrogen energy are crucial pathways for decarbonization in both transportation and buildings. However, life-cycle stage-wise carbon intensity is still unclear for both hydrogen- and electricity-driven energy. Furthermore, systematic evaluation on low-carbon transition pathways is insufficient specifically within the Internet of Energy that interfaces hydrogen and electricity. Here, a generic approach is proposed for quantifying life-cycle stage-wise carbon intensity of both hydrogen- and electricity-driven energy internets. Life-cycle decarbonization effects on vehicle pathways are compared with traditional vehicles with internal-combustion engines. Techno-economic and environmental feasibility of the future advanced hydrogen-driven Internet of Energy is analyzed based on net present value. The region-wise carbon-intensity map and associated decarbonization strategies will help researchers and policymakers in promoting sustainable development with the hydrogen economy.
{"title":"Life-cycle carbon-intensity mapping for hydrogen-driven energy and economy","authors":"","doi":"10.1016/j.xcrp.2024.102146","DOIUrl":"https://doi.org/10.1016/j.xcrp.2024.102146","url":null,"abstract":"<p>Innovative approaches on clean alternative energy sources are important for future decarbonization. Electrification and hydrogen energy are crucial pathways for decarbonization in both transportation and buildings. However, life-cycle stage-wise carbon intensity is still unclear for both hydrogen- and electricity-driven energy. Furthermore, systematic evaluation on low-carbon transition pathways is insufficient specifically within the Internet of Energy that interfaces hydrogen and electricity. Here, a generic approach is proposed for quantifying life-cycle stage-wise carbon intensity of both hydrogen- and electricity-driven energy internets. Life-cycle decarbonization effects on vehicle pathways are compared with traditional vehicles with internal-combustion engines. Techno-economic and environmental feasibility of the future advanced hydrogen-driven Internet of Energy is analyzed based on net present value. The region-wise carbon-intensity map and associated decarbonization strategies will help researchers and policymakers in promoting sustainable development with the hydrogen economy.</p>","PeriodicalId":9703,"journal":{"name":"Cell Reports Physical Science","volume":"30 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225846","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-13DOI: 10.1016/j.xcrp.2024.102144
Dayanand Kumar, Rajan Bharti, Hanrui Li, Dhananjay D. Kumbhar, Nazek El-Atab
By integrating sensing, processing, and memory functionalities, the human sensory systems are extraordinarily energy and power efficient. Here, we report a ZnSnO (ZTO)/InO-based optoelectronic device that senses varying light intensities and perceives different motion behaviors. The device exhibits exceptional voltage-activated synaptic properties, encompassing features such as short-term and long-term plasticity, alongside notable light-sensitive characteristics that enable diverse light-triggered synaptic functions. Through simultaneous light and electrical voltage signals, we achieve light-enhanced/electrically erasing behavior, light-initiated paired-pulse facilitation (PPF), and learning-forgetting-relearning processes by tuning the 405 nm wavelength optical light. Furthermore, by manipulating charge dynamics through light intensity and duration, we replicate the basic sensing and perception function of the human eyes as a volatile receptor, showing potential for artificial retina applications. The device also demonstrates the capability to track objects and eye movement, holding promise for virtual reality systems.
{"title":"Optoelectronic wide-band-gap oxide-based memristor for mimicking human eye sensory perception and object tracking","authors":"Dayanand Kumar, Rajan Bharti, Hanrui Li, Dhananjay D. Kumbhar, Nazek El-Atab","doi":"10.1016/j.xcrp.2024.102144","DOIUrl":"https://doi.org/10.1016/j.xcrp.2024.102144","url":null,"abstract":"By integrating sensing, processing, and memory functionalities, the human sensory systems are extraordinarily energy and power efficient. Here, we report a ZnSnO (ZTO)/InO-based optoelectronic device that senses varying light intensities and perceives different motion behaviors. The device exhibits exceptional voltage-activated synaptic properties, encompassing features such as short-term and long-term plasticity, alongside notable light-sensitive characteristics that enable diverse light-triggered synaptic functions. Through simultaneous light and electrical voltage signals, we achieve light-enhanced/electrically erasing behavior, light-initiated paired-pulse facilitation (PPF), and learning-forgetting-relearning processes by tuning the 405 nm wavelength optical light. Furthermore, by manipulating charge dynamics through light intensity and duration, we replicate the basic sensing and perception function of the human eyes as a volatile receptor, showing potential for artificial retina applications. The device also demonstrates the capability to track objects and eye movement, holding promise for virtual reality systems.","PeriodicalId":9703,"journal":{"name":"Cell Reports Physical Science","volume":"45 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225848","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-13DOI: 10.1016/j.xcrp.2024.102148
Silicon anodes for lithium-ion batteries offer high theoretical capacity but face practical challenges of capacity fading due to significant volumetric changes during charge-discharge cycles. To reveal the underlying mechanisms, we employ reactive force fields (ReaxFFs) in molecular dynamics simulations to conduct atomic analyses of lithiation and delithiation cycles of silicon particles with three diameters. Our simulations demonstrate a volumetric expansion exceeding 280%, primarily along the ⟨110⟩ direction, with an inward movement of the interface between lithiated and unlithiated regions. We introduce a metric, “geometric defect,” derived from the centroid deviation of neighboring atoms, to evaluate the structural integrity of the silicon anode. Geometric defect state of charge curves show a 5% capacity fade due to silicon loss after the initial cycle. Experimental validation confirms a capacity loss exceeding 40% after the first cycle, attributed to internal defects within silicon particles, aligning well with our simulation results.
{"title":"Reactive force-field simulation and experimental validation of cyclic defects in silicon anodes for lithium-ion batteries","authors":"","doi":"10.1016/j.xcrp.2024.102148","DOIUrl":"https://doi.org/10.1016/j.xcrp.2024.102148","url":null,"abstract":"<p>Silicon anodes for lithium-ion batteries offer high theoretical capacity but face practical challenges of capacity fading due to significant volumetric changes during charge-discharge cycles. To reveal the underlying mechanisms, we employ reactive force fields (ReaxFFs) in molecular dynamics simulations to conduct atomic analyses of lithiation and delithiation cycles of silicon particles with three diameters. Our simulations demonstrate a volumetric expansion exceeding 280%, primarily along the ⟨110⟩ direction, with an inward movement of the interface between lithiated and unlithiated regions. We introduce a metric, “geometric defect,” derived from the centroid deviation of neighboring atoms, to evaluate the structural integrity of the silicon anode. Geometric defect state of charge curves show a 5% capacity fade due to silicon loss after the initial cycle. Experimental validation confirms a capacity loss exceeding 40% after the first cycle, attributed to internal defects within silicon particles, aligning well with our simulation results.</p>","PeriodicalId":9703,"journal":{"name":"Cell Reports Physical Science","volume":"63 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225847","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-13DOI: 10.1016/j.xcrp.2024.102149
Emulating nature’s living properties in functional materials is a crucial step toward creating adaptive and self-regulating systems capable of integration with biological tissues. In this perspective, we first investigate the various strategies employed in the field of bioelectronics and engineered living materials to replicate nature's living functionalities. Then, we explore the convergence of bioelectronics and engineered living materials, highlighting an approach called living bioelectronics. We posit that merging these two fields can enable the creation of robust, adaptable devices that replicate the dynamic functionalities of living systems. Living bioelectronics integrate the strength of both disciplines while complementing their weaknesses, heralding opportunities for biosensing, personalized therapies, and applications beyond healthcare.
{"title":"The convergence of bioelectronics and engineered living materials","authors":"","doi":"10.1016/j.xcrp.2024.102149","DOIUrl":"https://doi.org/10.1016/j.xcrp.2024.102149","url":null,"abstract":"<p>Emulating nature’s living properties in functional materials is a crucial step toward creating adaptive and self-regulating systems capable of integration with biological tissues. In this perspective, we first investigate the various strategies employed in the field of bioelectronics and engineered living materials to replicate nature's living functionalities. Then, we explore the convergence of bioelectronics and engineered living materials, highlighting an approach called living bioelectronics. We posit that merging these two fields can enable the creation of robust, adaptable devices that replicate the dynamic functionalities of living systems. Living bioelectronics integrate the strength of both disciplines while complementing their weaknesses, heralding opportunities for biosensing, personalized therapies, and applications beyond healthcare.</p>","PeriodicalId":9703,"journal":{"name":"Cell Reports Physical Science","volume":"61 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225845","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-12DOI: 10.1016/j.xcrp.2024.102150
RNA secondary structures comprise double-stranded (ds) and single-stranded (ss) regions. Antisense peptide nucleic acids (asPNAs) enable the targeting of ssRNAs and weakly formed dsRNAs. Nucleobase-modified dsRNA-binding PNAs (dbPNAs) allow for dsRNA targeting. A programmable RNA-structure-specific targeting strategy is needed for the simultaneous recognition of dsRNAs and ssRNAs. Here, we report on combining dbPNAs and asPNAs (designated as daPNAs) for the targeting of dsRNA-ssRNA junctions. Our data suggest that combining traditional asPNA (with a 4-letter code: T, C, A, and G) and dbPNA (with a 4-letter code: T or s2U, L, Q, and E) scaffolds facilitates RNA-structure-specific tight binding (nM to μM). We further apply our daPNAs in substrate-specific inhibition of Dicer acting on precursor miRNA (pre-miR)-198 in a cell-free assay and regulating ribosomal frameshifting induced by model hairpins in both cell-free and cell culture assays. daPNAs would be a useful platform for developing chemical probes and therapeutic ligands targeting RNA.
{"title":"Recognition of RNA secondary structures with a programmable peptide nucleic acid-based platform","authors":"","doi":"10.1016/j.xcrp.2024.102150","DOIUrl":"https://doi.org/10.1016/j.xcrp.2024.102150","url":null,"abstract":"<p>RNA secondary structures comprise double-stranded (ds) and single-stranded (ss) regions. Antisense peptide nucleic acids (asPNAs) enable the targeting of ssRNAs and weakly formed dsRNAs. Nucleobase-modified dsRNA-binding PNAs (dbPNAs) allow for dsRNA targeting. A programmable RNA-structure-specific targeting strategy is needed for the simultaneous recognition of dsRNAs and ssRNAs. Here, we report on combining dbPNAs and asPNAs (designated as daPNAs) for the targeting of dsRNA-ssRNA junctions. Our data suggest that combining traditional asPNA (with a 4-letter code: T, C, A, and G) and dbPNA (with a 4-letter code: T or s<sup>2</sup>U, L, Q, and E) scaffolds facilitates RNA-structure-specific tight binding (nM to μM). We further apply our daPNAs in substrate-specific inhibition of Dicer acting on precursor miRNA (pre-miR)-198 in a cell-free assay and regulating ribosomal frameshifting induced by model hairpins in both cell-free and cell culture assays. daPNAs would be a useful platform for developing chemical probes and therapeutic ligands targeting RNA.</p>","PeriodicalId":9703,"journal":{"name":"Cell Reports Physical Science","volume":"35 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141945243","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-09DOI: 10.1016/j.xcrp.2024.102147
Diabetes is an inflammatory disease that usually causes chronic wounds for which no satisfactory therapies currently exist. Here we report a physical approach using a cold atmospheric plasma (CAP) to target diabetic wounds locally for regulating the inflammatory phase of the wounds. In this paper, a comprehensive analysis of inflammatory factors combined with physical investigations of the helium plasma jet characteristics is conducted. The physical and biological safety and clinical application prospects of the CAP jet for the human body are also analyzed. The results demonstrate for the first time that CAP therapy can stimulate the body’s own inflammatory regulation function to achieve a normal state, rather than excessively interfere in a single target. This involves the inhibition of pro-inflammatory factors in the onset subphase and the promotion of anti-inflammatory factors in the subsequent resolution subphase. This research contributes to the development of highly effective and safe topical therapies to promote chronic wound healing.
糖尿病是一种炎症性疾病,通常会导致慢性伤口,目前还没有令人满意的治疗方法。在此,我们报告了一种利用冷大气等离子体(CAP)针对糖尿病伤口局部调节伤口炎症阶段的物理方法。本文结合氦等离子体射流特性的物理研究,对炎症因素进行了全面分析。同时还分析了 CAP 射流对人体的物理和生物安全性以及临床应用前景。研究结果首次证明,CAP疗法可以激发人体自身的炎症调节功能,使其达到正常状态,而不是对单一目标进行过度干预。这包括在发病子阶段抑制促炎因子,在随后的消炎子阶段促进抗炎因子。这项研究有助于开发高效安全的局部疗法,促进慢性伤口愈合。
{"title":"A nature-based solution for regulating the inflammatory phase of diabetic wound healing using a cold atmospheric plasma","authors":"","doi":"10.1016/j.xcrp.2024.102147","DOIUrl":"https://doi.org/10.1016/j.xcrp.2024.102147","url":null,"abstract":"<p>Diabetes is an inflammatory disease that usually causes chronic wounds for which no satisfactory therapies currently exist. Here we report a physical approach using a cold atmospheric plasma (CAP) to target diabetic wounds locally for regulating the inflammatory phase of the wounds. In this paper, a comprehensive analysis of inflammatory factors combined with physical investigations of the helium plasma jet characteristics is conducted. The physical and biological safety and clinical application prospects of the CAP jet for the human body are also analyzed. The results demonstrate for the first time that CAP therapy can stimulate the body’s own inflammatory regulation function to achieve a normal state, rather than excessively interfere in a single target. This involves the inhibition of pro-inflammatory factors in the onset subphase and the promotion of anti-inflammatory factors in the subsequent resolution subphase. This research contributes to the development of highly effective and safe topical therapies to promote chronic wound healing.</p>","PeriodicalId":9703,"journal":{"name":"Cell Reports Physical Science","volume":"47 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-08-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141945165","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-08DOI: 10.1016/j.xcrp.2024.102143
Commercial lithium-ion battery electrodes today are manufactured by slurry casting active material powder onto a metal current collector foil. This manufacturing process has become embedded over recent decades but limits commercial cell performance. This paper presents patterning of a monolithic active material sheet as an alternative to slurry casting. The concept is proven experimentally by laser drilling a pyrolytic graphite sheet to increase the gravimetric active material capacity from 10 mA h g−1 to 450 mA h g−1, when used as a negative lithium-intercalation electrode. Cell-level calculations show that, without changing the chemistry, a pyrolytic graphite sheet electrode with a hexagonal array of 5 μm diameter, 20 μm pitch channels could increase the gravimetric energy density of a LGM50 cell by 22% to 322 W h kg−1. By moving beyond slurry casting, patterned monolithic electrodes could enable batteries with lower cost, reduced energy intensity, and enhanced performance.
目前,商用锂离子电池电极的制造方法是将活性材料粉末浆状浇铸到金属集流箔上。近几十年来,这种制造工艺已成为嵌入式工艺,但却限制了商用电池的性能。本文介绍了整体活性材料片的图案化,作为浆料浇铸的替代方法。通过激光钻孔热解石墨片,实验证明了这一概念,在用作锂闰负极时,可将活性材料的重力容量从 10 mA h g-1 提高到 450 mA h g-1。电池级计算显示,在不改变化学成分的情况下,具有直径 5 μm、间距 20 μm 的六边形沟道阵列的热解石墨片电极可将 LGM50 电池的重力能量密度提高 22%,达到 322 W h kg-1。通过超越浆料浇铸技术,图案化单片电极可使电池成本更低、能量密度更低、性能更强。
{"title":"Beyond slurry cast: Patterning of a monolithic active material sheet to form free-standing, solvent-free, and low-tortuosity battery electrodes","authors":"","doi":"10.1016/j.xcrp.2024.102143","DOIUrl":"https://doi.org/10.1016/j.xcrp.2024.102143","url":null,"abstract":"<p>Commercial lithium-ion battery electrodes today are manufactured by slurry casting active material powder onto a metal current collector foil. This manufacturing process has become embedded over recent decades but limits commercial cell performance. This paper presents patterning of a monolithic active material sheet as an alternative to slurry casting. The concept is proven experimentally by laser drilling a pyrolytic graphite sheet to increase the gravimetric active material capacity from 10 mA h g<sup>−1</sup> to 450 mA h g<sup>−1</sup>, when used as a negative lithium-intercalation electrode. Cell-level calculations show that, without changing the chemistry, a pyrolytic graphite sheet electrode with a hexagonal array of 5 μm diameter, 20 μm pitch channels could increase the gravimetric energy density of a LGM50 cell by 22% to 322 W h kg<sup>−1</sup>. By moving beyond slurry casting, patterned monolithic electrodes could enable batteries with lower cost, reduced energy intensity, and enhanced performance.</p>","PeriodicalId":9703,"journal":{"name":"Cell Reports Physical Science","volume":"65 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141945244","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-06DOI: 10.1016/j.xcrp.2024.102140
Dense bioceramics feature hierarchical microstructures with weak interfaces that endow them with strength, toughness, and structural functionalities. Conversely, most technical ceramics possess limited structural complexity and strong grain boundaries that restrict their toughness and functions. Here, we report a rational design strategy to fabricate ceramics with various bioinspired microstructural motifs, leading to strength, toughness, and locally varying properties. We employ magnetically assisted slip casting (MASC) for local orientations of alumina microplatelets and ultrafast high-temperature sintering (UHS) as a densifying method. We sequentially vary the slurry composition and sintering processes to attain high texture, relative density, and weak grain interfaces. We realize dense ceramics with horizontal, periodic, and graded motifs that exhibit direction- and site-specific properties, with flexural strengths of ∼290, 155, and 215 MPa, and fracture toughness of ∼7, 5, and 10 MPa·m0.5, respectively. The strategy could be used to fabricate ceramic composites for tailorable local and bulk properties.
{"title":"Rational design and fabrication of hierarchical ceramics using bioinspired microstructures for tailorable strength and toughness","authors":"","doi":"10.1016/j.xcrp.2024.102140","DOIUrl":"https://doi.org/10.1016/j.xcrp.2024.102140","url":null,"abstract":"<p>Dense bioceramics feature hierarchical microstructures with weak interfaces that endow them with strength, toughness, and structural functionalities. Conversely, most technical ceramics possess limited structural complexity and strong grain boundaries that restrict their toughness and functions. Here, we report a rational design strategy to fabricate ceramics with various bioinspired microstructural motifs, leading to strength, toughness, and locally varying properties. We employ magnetically assisted slip casting (MASC) for local orientations of alumina microplatelets and ultrafast high-temperature sintering (UHS) as a densifying method. We sequentially vary the slurry composition and sintering processes to attain high texture, relative density, and weak grain interfaces. We realize dense ceramics with horizontal, periodic, and graded motifs that exhibit direction- and site-specific properties, with flexural strengths of ∼290, 155, and 215 MPa, and fracture toughness of ∼7, 5, and 10 MPa·m<sup>0.5</sup>, respectively. The strategy could be used to fabricate ceramic composites for tailorable local and bulk properties.</p>","PeriodicalId":9703,"journal":{"name":"Cell Reports Physical Science","volume":"25 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141945164","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-06DOI: 10.1016/j.xcrp.2024.102145
Recycling diverse waste plastics poses challenges due to complex sorting and processing, resulting in high costs and inefficiency. To tackle this, we present a metal-free catalytic sorting method for targeted deconstruction of polyester from post-consumer plastic waste, encompassing textiles, plastic mixtures, and multilayer packaging materials. This method employs N-methylpiperidine, a tertiary amine catalyst in methanol, to depolymerize polyethylene terephthalate (PET). Operating under these conditions (160°C, 1 h), we achieve 100% yields of dimethyl terephthalate and ethylene glycol. This technique also effectively breaks down other polyesters, including polylactic acid, polycarbonate, and polybutylene terephthalate, yielding high-yield monomers at relatively low temperatures. Through comprehensive nuclear magnetic resonance (NMR) analysis, we propose that N-methylpiperidine’s role is in enhancing methanol nucleophilicity and activating PET’s ester bond. Our insights advance the chemical recycling of post-consumer plastic waste, offering a potentially simple and efficient path to closing the polyester production loop.
由于分拣和处理过程复杂,各种废塑料的回收利用面临挑战,导致成本高、效率低。为解决这一问题,我们提出了一种无金属催化分拣方法,用于从消费后塑料垃圾(包括纺织品、塑料混合物和多层包装材料)中有针对性地解构聚酯。该方法采用甲醇中的叔胺催化剂 N-甲基哌啶来解聚聚对苯二甲酸乙二酯(PET)。在这种条件下(160°C,1 小时),我们可以获得 100% 产率的对苯二甲酸二甲酯和乙二醇。这种技术还能有效分解其他聚酯,包括聚乳酸、聚碳酸酯和聚对苯二甲酸丁二醇酯,在相对较低的温度下产生高产单体。通过全面的核磁共振 (NMR) 分析,我们提出 N-甲基哌啶的作用是增强甲醇的亲核性并激活 PET 的酯键。我们的见解推动了消费后塑料废弃物的化学回收,为聚酯生产的闭环提供了一条简单而高效的潜在途径。
{"title":"Chemical recycling of post-consumer polyester wastes using a tertiary amine organocatalyst","authors":"","doi":"10.1016/j.xcrp.2024.102145","DOIUrl":"https://doi.org/10.1016/j.xcrp.2024.102145","url":null,"abstract":"<p>Recycling diverse waste plastics poses challenges due to complex sorting and processing, resulting in high costs and inefficiency. To tackle this, we present a metal-free catalytic sorting method for targeted deconstruction of polyester from post-consumer plastic waste, encompassing textiles, plastic mixtures, and multilayer packaging materials. This method employs N-methylpiperidine, a tertiary amine catalyst in methanol, to depolymerize polyethylene terephthalate (PET). Operating under these conditions (160°C, 1 h), we achieve 100% yields of dimethyl terephthalate and ethylene glycol. This technique also effectively breaks down other polyesters, including polylactic acid, polycarbonate, and polybutylene terephthalate, yielding high-yield monomers at relatively low temperatures. Through comprehensive nuclear magnetic resonance (NMR) analysis, we propose that N-methylpiperidine’s role is in enhancing methanol nucleophilicity and activating PET’s ester bond. Our insights advance the chemical recycling of post-consumer plastic waste, offering a potentially simple and efficient path to closing the polyester production loop.</p>","PeriodicalId":9703,"journal":{"name":"Cell Reports Physical Science","volume":"4 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141969258","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-06DOI: 10.1016/j.xcrp.2024.102141
Fusicoccane diterpenoids, originating from fungi, plants, and bacteria, constitute a diverse natural product family featuring a 5-8-5 tricyclic framework. They were restricted to plant physiology in the past. However, fusicoccanes are presently at the forefront of biomedicine and are indispensable for probing 14-3-3 protein-protein interactions (PPIs). The need for material supply and scaffold diversification encouraged their study by the synthetic community. This review highlights the total synthetic works on fusicoccane diterpenoids published in the last 5 years. Key transformations including ring-closing metathesis, metal-catalyzed cross-coupling, and carbocyclization markedly enhanced synthetic efficiency and versatility. Recently identified biosynthetic transformations inspired innovative chemoenzymatic strategies. Investigation into the functional aspects of fusicoccanes should be the future direction to realize their therapeutic potential as general 14-3-3 PPI modulators.
{"title":"Recent total syntheses of fusicoccanes","authors":"","doi":"10.1016/j.xcrp.2024.102141","DOIUrl":"https://doi.org/10.1016/j.xcrp.2024.102141","url":null,"abstract":"<p>Fusicoccane diterpenoids, originating from fungi, plants, and bacteria, constitute a diverse natural product family featuring a 5-8-5 tricyclic framework. They were restricted to plant physiology in the past. However, fusicoccanes are presently at the forefront of biomedicine and are indispensable for probing 14-3-3 protein-protein interactions (PPIs). The need for material supply and scaffold diversification encouraged their study by the synthetic community. This review highlights the total synthetic works on fusicoccane diterpenoids published in the last 5 years. Key transformations including ring-closing metathesis, metal-catalyzed cross-coupling, and carbocyclization markedly enhanced synthetic efficiency and versatility. Recently identified biosynthetic transformations inspired innovative chemoenzymatic strategies. Investigation into the functional aspects of fusicoccanes should be the future direction to realize their therapeutic potential as general 14-3-3 PPI modulators.</p>","PeriodicalId":9703,"journal":{"name":"Cell Reports Physical Science","volume":"26 1","pages":""},"PeriodicalIF":8.9,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141945163","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}