Pub Date : 2024-09-30DOI: 10.1038/s42004-024-01311-2
Yi Han, Yaojie Guo, Nan Zhang, Fan Xu, Jarukitt Limwachiranon, Zhenzhen Xiong, Liru Xu, Xu-Ming Mao, Daniel H. Scharf
Fungal natural products from various species often feature hydroxamic acid motifs that have the ability to chelate iron. These compounds have an array of medicinally and ecologically relevant activities. Through genome mining, gene deletion in the host Aspergillus terreus, and heterologous expression experiments, this study has revealed that a nonribosomal peptide synthetase (NRPS) TamA and a specialized cytochrome P450 monooxygenase TamB catalyze the sequential biosynthetic reactions in the formation of terramides A-C, a series of diketopiperazines (DKPs) with hydroxamic acid motifs. Feeding experiments showed that TamB catalyzes an unprecedented di-hydroxylation of the amide nitrogens in the diketopiperazine core. This tailoring reaction led to the formation of two bidentate iron-binding sites per molecule with an unusual iron-binding stoichiometry. The structure of the terramide A-Fe complex was characterized by liquid chromatography-mass spectrometry (LC-MS), Fourier transform infrared spectroscopy (FT-IR), Raman spectroscopy and electron paramagnetic resonance spectroscopy (EPR). Antimicrobial assays showed that the iron-binding motifs are crucial for the activity against bacteria and fungi. Murine infection experiments indicated that terramide production is crucial for the virulence of A. terreus and could be a potential antifungal drug target. Terramides A-C are produced by Aspergillus terreus and feature hydroxamic acid motifs in diketopiperazines to chelate iron; however, their biosynthesis is not fully understood. Here, the authors probe the function of two key enzymes TamA and TamB and propose the biosynthesis of terramides A-C as well as their function in the virulence of A. terreus.
{"title":"Biosynthesis of iron-chelating terramides A-C and their role in Aspergillus terreus infection","authors":"Yi Han, Yaojie Guo, Nan Zhang, Fan Xu, Jarukitt Limwachiranon, Zhenzhen Xiong, Liru Xu, Xu-Ming Mao, Daniel H. Scharf","doi":"10.1038/s42004-024-01311-2","DOIUrl":"10.1038/s42004-024-01311-2","url":null,"abstract":"Fungal natural products from various species often feature hydroxamic acid motifs that have the ability to chelate iron. These compounds have an array of medicinally and ecologically relevant activities. Through genome mining, gene deletion in the host Aspergillus terreus, and heterologous expression experiments, this study has revealed that a nonribosomal peptide synthetase (NRPS) TamA and a specialized cytochrome P450 monooxygenase TamB catalyze the sequential biosynthetic reactions in the formation of terramides A-C, a series of diketopiperazines (DKPs) with hydroxamic acid motifs. Feeding experiments showed that TamB catalyzes an unprecedented di-hydroxylation of the amide nitrogens in the diketopiperazine core. This tailoring reaction led to the formation of two bidentate iron-binding sites per molecule with an unusual iron-binding stoichiometry. The structure of the terramide A-Fe complex was characterized by liquid chromatography-mass spectrometry (LC-MS), Fourier transform infrared spectroscopy (FT-IR), Raman spectroscopy and electron paramagnetic resonance spectroscopy (EPR). Antimicrobial assays showed that the iron-binding motifs are crucial for the activity against bacteria and fungi. Murine infection experiments indicated that terramide production is crucial for the virulence of A. terreus and could be a potential antifungal drug target. Terramides A-C are produced by Aspergillus terreus and feature hydroxamic acid motifs in diketopiperazines to chelate iron; however, their biosynthesis is not fully understood. Here, the authors probe the function of two key enzymes TamA and TamB and propose the biosynthesis of terramides A-C as well as their function in the virulence of A. terreus.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-10"},"PeriodicalIF":5.9,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01311-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329467","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-30DOI: 10.1038/s42004-024-01304-1
Atanu Baksi, Hasan Zerze, Aman Agrawal, Alamgir Karim, Gül H. Zerze
Complex coacervates play essential roles in various biological processes and applications. Although substantial progress has been made in understanding the molecular interactions driving complex coacervation, the mechanisms stabilizing coacervates against coalescence remain experimentally challenging and not fully elucidated. We recently showed that polydiallyldimethylammonium chloride (PDDA) and adenosine triphosphate (ATP) coacervates stabilize upon their transfer to deionized (DI) water. Here, we perform molecular dynamics simulations of PDDA-ATP coacervates in supernatant and DI water, to understand the ion dynamics and structure within stable coacervates. We found that transferring the coacervates to DI water results in an immediate ejection of a significant fraction of small ions (Na+ and Cl−) from the surface of the coacervates to DI water. We also observed a notable reduction in the mobility of these counterions in coacervates when in DI water, both in the cluster-forming and slab simulations, together with a lowered displacement of PDDA and ATP. These results suggest that the initial ejection of the ions from the coacervates in DI water may induce an interfacial skin layer formation, inhibiting further mobility of ions in the skin layer. Transferring coacervates based on polydiallyldimethylammonium chloride and adenosine triphosphate into deionized water has been experimentally demonstrated to stabilize them against coalescence. Here, molecular modeling and simulations are used to study the coacervation and stabilization of the relevant polyelectrolyte mixture, systematically investigating the structural and dynamic properties that lead to stability.
复合凝聚态在各种生物过程和应用中发挥着至关重要的作用。尽管在理解驱动复合凝聚的分子相互作用方面取得了重大进展，但稳定凝聚体防止凝聚的机制仍具有实验挑战性，尚未完全阐明。我们最近的研究表明，聚二烯丙基二甲基氯化铵（PDDA）和三磷酸腺苷（ATP）凝聚体在转移到去离子水中后会变得稳定。在此，我们对上清液和去离子水中的 PDDA-ATP 凝聚态进行了分子动力学模拟，以了解稳定凝聚态中的离子动力学和结构。我们发现，将共蒸物转移到去离子水中会导致大量小离子（Na+ 和 Cl-）立即从共蒸物表面喷射到去离子水中。在成团模拟和板块模拟中，我们还观察到这些反离子在去离子水中的流动性明显降低，同时 PDDA 和 ATP 的位移也降低了。这些结果表明，离子最初从去离子水中的共凝聚体中喷出时，可能会诱发界面表皮层的形成，从而抑制离子在表皮层中的进一步移动。实验证明，将基于聚二烯丙基二甲基氯化铵和三磷酸腺苷的凝聚态水转移到去离子水中可以使其稳定，防止凝聚。在此，我们利用分子建模和模拟来研究相关聚电解质混合物的凝聚和稳定，系统地研究了导致稳定的结构和动态特性。
{"title":"The molecular picture of the local environment in a stable model coacervate","authors":"Atanu Baksi, Hasan Zerze, Aman Agrawal, Alamgir Karim, Gül H. Zerze","doi":"10.1038/s42004-024-01304-1","DOIUrl":"10.1038/s42004-024-01304-1","url":null,"abstract":"Complex coacervates play essential roles in various biological processes and applications. Although substantial progress has been made in understanding the molecular interactions driving complex coacervation, the mechanisms stabilizing coacervates against coalescence remain experimentally challenging and not fully elucidated. We recently showed that polydiallyldimethylammonium chloride (PDDA) and adenosine triphosphate (ATP) coacervates stabilize upon their transfer to deionized (DI) water. Here, we perform molecular dynamics simulations of PDDA-ATP coacervates in supernatant and DI water, to understand the ion dynamics and structure within stable coacervates. We found that transferring the coacervates to DI water results in an immediate ejection of a significant fraction of small ions (Na+ and Cl−) from the surface of the coacervates to DI water. We also observed a notable reduction in the mobility of these counterions in coacervates when in DI water, both in the cluster-forming and slab simulations, together with a lowered displacement of PDDA and ATP. These results suggest that the initial ejection of the ions from the coacervates in DI water may induce an interfacial skin layer formation, inhibiting further mobility of ions in the skin layer. Transferring coacervates based on polydiallyldimethylammonium chloride and adenosine triphosphate into deionized water has been experimentally demonstrated to stabilize them against coalescence. Here, molecular modeling and simulations are used to study the coacervation and stabilization of the relevant polyelectrolyte mixture, systematically investigating the structural and dynamic properties that lead to stability.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-11"},"PeriodicalIF":5.9,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01304-1.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329463","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-29DOI: 10.1038/s42004-024-01284-2
César Moreno, Xabier Diaz de Cerio, Maria Tenorio, Fei Gao, Manuel Vilas-Varela, Ane Sarasola, Diego Peña, Aran Garcia-Lekue, Aitor Mugarza
Advancements in the on-surface synthesis of atomically precise graphene nanostructures are propelled by the introduction of innovative precursor designs and reaction types. Until now, the latter has been confined to cross-coupling and cyclization reactions that involve the cleavage of specific atoms or groups. In this article, we elucidate how the migration of phenyl substituents attached to graphene nanoribbons can be harnessed to generate arrays of [18]-annulene pores at the edges of the nanostructures. This sequential pathway is revealed through a comprehensive study employing bond-resolved scanning tunneling microscopy and ab-initio computational techniques. The yield of pore formation is maximized by anchoring the graphene nanoribbons at steps of vicinal surfaces, underscoring the potential of these substrates to guide reaction paths. Our study introduces a new reaction to the on-surface synthesis toolbox along with a sequential route, altogether enabling the extension of this strategy towards the formation of other porous nanostructures. The on-surface synthesis of graphene nanoribbons typically relies on Ullmann polymerization followed by an internal cyclodehydrogenation. Here, following these two steps, the authors expand the synthetic protocol by adding controlled phenyl migration and intraribbon aryl-aryl dehydrogenative coupling to afford graphene nanoribbons with periodic arrays of [18]annulene pores at the edges.
{"title":"On-surface synthesis of porous graphene nanoribbons mediated by phenyl migration","authors":"César Moreno, Xabier Diaz de Cerio, Maria Tenorio, Fei Gao, Manuel Vilas-Varela, Ane Sarasola, Diego Peña, Aran Garcia-Lekue, Aitor Mugarza","doi":"10.1038/s42004-024-01284-2","DOIUrl":"10.1038/s42004-024-01284-2","url":null,"abstract":"Advancements in the on-surface synthesis of atomically precise graphene nanostructures are propelled by the introduction of innovative precursor designs and reaction types. Until now, the latter has been confined to cross-coupling and cyclization reactions that involve the cleavage of specific atoms or groups. In this article, we elucidate how the migration of phenyl substituents attached to graphene nanoribbons can be harnessed to generate arrays of [18]-annulene pores at the edges of the nanostructures. This sequential pathway is revealed through a comprehensive study employing bond-resolved scanning tunneling microscopy and ab-initio computational techniques. The yield of pore formation is maximized by anchoring the graphene nanoribbons at steps of vicinal surfaces, underscoring the potential of these substrates to guide reaction paths. Our study introduces a new reaction to the on-surface synthesis toolbox along with a sequential route, altogether enabling the extension of this strategy towards the formation of other porous nanostructures. The on-surface synthesis of graphene nanoribbons typically relies on Ullmann polymerization followed by an internal cyclodehydrogenation. Here, following these two steps, the authors expand the synthetic protocol by adding controlled phenyl migration and intraribbon aryl-aryl dehydrogenative coupling to afford graphene nanoribbons with periodic arrays of [18]annulene pores at the edges.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-7"},"PeriodicalIF":5.9,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01284-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329453","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Increasing chemical pollution is a threat to sustainable water resources worldwide. Plastics and harmful additives released from plastics add to this burden and might pose a risk to aquatic organisms, and human health. Phthalates, which are common plasticizers and endocrine-disrupting chemicals, are released from polyvinyl chloride (PVC) microplastics and are a cause of concern. Therefore, the leaching kinetics of additives, including the influence of environmental weathering, are key to assessing exposure concentrations but remain largely unknown. We show that photoaging strongly enhances the leaching rates of di(2-ethylhexyl) phthalate (DEHP) by a factor of 1.5, and newly-formed harmful transformation products, such as mono(2-ethylhexyl) phthalate (MEHP), phthalic acid, and phthalic anhydride from PVC microplastics into the aquatic environment. Leaching half-lives of DEHP reduced from 449 years for pristine PVC to 121 years for photoaged PVC. Aqueous boundary layer diffusion (ABLD) is the limiting mass transfer process for the release of DEHP from pristine and photoaged PVC microplastics. The leaching of transformation products is limited by intraparticle diffusion (IPD). The calculated mass transfer rates can be used to predict exposure concentrations of harmful additives in the aquatic environment. The environmental weathering of plastics and the leaching kinetics of additives are key to assessing exposure concentrations. Here, the authors show that photoaging enhances the leaching rate of the common additive di(2-ethylhexyl) phthalate (DEHP) by a factor of 1.5, and newly-formed harmful transformation products, such as mono(2-ethylhexyl) phthalate (MEHP), phthalic acid, and phthalic anhydride, are released from PVC microplastics into the aquatic environment.
{"title":"Photoaging enhances the leaching of di(2-ethylhexyl) phthalate and transformation products from polyvinyl chloride microplastics into aquatic environments","authors":"Charlotte Henkel, Thorsten Hüffer, Ruoting Peng, Xiaoyu Gao, Subhasis Ghoshal, Thilo Hofmann","doi":"10.1038/s42004-024-01310-3","DOIUrl":"10.1038/s42004-024-01310-3","url":null,"abstract":"Increasing chemical pollution is a threat to sustainable water resources worldwide. Plastics and harmful additives released from plastics add to this burden and might pose a risk to aquatic organisms, and human health. Phthalates, which are common plasticizers and endocrine-disrupting chemicals, are released from polyvinyl chloride (PVC) microplastics and are a cause of concern. Therefore, the leaching kinetics of additives, including the influence of environmental weathering, are key to assessing exposure concentrations but remain largely unknown. We show that photoaging strongly enhances the leaching rates of di(2-ethylhexyl) phthalate (DEHP) by a factor of 1.5, and newly-formed harmful transformation products, such as mono(2-ethylhexyl) phthalate (MEHP), phthalic acid, and phthalic anhydride from PVC microplastics into the aquatic environment. Leaching half-lives of DEHP reduced from 449 years for pristine PVC to 121 years for photoaged PVC. Aqueous boundary layer diffusion (ABLD) is the limiting mass transfer process for the release of DEHP from pristine and photoaged PVC microplastics. The leaching of transformation products is limited by intraparticle diffusion (IPD). The calculated mass transfer rates can be used to predict exposure concentrations of harmful additives in the aquatic environment. The environmental weathering of plastics and the leaching kinetics of additives are key to assessing exposure concentrations. Here, the authors show that photoaging enhances the leaching rate of the common additive di(2-ethylhexyl) phthalate (DEHP) by a factor of 1.5, and newly-formed harmful transformation products, such as mono(2-ethylhexyl) phthalate (MEHP), phthalic acid, and phthalic anhydride, are released from PVC microplastics into the aquatic environment.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-10"},"PeriodicalIF":5.9,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01310-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142328598","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-25DOI: 10.1038/s42004-024-01302-3
Dr Ritika Gautam-Singh is an Assistant Professor at the Indian Institute of Technology Kanpur, India, where she leads a research group focused on medicinal inorganic chemistry.
{"title":"Women in chemistry: Q&A with Dr Ritika Gautam-Singh","authors":"","doi":"10.1038/s42004-024-01302-3","DOIUrl":"10.1038/s42004-024-01302-3","url":null,"abstract":"Dr Ritika Gautam-Singh is an Assistant Professor at the Indian Institute of Technology Kanpur, India, where she leads a research group focused on medicinal inorganic chemistry.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-2"},"PeriodicalIF":5.9,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01302-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142320934","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-25DOI: 10.1038/s42004-024-01291-3
Prof. Hyunjoo Lee is a Full Professor in the Department of Chemical and Biomolecular Engineering at the Korea Advanced Institute of Science & Technology (KAIST), Korea, and a KAIST Endowed Chair Professor. She also serves as the Director of the Heterogeneous Atomic Catalysts Research Center.
Hyunjoo Lee 教授是韩国科学技术院 (KAIST) 化学与生物分子工程系的全职教授和 KAIST 捐赠讲座教授。她还担任异相原子催化剂研究中心主任。
{"title":"Women in chemistry: Q&A with Professor Hyunjoo Lee","authors":"","doi":"10.1038/s42004-024-01291-3","DOIUrl":"10.1038/s42004-024-01291-3","url":null,"abstract":"Prof. Hyunjoo Lee is a Full Professor in the Department of Chemical and Biomolecular Engineering at the Korea Advanced Institute of Science & Technology (KAIST), Korea, and a KAIST Endowed Chair Professor. She also serves as the Director of the Heterogeneous Atomic Catalysts Research Center.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-2"},"PeriodicalIF":5.9,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01291-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142320940","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-25DOI: 10.1038/s42004-024-01290-4
Dr. Stefanie Flohr serves as an Associate Director at Novartis Biomedical Research in Basel, Switzerland.
Stefanie Flohr 博士是瑞士巴塞尔诺华生物医学研究公司的副主任。
{"title":"Women in chemistry: Q&A with Dr. Stefanie Flohr","authors":"","doi":"10.1038/s42004-024-01290-4","DOIUrl":"10.1038/s42004-024-01290-4","url":null,"abstract":"Dr. Stefanie Flohr serves as an Associate Director at Novartis Biomedical Research in Basel, Switzerland.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-2"},"PeriodicalIF":5.9,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01290-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142320936","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Women in chemistry: Q&A with Dr Janelle Sauvageau","authors":"","doi":"10.1038/s42004-024-01277-1","DOIUrl":"10.1038/s42004-024-01277-1","url":null,"abstract":"Dr Janelle Sauvageau is a carbohydrate chemist within the Human Health Therapeutics Research Centre at the National Research Council of Canada (NRC).","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-2"},"PeriodicalIF":5.9,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01277-1.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142320926","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-19DOI: 10.1038/s42004-024-01292-2
Shixuan Du is a Professor at the Institute of Physics, Chinese Academy of Sciences, in China. Shixuan’s research focuses on the interface properties and assembly mechanism of molecules on substrates, and the design of novel low-dimensional materials by using first-principle computational methods based on density functional theory as the main research tools.
{"title":"Women in chemistry: Q&A with Professor Shixuan Du","authors":"","doi":"10.1038/s42004-024-01292-2","DOIUrl":"10.1038/s42004-024-01292-2","url":null,"abstract":"Shixuan Du is a Professor at the Institute of Physics, Chinese Academy of Sciences, in China. Shixuan’s research focuses on the interface properties and assembly mechanism of molecules on substrates, and the design of novel low-dimensional materials by using first-principle computational methods based on density functional theory as the main research tools.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-1"},"PeriodicalIF":5.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01292-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142273315","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-18DOI: 10.1038/s42004-024-01306-z
Gad Licht, Kyle Hofstetter, Xirui Wang, Stuart Licht
The molten Li2CO3 transformation of CO2 to oxygen and graphene nanocarbons (GNCs), such as carbon nanotubes, is a large scale process of CO2 removal to mitigate climate change. Sustainability benefits include the stability and storage of the products, and the GNC product value is an incentive for carbon removal. However, high Li2CO3 cost and its competitive use as the primary raw material for EV batteries are obstacles. Common alternative alkali or alkali earth carbonates are ineffective substitutes due to impure GNC products or high energy limitations. A new decarbonization chemistry utilizing a majority of SrCO3 is investigated. SrCO3 is much more abundant, and an order of magnitude less expensive, than Li2CO3. The equivalent affinities of SrCO3 and Li2CO3 for absorbing and releasing CO2 are demonstrated to be comparable, and are unlike all the other alkali and alkali earth carbonates. The temperature domain in which the CO2 transformation to GNCs can be effective is <800 °C. Although the solidus temperature of SrCO3 is 1494 °C, it is remarkably soluble in Li2CO3 at temperatures less than 800 °C, and the electrolysis energy is low. High purity CNTs are synthesized from CO2 respectively in SrCO3 based electrolytes containing 30% or less Li2CO3. The transformation of CO2 to oxygen and graphene nanocarbons using lithium carbonate as an electrolyte is a promising, large-scale process for CO2 removal and valorization, but lithium carbonate is already in high demand as an important battery material. Here, the authors report the use of strontium carbonate as an alternative electrolyte in the electrochemical reduction of CO2 to carbon nanotubes.
{"title":"A new electrolyte for molten carbonate decarbonization","authors":"Gad Licht, Kyle Hofstetter, Xirui Wang, Stuart Licht","doi":"10.1038/s42004-024-01306-z","DOIUrl":"10.1038/s42004-024-01306-z","url":null,"abstract":"The molten Li2CO3 transformation of CO2 to oxygen and graphene nanocarbons (GNCs), such as carbon nanotubes, is a large scale process of CO2 removal to mitigate climate change. Sustainability benefits include the stability and storage of the products, and the GNC product value is an incentive for carbon removal. However, high Li2CO3 cost and its competitive use as the primary raw material for EV batteries are obstacles. Common alternative alkali or alkali earth carbonates are ineffective substitutes due to impure GNC products or high energy limitations. A new decarbonization chemistry utilizing a majority of SrCO3 is investigated. SrCO3 is much more abundant, and an order of magnitude less expensive, than Li2CO3. The equivalent affinities of SrCO3 and Li2CO3 for absorbing and releasing CO2 are demonstrated to be comparable, and are unlike all the other alkali and alkali earth carbonates. The temperature domain in which the CO2 transformation to GNCs can be effective is <800 °C. Although the solidus temperature of SrCO3 is 1494 °C, it is remarkably soluble in Li2CO3 at temperatures less than 800 °C, and the electrolysis energy is low. High purity CNTs are synthesized from CO2 respectively in SrCO3 based electrolytes containing 30% or less Li2CO3. The transformation of CO2 to oxygen and graphene nanocarbons using lithium carbonate as an electrolyte is a promising, large-scale process for CO2 removal and valorization, but lithium carbonate is already in high demand as an important battery material. Here, the authors report the use of strontium carbonate as an alternative electrolyte in the electrochemical reduction of CO2 to carbon nanotubes.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-17"},"PeriodicalIF":5.9,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01306-z.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236102","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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