Communications Chemistry最新文献_第10页

Influence of the backbone chemistry and ionic functional groups of five pairs of oppositely charged polyelectrolytes on complex coacervation 五对带相反电荷的聚电解质的骨架化学和离子官能团对络合物凝聚的影响。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-15 DOI: 10.1038/s42004-024-01271-7

Yuri Hong, Surim Yoo, Jihoon Han, Junseong Kim, Yongjin Lee, YongSeok Jho, Youn Soo Kim, Dong Soo Hwang

{"title":"Influence of the backbone chemistry and ionic functional groups of five pairs of oppositely charged polyelectrolytes on complex coacervation","authors":"Yuri Hong, Surim Yoo, Jihoon Han, Junseong Kim, Yongjin Lee, YongSeok Jho, Youn Soo Kim, Dong Soo Hwang","doi":"10.1038/s42004-024-01271-7","DOIUrl":"10.1038/s42004-024-01271-7","url":null,"abstract":"Complex coacervation plays an important role in various fields. Here, the influences of the backbone chemistry and ionic functional groups of five pairs of oppositely charged polyelectrolytes on complex coacervation were investigated. These pairs include synthetic polymers with aliphatic hydrocarbon backbones, peptides with amide bonds, and carbohydrates with glycosidic linkages. Despite sharing identical charged groups, specific pairs displayed distinct liquid/liquid and liquid/solid phase separations depending on the polyelectrolyte mixing ratio, buffer, and ionic strength. The coacervate phase boundary broadened in the orders: glycosidic linkages > amide backbone > aliphatic hydrocarbon backbone, and Tris-phosphate > Tris-acetate > Tris-chloride buffers. Coacervates prepared from polyelectrolytes with lower solubilities in water resisted disassembly at high salt concentrations, and their merge rate was slow. These observations suggest that the hydrophobic segments in polyelectrolytes interfere with the formation of complex coacervates; however, following coacervate formation, the hydrophobic segments render the coacervates stable and elastic. Complex coacervation is propelled by the electrostatic association between oppositely charged polyelectrolytes, but the factors that drive complex coacervation have yet to be fully understood. Here, the authors investigate the influence of the backbone chemistry and ionic functional groups of five pairs of oppositely charged polyelectrolytes on complex coacervation.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-10"},"PeriodicalIF":5.9,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01271-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141987592","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}

引用次数: 0

Cyanine dyes in the mitochondria-targeting photodynamic and photothermal therapy 线粒体靶向光动力和光热疗法中的蓝染料。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-13 DOI: 10.1038/s42004-024-01256-6

Zdeněk Kejík, Jan Hajduch, Nikita Abramenko, Frédéric Vellieux, Kateřina Veselá, Jindřiška Leischner Fialová, Kateřina Petrláková, Kateřina Kučnirová, Robert Kaplánek, Ameneh Tatar, Markéta Skaličková, Michal Masařík, Petr Babula, Petr Dytrych, David Hoskovec, Pavel Martásek, Milan Jakubek

{"title":"Cyanine dyes in the mitochondria-targeting photodynamic and photothermal therapy","authors":"Zdeněk Kejík, Jan Hajduch, Nikita Abramenko, Frédéric Vellieux, Kateřina Veselá, Jindřiška Leischner Fialová, Kateřina Petrláková, Kateřina Kučnirová, Robert Kaplánek, Ameneh Tatar, Markéta Skaličková, Michal Masařík, Petr Babula, Petr Dytrych, David Hoskovec, Pavel Martásek, Milan Jakubek","doi":"10.1038/s42004-024-01256-6","DOIUrl":"10.1038/s42004-024-01256-6","url":null,"abstract":"Mitochondrial dysregulation plays a significant role in the carcinogenesis. On the other hand, its destabilization strongly represses the viability and metastatic potential of cancer cells. Photodynamic and photothermal therapies (PDT and PTT) target mitochondria effectively, providing innovative and non-invasive anticancer therapeutic modalities. Cyanine dyes, with strong mitochondrial selectivity, show significant potential in enhancing PDT and PTT. The potential and limitations of cyanine dyes for mitochondrial PDT and PTT are discussed, along with their applications in combination therapies, theranostic techniques, and optimal delivery systems. Additionally, novel approaches for sonodynamic therapy using photoactive cyanine dyes are presented, highlighting advances in cancer treatment. Photodynamic and photothermal therapies (PDT and PTT) target mitochondria effectively, providing innovative and non-invasive anticancer therapeutic modalities. Here, the authors summarize the promise and limitations of cyanine dyes in enhancing mitochondrial PDT and PTT in cancer treatment.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-39"},"PeriodicalIF":5.9,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11322665/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141975303","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}

引用次数: 0

Activity of botulinum neurotoxin X and its structure when shielded by a non-toxic non-hemagglutinin protein 肉毒杆菌神经毒素 X 的活性及其在无毒非凝集素蛋白保护下的结构

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-13 DOI: 10.1038/s42004-024-01262-8

Markel Martínez-Carranza, Jana Škerlová, Pyung-Gang Lee, Jie Zhang, Ajda Krč, Abhishek Sirohiwal, Dave Burgin, Mark Elliott, Jules Philippe, Sarah Donald, Fraser Hornby, Linda Henriksson, Geoffrey Masuyer, Ville R. I. Kaila, Matthew Beard, Min Dong, Pål Stenmark

{"title":"Activity of botulinum neurotoxin X and its structure when shielded by a non-toxic non-hemagglutinin protein","authors":"Markel Martínez-Carranza, Jana Škerlová, Pyung-Gang Lee, Jie Zhang, Ajda Krč, Abhishek Sirohiwal, Dave Burgin, Mark Elliott, Jules Philippe, Sarah Donald, Fraser Hornby, Linda Henriksson, Geoffrey Masuyer, Ville R. I. Kaila, Matthew Beard, Min Dong, Pål Stenmark","doi":"10.1038/s42004-024-01262-8","DOIUrl":"10.1038/s42004-024-01262-8","url":null,"abstract":"Botulinum neurotoxins (BoNTs) are the most potent toxins known and are used to treat an increasing number of medical disorders. All BoNTs are naturally co-expressed with a protective partner protein (NTNH) with which they form a 300 kDa complex, to resist acidic and proteolytic attack from the digestive tract. We have previously identified a new botulinum neurotoxin serotype, BoNT/X, that has unique and therapeutically attractive properties. We present the cryo-EM structure of the BoNT/X-NTNH/X complex and the crystal structure of the isolated NTNH protein. Unexpectedly, the BoNT/X complex is stable and protease-resistant at both neutral and acidic pH and disassembles only in alkaline conditions. Using the stabilizing effect of NTNH, we isolated BoNT/X and showed that it has very low potency both in vitro and in vivo. Given the high catalytic activity and translocation efficacy of BoNT/X, low activity of the full toxin is likely due to the receptor-binding domain, which presents very weak ganglioside binding and exposed hydrophobic surfaces. Botulinum neurotoxins (BoNTs) are a family of protein toxins produced by clostridial bacteria that cause muscle paralysis, and exhibit structural and functional diversity within the BoNTs family. Here, the authors report the cryo-EM structure complex of a newly identified serotype BoNT/X with their partner protein NTNH/X and reveal the complex’s pH-dependent stability and receptor-binding properties.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-15"},"PeriodicalIF":5.9,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01262-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141973749","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}

引用次数: 0

Electrodeposition of porous metal-organic frameworks for efficient charge storage 用于高效电荷存储的多孔金属有机框架的电沉积。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-10 DOI: 10.1038/s42004-024-01260-w

Deepa B. Bailmare, Boris V. Malozyomov, Abhay D. Deshmukh

{"title":"Electrodeposition of porous metal-organic frameworks for efficient charge storage","authors":"Deepa B. Bailmare, Boris V. Malozyomov, Abhay D. Deshmukh","doi":"10.1038/s42004-024-01260-w","DOIUrl":"10.1038/s42004-024-01260-w","url":null,"abstract":"Efficient charge storage is a key requirement for a range of applications, including energy storage devices and catalysis. Metal-organic frameworks are potential materials for efficient charge storage due to their self-supported three-dimensional design. MOFs are high surface area materials made up of coordination of appropriate amounts of metal ions and organic linkers, hence used in various applications. Yet, creating an effective MOF nanostructure with reduced random crystal formation continues to be a difficult task. The energy efficiency and electrochemical yield of bulk electrodes are improved in this study by demonstrating an effective technique for growing MOFs over a conducting substrate utilizing electrodeposition. An exceptionally stable asymmetric supercapacitor is created when activated carbon cloth is combined with the resulting MOF structure that was directly synthesized via an electrochemical method resulting in 97% stability over 5k cycles which is higher than conventional processes. High performance in supercapacitors is ensured by this practical approach for producing MOF electrodes, making it a suitable structure for effective charge storage. Metal-organic frameworks (MOFs) are promising charge storage materials due to their high surface area, tunable pore size, and chemical diversity, but reliable and easy syntheses of MOF conductors are needed. Here, the authors report the electrodeposition synthesis of highly conductive cobalt MOF films and their application in a supercapacitor with a power density of 480 Wkg-1 and 5k cycle stability.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-11"},"PeriodicalIF":5.9,"publicationDate":"2024-08-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s42004-024-01260-w.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141912043","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}

引用次数: 0

Photodetachment photoelectron spectroscopy shows isomer-specific proton-coupled electron transfer reactions in phenolic nitrate complexes 光脱附光电子能谱显示了酚类硝酸盐复合物中的同分异构质子耦合电子转移反应。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-09 DOI: 10.1038/s42004-024-01257-5

Qinqin Yuan, Ziheng Zhang, Xiangtao Kong, Zicheng Ling, Hanhui Zhang, Longjiu Cheng, Xue-Bin Wang

{"title":"Photodetachment photoelectron spectroscopy shows isomer-specific proton-coupled electron transfer reactions in phenolic nitrate complexes","authors":"Qinqin Yuan, Ziheng Zhang, Xiangtao Kong, Zicheng Ling, Hanhui Zhang, Longjiu Cheng, Xue-Bin Wang","doi":"10.1038/s42004-024-01257-5","DOIUrl":"10.1038/s42004-024-01257-5","url":null,"abstract":"The oxidation of phenolic compounds is one of the most important reactions prevalent in various biological processes, often explicitly coupled with proton transfers (PTs). Quantitative descriptions and molecular-level understanding of these proton-coupled electron transfer (PCET) reactions have been challenging. This work reports a direct observation of PCET in photodetachment (PD) photoelectron spectroscopy (PES) of hydrogen-bonded phenolic (ArOH) nitrate (NO3−) complexes, in which a much slower rising edge provides a spectroscopic signature to evidence PCET. Electronic structure calculations unveil the PCET processes to be isomer-specific, occurred only in those with their HOMOs localized on ArOH, leading to charge-separated transient states ArOH•+·NO3− triggered by ionizing phenols while simultaneously promoting PT from ArOH•+ to NO3−. Importantly, this study showcases that gas-phase PD-PES is a generic means enabling to identify PCET reactions with explicit structural and binding information. The oxidation of phenolic compounds is one of the most important reactions prevalent in various biological processes, but quantitative descriptions and molecular-level understanding of these proton-coupled electron transfer (PCET) reactions have been challenging. Here, the authors use photodetachment photoelectron spectroscopy to directly observe PCET in hydrogen-bonded phenolic nitrate complexes, in which a much slower rising edge provides a spectroscopic signature to evidence PCET","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-9"},"PeriodicalIF":5.9,"publicationDate":"2024-08-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11315994/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141912045","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}

引用次数: 0

Mechanism of allosteric inhibition of human p97/VCP ATPase and its disease mutant by triazole inhibitors 三唑类抑制剂对人类 p97/VCP ATPase 及其疾病突变体的异位抑制机制。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-09 DOI: 10.1038/s42004-024-01267-3

Purbasha Nandi, Kira DeVore, Feng Wang, Shan Li, Joel D. Walker, Thanh Tung Truong, Matthew G. LaPorte, Peter Wipf, Heidi Schlager, John McCleerey, William Paquette, Rod Carlo A. Columbres, Taiping Gan, Yu-Ping Poh, Petra Fromme, Andrew J. Flint, Mark Wolf, Donna M. Huryn, Tsui-Fen Chou, Po-Lin Chiu

{"title":"Mechanism of allosteric inhibition of human p97/VCP ATPase and its disease mutant by triazole inhibitors","authors":"Purbasha Nandi, Kira DeVore, Feng Wang, Shan Li, Joel D. Walker, Thanh Tung Truong, Matthew G. LaPorte, Peter Wipf, Heidi Schlager, John McCleerey, William Paquette, Rod Carlo A. Columbres, Taiping Gan, Yu-Ping Poh, Petra Fromme, Andrew J. Flint, Mark Wolf, Donna M. Huryn, Tsui-Fen Chou, Po-Lin Chiu","doi":"10.1038/s42004-024-01267-3","DOIUrl":"10.1038/s42004-024-01267-3","url":null,"abstract":"Human p97 ATPase is crucial in various cellular processes, making it a target for inhibitors to treat cancers, neurological, and infectious diseases. Triazole allosteric p97 inhibitors have been demonstrated to match the efficacy of CB-5083, an ATP-competitive inhibitor, in cellular models. However, the mechanism is not well understood. This study systematically investigates the structures of new triazole inhibitors bound to  both wild-type and disease mutant forms of p97 and measures their effects on function. These inhibitors bind at the interface of the D1 and D2 domains of each p97 subunit, shifting surrounding helices and altering the loop structures near the C-terminal α2 G helix to modulate domain-domain communications. A key structural moiety of the inhibitor affects the rotameric conformations of interacting side chains, indirectly modulating the N-terminal domain conformation in p97 R155H mutant. The differential effects of inhibitor binding to wild-type and mutant p97 provide insights into drug design with enhanced specificity, particularly for oncology applications. Human p97 ATPase, a critical drug target for neurodegenerative disorders and cancers, can be allosterically inhibited by triazole-based inhibitors. In this study, the authors investigate the structure and functions of newly designed triazole inhibitors in both wild-type and disease mutant forms of p97 to elucidate the previously unexplored inhibitory mechanisms, shedding new light on the design concept for p97 allosteric inhibitors.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-14"},"PeriodicalIF":5.9,"publicationDate":"2024-08-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11316111/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141912044","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}

引用次数: 0

Selection of antibody-binding covalent aptamers 筛选抗体结合型共价配合物。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-08 DOI: 10.1038/s42004-024-01255-7

Noah Soxpollard, Sebastian Strauss, Ralf Jungmann, Iain S. MacPherson

{"title":"Selection of antibody-binding covalent aptamers","authors":"Noah Soxpollard, Sebastian Strauss, Ralf Jungmann, Iain S. MacPherson","doi":"10.1038/s42004-024-01255-7","DOIUrl":"10.1038/s42004-024-01255-7","url":null,"abstract":"Aptamers are oligonucleotides with antibody-like binding function, selected from large combinatorial libraries. In this study, we modified a DNA aptamer library with N-hydroxysuccinimide esters, enabling covalent conjugation with cognate proteins. We selected for the ability to bind to mouse monoclonal antibodies, resulting in the isolation of two distinct covalent binding motifs. The covalent aptamers are specific for the Fc region of mouse monoclonal IgG1 and are cross-reactive with mouse IgG2a and other IgGs. Investigation into the covalent conjugation of the aptamers revealed a dependence on micromolar concentrations of Cu2+ ions which can be explained by residual catalyst remaining after modification of the aptamer library. The aptamers were successfully used as adapters in the formation of antibody-oligonucleotide conjugates (AOCs) for use in detection of HIV protein p24 and super-resolution imaging of actin. This work introduces a new method for the site-specific modification of native monoclonal antibodies and may be useful in applications requiring AOCs or other antibody conjugates. Site-specific conjugation of oligonucleotides and native proteins remains challenging. Here, the authors select covalent DNA aptamers from a library modified with N-hydroxysuccinimide esters, and show their application in the formation of antibody–oligonucleotide conjugates for protein detection.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-11"},"PeriodicalIF":5.9,"publicationDate":"2024-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11310417/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141906156","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}

引用次数: 0

A dual-functional electrolyte additive displaying hydrogen bond fusion enables highly reversible aqueous zinc ion batteries 一种显示氢键融合的双功能电解质添加剂可实现高度可逆的锌离子水电池。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-08 DOI: 10.1038/s42004-024-01259-3

Qiuxia Zhang, Xuan Gao, Kejiang Liu, Nan Gao, Shaoheng Cheng, Yuhang Dai, Haobo Dong, Junsong Liu, Guanjie He, Hongdong Li

{"title":"A dual-functional electrolyte additive displaying hydrogen bond fusion enables highly reversible aqueous zinc ion batteries","authors":"Qiuxia Zhang, Xuan Gao, Kejiang Liu, Nan Gao, Shaoheng Cheng, Yuhang Dai, Haobo Dong, Junsong Liu, Guanjie He, Hongdong Li","doi":"10.1038/s42004-024-01259-3","DOIUrl":"10.1038/s42004-024-01259-3","url":null,"abstract":"In recent years, aqueous zinc-ion batteries (AZIBs) have attracted significant attention in energy storage due to their notable advantages, including high safety, low cost, high capacity, and environmental friendliness. However, side reactions like hydrogen evolution and zinc (Zn) dendrites can significantly impact their Coulombic efficiency (CE) and lifespan. Effectively addressing these issues has become a focus of research in this field. In our study, dimethyl sulfoxide (DMSO) and nanodiamonds (NDs) were used to optimize the electrolyte of AZIBs. Benefiting from the hydrogen bond fusion of DMSO and NDs, which regulates the Zn deposition behavior, effectively inhibiting the growth of Zn dendrites, hydrogen evolution, and corrosion. The Zn | |Zn symmetric cells using NDs-DMSO-ZS demonstrate exceptional cycling stability for over 1500 h at 1 mA cm−2, while the Zn//Cu asymmetric cells achieve up to 99.8% CE at 2 mA cm−2. This study not only shows the application prospects of electrolyte optimization in enhancing AZIBs performance, but also provides a reference for the advancement of electrolyte technology in advanced AZIBs technology. Aqueous zinc ion batteries represent promising next-generation energy storage systems, but unwanted side reactions such as hydrogen evolution and zinc dendrite formation can significantly impact their Coulombic efficiency and lifespan. Here, dimethyl sulfoxide and nanodiamond additives are introduced to a ZnSO4 electrolyte, effectively inhibiting side reactions and dendrite formation through hydrogen bond fusion, and enabling exceptional cycling stability for over 1500 h at 1 mA cm−2.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-9"},"PeriodicalIF":5.9,"publicationDate":"2024-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11310298/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141906154","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}

引用次数: 0

Pressure induced structural and electronic band transition in CsPbBr3 CsPbBr3 中压力诱导的结构和电子能带转变。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-08 DOI: 10.1038/s42004-024-01265-5

Dongzhou Zhang, Sagarmoy Mandal, Duck Young Chung, Jingui Xu, Nannan Shan, Mercouri G. Kanatzidis, Ming Chen

{"title":"Pressure induced structural and electronic band transition in CsPbBr3","authors":"Dongzhou Zhang, Sagarmoy Mandal, Duck Young Chung, Jingui Xu, Nannan Shan, Mercouri G. Kanatzidis, Ming Chen","doi":"10.1038/s42004-024-01265-5","DOIUrl":"10.1038/s42004-024-01265-5","url":null,"abstract":"Cesium lead bromide (CsPbBr3) is a prominent halide perovskite with extensive optoelectronic applications. In this study, we report the pressure modulation of CsPbBr3’s crystal structure and electronic properties at room temperature up to 5 GPa. We have observed a crystal structure transition from the orthorhombic Pnma space group to a new monoclinic phase in the space group P21/c at 2.08 GPa. The structure is associated with ~8% of density jump across the transition boundary. DFT calculations have suggested that the structure transition leads to a change in the electronic band structure, and there is an emergent indirect bandgap at the Pnma-P21/c phase transition boundary at 2.08 GPa. Across the transition boundary, the electronic band gap of CsPbBr3 increased from 2.07 eV to 2.38 eV, which explains its pressure-induced color change. Our study demonstrates the importance of using in-situ crystal structure in the electronic band structure calculations in halide perovskites. CsPbBr3 is a characteristic halide perovskite with extensive optoelectronic application potential. Here, the authors report the pressure modulation of the crystal structure and electronic properties of CsPbBr3 at room temperature and pressures up to 5 GPa.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-7"},"PeriodicalIF":5.9,"publicationDate":"2024-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11310203/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141906155","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}

引用次数: 0

Nuclear spin polarization of lactic acid via exchange of parahydrogen-polarized protons 通过对氢极化质子的交换实现乳酸的核自旋极化。

IF 5.9 2区化学

Communications Chemistry Pub Date : 2024-08-08 DOI: 10.1038/s42004-024-01254-8

Kolja Them, Jule Kuhn, Andrey N. Pravdivtsev, Jan-Bernd Hövener

{"title":"Nuclear spin polarization of lactic acid via exchange of parahydrogen-polarized protons","authors":"Kolja Them, Jule Kuhn, Andrey N. Pravdivtsev, Jan-Bernd Hövener","doi":"10.1038/s42004-024-01254-8","DOIUrl":"10.1038/s42004-024-01254-8","url":null,"abstract":"Hyperpolarization has become a powerful tool to enhance the sensitivity of magnetic resonance. A universal tool to hyperpolarize small molecules in solution, however, has not yet emerged. Transferring hyperpolarized, labile protons between molecules is a promising approach towards this end. Therefore, hydrogenative parahydrogen-induced polarization (PHIP) was recently proposed as a source to polarize exchanging protons (PHIP-X). Here, we identified four key components that govern PHIP-X: adding the spin order, polarizing the labile proton, proton exchange, and polarization of the target nucleus. We investigated the last two steps experimentally and using simulations. We found optimal exchange rates and field cycling methods to polarize the target molecules. We also investigated the influence of spin relaxation of exchanging protons on the target polarization. It was found experimentally that transferring the polarization from protons directly bound to the target X-nucleus (here 13C) of lactate and methanol using a pulse sequence was more efficient than applying a corresponding sequence to the labile proton. Furthermore, varying the concentrations of the transfer and target molecules yielded a distinct maximum 13C polarization. We believe this work will further help to understand and optimize PHIP-X towards a broadly applicable hyperpolarization method. Hyperpolarization has become a powerful tool to enhance the sensitivity of NMR analyses, whereby hydrogenative parahydrogen-induced polarization with exchanging protons could broaden its applicability. Here, the authors identify four key components that govern the polarization of exchanging protons, and propose optimal exchange rates and field cycling methods to polarize target molecules.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":" ","pages":"1-11"},"PeriodicalIF":5.9,"publicationDate":"2024-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11306230/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141901184","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}

引用次数: 0