This study aimed to investigate the anticancer efficacy and underlying mechanism of novel platinum nanoclusters (Pt NCs) in osteosarcoma cell lines exhibiting distinct P53 expression profiles, namely MG-63 (P53−) and U2-OS (P53+). The findings revealed that Pt NCs exerted an inhibitory effect on proliferation, migration, and colony formation while promoting apoptosis in both MG-63 (P53−) and U2-OS (P53+) cells. The inhibitory effect on the malignant characteristics of MG-63 (P53−) cells was more obvious, indicating that the potential anticancer effect of Pt NCs was not dependent on P53. Animal experiments have substantiated the in vivo anticancer properties of Pt NCs, while also revealing their lower toxicity on cells and tissues. Pt NCs possess the ability to impede cell proliferation by inducing DNA damage and arresting the cell cycle in the G1 phase and possess the ability to promote BAX/Bcl-2/Caspase-3/mitochondrial apoptosis. Pt NCs may promote mitochondrial apoptosis by promoting damaging autophagy, thereby promoting cellular demise. This study has confirmed the P53-independent anticancer impact of Pt NCs on osteosarcoma in vitro and in vivo. Pt NCs may play a therapeutic role in more sensitive MG-63 (P53−) cells by promoting DNA damage to arrest the cell cycle, stimulating BAX/Bcl-2/Caspase-3/mitochondrial apoptosis, and initiating damaging autophagy.
{"title":"Novel platinum nanoclusters (Pt NCs) induce mitochondrial apoptosis and damaging autophagy for the treatment of osteosarcoma—from the perspective of P53 mutation status in different cell lines","authors":"Jialin Wang, Haodi Yue, Xin Huang, Hongjian Liu, Mengjun Zhang","doi":"10.1038/s41427-024-00573-5","DOIUrl":"10.1038/s41427-024-00573-5","url":null,"abstract":"This study aimed to investigate the anticancer efficacy and underlying mechanism of novel platinum nanoclusters (Pt NCs) in osteosarcoma cell lines exhibiting distinct P53 expression profiles, namely MG-63 (P53−) and U2-OS (P53+). The findings revealed that Pt NCs exerted an inhibitory effect on proliferation, migration, and colony formation while promoting apoptosis in both MG-63 (P53−) and U2-OS (P53+) cells. The inhibitory effect on the malignant characteristics of MG-63 (P53−) cells was more obvious, indicating that the potential anticancer effect of Pt NCs was not dependent on P53. Animal experiments have substantiated the in vivo anticancer properties of Pt NCs, while also revealing their lower toxicity on cells and tissues. Pt NCs possess the ability to impede cell proliferation by inducing DNA damage and arresting the cell cycle in the G1 phase and possess the ability to promote BAX/Bcl-2/Caspase-3/mitochondrial apoptosis. Pt NCs may promote mitochondrial apoptosis by promoting damaging autophagy, thereby promoting cellular demise. This study has confirmed the P53-independent anticancer impact of Pt NCs on osteosarcoma in vitro and in vivo. Pt NCs may play a therapeutic role in more sensitive MG-63 (P53−) cells by promoting DNA damage to arrest the cell cycle, stimulating BAX/Bcl-2/Caspase-3/mitochondrial apoptosis, and initiating damaging autophagy.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-13"},"PeriodicalIF":8.6,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00573-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187387","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hysteresis is an inherent property of first-order transition materials that poses challenges for solid-state refrigeration applications. Extensive research has been conducted, but the intrinsic origins of hysteresis remain poorly understood. Here, we report a study of the kinetic origin of hysteresis and the enhanced barocaloric effect (BCE) in MnCoGe-based alloys with ~2% nonmagnetic In atoms. First-principles calculations demonstrate that substituting In atoms at Ge sites rather than Co sites results in a lower energy barrier, indicating a narrower hysteresis for the former. Combining neutron powder diffraction (NPD) with magnetic and calorimetric measurements completely verified the theoretical prediction. Electron local function (ELF) calculations further reveal the atomic coordination origin of regulated hysteresis due to weaker Co–Ge bonds when In atoms replace Ge, which is opposite to Co sites. Moreover, we experimentally investigate the BCE and find that although MnCo(Ge0.98In0.02) has a lower barocaloric entropy change ΔSP than does Mn(Co0.98In0.02)Ge, the reversible ΔSrev of the former is advantageous owing to a smaller hysteresis. The maximum ΔSrev of MnCo(Ge0.98In0.02) is 1.7 times greater than that of Mn(Co0.98In0.02)Ge. These results reveal the atomic-scale mechanism regulating hysteresis and provide insights into tailoring the functional properties of novel caloric refrigeration materials. First-principles calculations demonstrated that the substitution of In for Ge has a lower energy barrier for phase transition than the substitution of In for Co in MnCoGe alloys. ELF calculations further reveal the regulated hysteresis’s atomic coordination origin. This theoretical prediction is completely verified by combining neutron, magnetic and calorimetric measurements; consequently, a largely enhanced barocaloric effect has been achieved. Hysteresis is an inherent property of first-order transition materials that poses challenges for solid-state refrigeration applications. Here we report a study of the kinetic origin of hysteresis and enhanced barocaloric effect (BCE) in MnCoGe-based alloys with about 2% non-magnetic In atoms. First-principles calculations demonstrated that the substitution of In for Ge has a lower energy barrier of phase transition than the substitution of In for Co in MnCoGe alloys, indicating a narrower hysteresis for the former. Electron local function (ELF) calculations further reveal the atomic coordination origin of regulated hysteresis due to weaker Co-Ge bonds when In atoms replaced Ge, opposite to Co sites. Such theoretical prediction is completely verified by combining neutron with magnetic and calorimetric measurements, consequently strongly enhanced reversible BCE has been achieved. These results uncover the atomic-scale mechanism regulating hysteresis and provide insights for tailoring functional properties of novel caloric refrigeration materials.
{"title":"Kinetic origin of hysteresis and the strongly enhanced reversible barocaloric effect by regulating the atomic coordination environment","authors":"Zi-Bing Yu, Hou-Bo Zhou, Feng-Xia Hu, Jian-Tao Wang, Fei-Ran Shen, Lun-Hua He, Zheng-Ying Tian, Yi-Hong Gao, Bing-Jie Wang, Yuan Lin, Yue Kan, Jing Wang, Yun-Zhong Chen, Ji-Rong Sun, Tong-Yun Zhao, Bao-Gen Shen","doi":"10.1038/s41427-024-00571-7","DOIUrl":"10.1038/s41427-024-00571-7","url":null,"abstract":"Hysteresis is an inherent property of first-order transition materials that poses challenges for solid-state refrigeration applications. Extensive research has been conducted, but the intrinsic origins of hysteresis remain poorly understood. Here, we report a study of the kinetic origin of hysteresis and the enhanced barocaloric effect (BCE) in MnCoGe-based alloys with ~2% nonmagnetic In atoms. First-principles calculations demonstrate that substituting In atoms at Ge sites rather than Co sites results in a lower energy barrier, indicating a narrower hysteresis for the former. Combining neutron powder diffraction (NPD) with magnetic and calorimetric measurements completely verified the theoretical prediction. Electron local function (ELF) calculations further reveal the atomic coordination origin of regulated hysteresis due to weaker Co–Ge bonds when In atoms replace Ge, which is opposite to Co sites. Moreover, we experimentally investigate the BCE and find that although MnCo(Ge0.98In0.02) has a lower barocaloric entropy change ΔSP than does Mn(Co0.98In0.02)Ge, the reversible ΔSrev of the former is advantageous owing to a smaller hysteresis. The maximum ΔSrev of MnCo(Ge0.98In0.02) is 1.7 times greater than that of Mn(Co0.98In0.02)Ge. These results reveal the atomic-scale mechanism regulating hysteresis and provide insights into tailoring the functional properties of novel caloric refrigeration materials. First-principles calculations demonstrated that the substitution of In for Ge has a lower energy barrier for phase transition than the substitution of In for Co in MnCoGe alloys. ELF calculations further reveal the regulated hysteresis’s atomic coordination origin. This theoretical prediction is completely verified by combining neutron, magnetic and calorimetric measurements; consequently, a largely enhanced barocaloric effect has been achieved. Hysteresis is an inherent property of first-order transition materials that poses challenges for solid-state refrigeration applications. Here we report a study of the kinetic origin of hysteresis and enhanced barocaloric effect (BCE) in MnCoGe-based alloys with about 2% non-magnetic In atoms. First-principles calculations demonstrated that the substitution of In for Ge has a lower energy barrier of phase transition than the substitution of In for Co in MnCoGe alloys, indicating a narrower hysteresis for the former. Electron local function (ELF) calculations further reveal the atomic coordination origin of regulated hysteresis due to weaker Co-Ge bonds when In atoms replaced Ge, opposite to Co sites. Such theoretical prediction is completely verified by combining neutron with magnetic and calorimetric measurements, consequently strongly enhanced reversible BCE has been achieved. These results uncover the atomic-scale mechanism regulating hysteresis and provide insights for tailoring functional properties of novel caloric refrigeration materials.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-14"},"PeriodicalIF":8.6,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00571-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187386","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
On-demand underwater adhesives with excellent adhesive and gentle detachment properties enable stable connections to various biomedical devices and biointerfaces and avoid the risk of harmful tissue damage upon detachment. Herein, we present a Janus hydrogel adhesive that can reversibly switch its adhesion strength, which is controlled by temperature, using a thermoresponsive polymer and mussel-inspired molecules. This thermoswitchable adhesive (TSA) hydrogel displays both strong adhesion and gentle detachment with an over 1000-fold gap in underwater adhesion strength onto glass, titanium, aluminum, and Teflon substrates when exposed to temperatures above and below the lower critical solution temperature (LCST). The adhesion switch is possibly caused by the change in toughness of the TSA hydrogels with temperature because the Janus hydrogel possesses gradient crosslinked structures. Moreover, the lowermost surface is sufficiently soft to gently detach from the substrate below the LCST. The electrode-integrated hydrogel remains on human skin, and electrical signals are continuous over 10 min above the LCST. In contrast, commercially available hydrogel electrodes quickly swell and detach from the skin. The thermoswitchability of the TSA hydrogel, with its robust adhesion and gentle detachment, offers significant potential for biomedical applications characterized by minimally invasive procedures. On-demand underwater adhesives with excellent adhesive and gentle detachment properties enable stable connections to various biomedical devices and bio-interfaces and avoid the risk of harmful tissue damage upon detachment. Herein, we present a Janus hydrogel adhesive that can reversibly switch its adhesion strength, which is controlled by temperature, using a thermoresponsive polymer and mussel-inspired molecules. This thermoswitchable adhesive hydrogel displays both strong adhesion and gentle detachment with an over 1,000-fold gap in underwater adhesion strength. The thermoswitchability of the hydrogel adhesives, with its robust adhesion and gentle detachment, offers significant potential for biomedical applications characterized by minimally invasive procedures.
{"title":"Mussel-inspired thermo-switchable underwater adhesive based on a Janus hydrogel","authors":"Hiroya Abe, Daichi Yoshihara, Soichiro Tottori, Matsuhiko Nishizawa","doi":"10.1038/s41427-024-00569-1","DOIUrl":"10.1038/s41427-024-00569-1","url":null,"abstract":"On-demand underwater adhesives with excellent adhesive and gentle detachment properties enable stable connections to various biomedical devices and biointerfaces and avoid the risk of harmful tissue damage upon detachment. Herein, we present a Janus hydrogel adhesive that can reversibly switch its adhesion strength, which is controlled by temperature, using a thermoresponsive polymer and mussel-inspired molecules. This thermoswitchable adhesive (TSA) hydrogel displays both strong adhesion and gentle detachment with an over 1000-fold gap in underwater adhesion strength onto glass, titanium, aluminum, and Teflon substrates when exposed to temperatures above and below the lower critical solution temperature (LCST). The adhesion switch is possibly caused by the change in toughness of the TSA hydrogels with temperature because the Janus hydrogel possesses gradient crosslinked structures. Moreover, the lowermost surface is sufficiently soft to gently detach from the substrate below the LCST. The electrode-integrated hydrogel remains on human skin, and electrical signals are continuous over 10 min above the LCST. In contrast, commercially available hydrogel electrodes quickly swell and detach from the skin. The thermoswitchability of the TSA hydrogel, with its robust adhesion and gentle detachment, offers significant potential for biomedical applications characterized by minimally invasive procedures. On-demand underwater adhesives with excellent adhesive and gentle detachment properties enable stable connections to various biomedical devices and bio-interfaces and avoid the risk of harmful tissue damage upon detachment. Herein, we present a Janus hydrogel adhesive that can reversibly switch its adhesion strength, which is controlled by temperature, using a thermoresponsive polymer and mussel-inspired molecules. This thermoswitchable adhesive hydrogel displays both strong adhesion and gentle detachment with an over 1,000-fold gap in underwater adhesion strength. The thermoswitchability of the hydrogel adhesives, with its robust adhesion and gentle detachment, offers significant potential for biomedical applications characterized by minimally invasive procedures.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-11"},"PeriodicalIF":8.6,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00569-1.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187384","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Cross-luminescence (CL) in a barium fluoride (BaF2) scintillator arising from the recombination of a valence band electron and a core band hole results in a fast picosecond decay time. However, the CL emission wavelength in the vacuum ultraviolet region is difficult to detect, and intrinsically intense and slow nanosecond self-trapped exciton (STE) luminescence occurs. Herein, we report a redshift in the CL emission wavelength with high-pressure application. The wavelength of the CL emission shifted from 221 nm to 240 nm when 5.0 GPa was applied via a sapphire anvil cell. Increasing the pressure decreases the core-valence bandgap due to the downward expansion of the valence band, resulting in a decrease in the valence band minimum. The onset of a phase transition from a cubic crystal structure to an orthorhombic crystal structure at 3.7 GPa inhibited the recombination of conduction band electrons and self-trapped holes, leading to the disappearance of the STE emission. Manipulating the band structure of BaF2 by high-pressure application enables control of its luminescence emission, providing a pathway toward solving the problems inherent in this leading fast-response scintillator. Cross-luminescence (CL) in a barium fluoride arising from the recombination of a valence band electron and a core band hole, and intrinsically intense self-trapped exciton (STE) luminescence occurs. Herein, we report a redshift in the CL emission wavelength with high-pressure application via a sapphire anvil cell. Increasing the pressure decreases the core-valence bandgap due to the downward expansion of the valence band. The onset of a phase transition from a cubic crystal structure to an orthorhombic crystal structure at 3.7 GPa inhibited the recombination of conduction band electrons and self-trapped holes, leading to the disappearance of the STE emission.
{"title":"Pressure-controlled luminescence in fast-response barium fluoride crystals","authors":"Marilou Cadatal-Raduban, Luong Viet Mui, Masahiro Yamashita, Yuki Shibazaki, Toshihiko Shimizu, Nobuhiko Sarukura, Kohei Yamanoi","doi":"10.1038/s41427-024-00570-8","DOIUrl":"10.1038/s41427-024-00570-8","url":null,"abstract":"Cross-luminescence (CL) in a barium fluoride (BaF2) scintillator arising from the recombination of a valence band electron and a core band hole results in a fast picosecond decay time. However, the CL emission wavelength in the vacuum ultraviolet region is difficult to detect, and intrinsically intense and slow nanosecond self-trapped exciton (STE) luminescence occurs. Herein, we report a redshift in the CL emission wavelength with high-pressure application. The wavelength of the CL emission shifted from 221 nm to 240 nm when 5.0 GPa was applied via a sapphire anvil cell. Increasing the pressure decreases the core-valence bandgap due to the downward expansion of the valence band, resulting in a decrease in the valence band minimum. The onset of a phase transition from a cubic crystal structure to an orthorhombic crystal structure at 3.7 GPa inhibited the recombination of conduction band electrons and self-trapped holes, leading to the disappearance of the STE emission. Manipulating the band structure of BaF2 by high-pressure application enables control of its luminescence emission, providing a pathway toward solving the problems inherent in this leading fast-response scintillator. Cross-luminescence (CL) in a barium fluoride arising from the recombination of a valence band electron and a core band hole, and intrinsically intense self-trapped exciton (STE) luminescence occurs. Herein, we report a redshift in the CL emission wavelength with high-pressure application via a sapphire anvil cell. Increasing the pressure decreases the core-valence bandgap due to the downward expansion of the valence band. The onset of a phase transition from a cubic crystal structure to an orthorhombic crystal structure at 3.7 GPa inhibited the recombination of conduction band electrons and self-trapped holes, leading to the disappearance of the STE emission.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-12"},"PeriodicalIF":8.6,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00570-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187385","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Metal nanoparticles have extraordinary properties, but their integration into mesostructures has been challenging. Producing uniformly dispersed nanoparticles attached to substrates in industrial quantities is difficult. Herein, a “plasmashock” method was developed to synthesize metal nanoparticles anchored on different types of carbonaceous substrates using liquid salt solution precursors. These self-supporting, nanoparticle-loaded carbon fabrics are mechanically robust and have been tested as antibacterial substrates and electrocatalysts for reducing carbon dioxide and nitrite. A piece of silver–carbon nanotube paper with a silver loading of ~0.13 mg cm−2 treated after a few-second plasmashock presents good antibacterial and electrocatalytic properties in wastewater, even after 20 bactericidal immersion cycles, due to the strong bonding of the nanoparticles to the substrate. The results prove the effectiveness of this plasmashock method in creating free-standing functional composite films or membranes. A “plasmashock” method was developed to synthesize metal nanoparticles anchored on different kinds of carbonaceous substrates using liquid salt solution precursors. These self-supporting, nanoparticles-loaded carbon fabrics are mechanically robust and tested as antibacterial substrate and electrocatalysts for reducing carbon dioxide and nitrite.
{"title":"Burst plasma preparation of metallic nanoparticles on carbon fabrics for antibacterial and electrocatalytic applications","authors":"Guiyin Xu, Zheyi Meng, Yunteng Cao, Zixu Tao, Qing-Jie Li, Myles Stapelberg, Bing Han, Rui Gao, Qipeng Yu, Meng Gu, Benedetto Marelli, Hailiang Wang, Meifang Zhu, Ju Li","doi":"10.1038/s41427-024-00566-4","DOIUrl":"10.1038/s41427-024-00566-4","url":null,"abstract":"Metal nanoparticles have extraordinary properties, but their integration into mesostructures has been challenging. Producing uniformly dispersed nanoparticles attached to substrates in industrial quantities is difficult. Herein, a “plasmashock” method was developed to synthesize metal nanoparticles anchored on different types of carbonaceous substrates using liquid salt solution precursors. These self-supporting, nanoparticle-loaded carbon fabrics are mechanically robust and have been tested as antibacterial substrates and electrocatalysts for reducing carbon dioxide and nitrite. A piece of silver–carbon nanotube paper with a silver loading of ~0.13 mg cm−2 treated after a few-second plasmashock presents good antibacterial and electrocatalytic properties in wastewater, even after 20 bactericidal immersion cycles, due to the strong bonding of the nanoparticles to the substrate. The results prove the effectiveness of this plasmashock method in creating free-standing functional composite films or membranes. A “plasmashock” method was developed to synthesize metal nanoparticles anchored on different kinds of carbonaceous substrates using liquid salt solution precursors. These self-supporting, nanoparticles-loaded carbon fabrics are mechanically robust and tested as antibacterial substrate and electrocatalysts for reducing carbon dioxide and nitrite.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-11"},"PeriodicalIF":8.6,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00566-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187401","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-27DOI: 10.1038/s41427-024-00568-2
Eun Mi Kim, Jinseok Han, Guk-Tae Kim, Huan Li, Meng Yang Cui, Ganghwan Park, Dong-Ho Baek, Bo Jin, Sang Mun Jeong, Jae-Kwang Kim
The demand for high-capacity batteries with long cycle life and safety has been increasing owing to the expanding mid-to-large battery market. Li–S batteries are suitable energy-storage devices because of their reversibility, high theoretical capacity, and inexpensive construction materials. However, their performance is limited by various factors, including the shuttle effect and dendrite growth at the anode. Here, an integrated electrode for use in all-solid-state (ASS) Li–S batteries was formed via hot pressing. In detail, S particles dispersed in a functionalized reduced graphite oxide (rGO) cathode with a binder-less polymer electrolyte (PE) and a dual-anion ionic liquid-containing cross-linked poly(ethylene oxide)–Li bis(fluoromethanesulfonyl)imide–N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl) imide-based solid polymer electrolyte (SPE, PEO–LiFSI0.1(Pyr14TFSI)0.4) were hot-pressed into an integrated electrode, which serves as both the cathode and electrolyte. The resulting S/rGO-based solid-state Li–S batteries exhibited more stable performance than Li–S batteries using liquid electrolytes did, indicating that the dual-anion SPE layer effectively suppressed dendritic Li formation and the shuttle effect with high ionic conductivity. At 0.1 C, the battery discharge capacities were 957 and 576 mAh g−1 in the first cycle and after 100 cycles, respectively. At 1 C, the reversible capacity was 590 and 417 mAh g−1 in the first cycle and after 100 cycles, respectively (capacity retention = 71%). Therefore, the proposed S/rGO/PE//LiFSI0.1(Pyr14TFSI)0.4-integrated electrodes are beneficial for ASS Li–S batteries. Sulfur particles disperse in a functionalized reduced graphite oxide (rGO) cathode with a binder-less polymer electrolyte and a dual-anion ionic liquid-containing cross-linked PEO–LiFSI0.1(Pyr14TFSI)0.4 are hot-pressed into an integrated electrode, serving as both the cathode and electrolyte. Dual-anion solid polymer electrolyte and rGO-functional integrated sulfur electrode presents a novel method to improve the electrochemical properties of lithium-sulfur batteries.
{"title":"Sulfur/reduced graphite oxide and dual-anion solid polymer‒electrolyte integrated structure for high-loading practical all-solid-state lithium–sulfur batteries","authors":"Eun Mi Kim, Jinseok Han, Guk-Tae Kim, Huan Li, Meng Yang Cui, Ganghwan Park, Dong-Ho Baek, Bo Jin, Sang Mun Jeong, Jae-Kwang Kim","doi":"10.1038/s41427-024-00568-2","DOIUrl":"10.1038/s41427-024-00568-2","url":null,"abstract":"The demand for high-capacity batteries with long cycle life and safety has been increasing owing to the expanding mid-to-large battery market. Li–S batteries are suitable energy-storage devices because of their reversibility, high theoretical capacity, and inexpensive construction materials. However, their performance is limited by various factors, including the shuttle effect and dendrite growth at the anode. Here, an integrated electrode for use in all-solid-state (ASS) Li–S batteries was formed via hot pressing. In detail, S particles dispersed in a functionalized reduced graphite oxide (rGO) cathode with a binder-less polymer electrolyte (PE) and a dual-anion ionic liquid-containing cross-linked poly(ethylene oxide)–Li bis(fluoromethanesulfonyl)imide–N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl) imide-based solid polymer electrolyte (SPE, PEO–LiFSI0.1(Pyr14TFSI)0.4) were hot-pressed into an integrated electrode, which serves as both the cathode and electrolyte. The resulting S/rGO-based solid-state Li–S batteries exhibited more stable performance than Li–S batteries using liquid electrolytes did, indicating that the dual-anion SPE layer effectively suppressed dendritic Li formation and the shuttle effect with high ionic conductivity. At 0.1 C, the battery discharge capacities were 957 and 576 mAh g−1 in the first cycle and after 100 cycles, respectively. At 1 C, the reversible capacity was 590 and 417 mAh g−1 in the first cycle and after 100 cycles, respectively (capacity retention = 71%). Therefore, the proposed S/rGO/PE//LiFSI0.1(Pyr14TFSI)0.4-integrated electrodes are beneficial for ASS Li–S batteries. Sulfur particles disperse in a functionalized reduced graphite oxide (rGO) cathode with a binder-less polymer electrolyte and a dual-anion ionic liquid-containing cross-linked PEO–LiFSI0.1(Pyr14TFSI)0.4 are hot-pressed into an integrated electrode, serving as both the cathode and electrolyte. Dual-anion solid polymer electrolyte and rGO-functional integrated sulfur electrode presents a novel method to improve the electrochemical properties of lithium-sulfur batteries.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-13"},"PeriodicalIF":8.6,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00568-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187400","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The charge density wave (CDW), as a hallmark of vanadium-based kagome superconductor AV3Sb5 (A = K, Rb, Cs), has attracted intensive attention. However, the fundamental controversy regarding the underlying mechanism of CDW therein persists. Recently, the vanadium-based bi-layered kagome metal ScV6Sn6, reported to exhibit a long-range charge order below 94 K, has emerged as a promising candidate to further clarify this core issue. Here, employing micro-focusing angle-resolved photoemission spectroscopy (μ-ARPES) and first-principles calculations, we systematically studied the unique CDW order in vanadium-based bi-layered kagome metals by comparing ScV6Sn6 with its isostructural counterpart YV6Sn6, which lacks a CDW ground state. Combining ARPES data and the corresponding joint density of states (DOS), we suggest that the VHS nesting mechanism might be invalid in these materials. Besides, in ScV6Sn6, we identified multiple hybridization energy gaps resulting from CDW-induced band folding, along with an anomalous band dispersion, implying a potential electron-phonon coupling-driven mechanism underlying the formation of the CDW order. Our finding not only comprehensively maps the electronic structure of V-based bi-layer kagome metals but also provides constructive experimental evidence for the unique origin of CDW in this system. We investigated the origins of charge density wave (CDW) mechanisms in the bi-layered kagome metal ScV6Sn6 by comparing its electronic structure with that of its isostructural counterpart YV6Sn6, which does not exhibit a CDW state. Our ARPES measurements reveal that the Van Hove singularity (VHS) nesting mechanism may not be valid in the CDW state. In ScV6Sn6, the electronic structure shows a CDW-induced band gap accompanied by anomalous band dispersion near the M point of the Brillouin zone. These findings provide experimental evidence for the origin of CDW in vanadium-based kagome metals.
{"title":"Unveiling the charge density wave mechanism in vanadium-based Bi-layered kagome metals","authors":"Yi-Chen Yang, Soohyun Cho, Tong-Rui Li, Xiang-Qi Liu, Zheng-Tai Liu, Zhi-Cheng Jiang, Jian-Yang Ding, Wei Xia, Zi-Cheng Tao, Jia-Yu Liu, Wen-Chuan Jing, Yu Huang, Yu-Ming Shi, Soonsang Huh, Takeshi Kondo, Zhe Sun, Ji-Shan Liu, Mao Ye, Yi-Lin Wang, Yan-Feng Guo, Da-Wei Shen","doi":"10.1038/s41427-024-00567-3","DOIUrl":"10.1038/s41427-024-00567-3","url":null,"abstract":"The charge density wave (CDW), as a hallmark of vanadium-based kagome superconductor AV3Sb5 (A = K, Rb, Cs), has attracted intensive attention. However, the fundamental controversy regarding the underlying mechanism of CDW therein persists. Recently, the vanadium-based bi-layered kagome metal ScV6Sn6, reported to exhibit a long-range charge order below 94 K, has emerged as a promising candidate to further clarify this core issue. Here, employing micro-focusing angle-resolved photoemission spectroscopy (μ-ARPES) and first-principles calculations, we systematically studied the unique CDW order in vanadium-based bi-layered kagome metals by comparing ScV6Sn6 with its isostructural counterpart YV6Sn6, which lacks a CDW ground state. Combining ARPES data and the corresponding joint density of states (DOS), we suggest that the VHS nesting mechanism might be invalid in these materials. Besides, in ScV6Sn6, we identified multiple hybridization energy gaps resulting from CDW-induced band folding, along with an anomalous band dispersion, implying a potential electron-phonon coupling-driven mechanism underlying the formation of the CDW order. Our finding not only comprehensively maps the electronic structure of V-based bi-layer kagome metals but also provides constructive experimental evidence for the unique origin of CDW in this system. We investigated the origins of charge density wave (CDW) mechanisms in the bi-layered kagome metal ScV6Sn6 by comparing its electronic structure with that of its isostructural counterpart YV6Sn6, which does not exhibit a CDW state. Our ARPES measurements reveal that the Van Hove singularity (VHS) nesting mechanism may not be valid in the CDW state. In ScV6Sn6, the electronic structure shows a CDW-induced band gap accompanied by anomalous band dispersion near the M point of the Brillouin zone. These findings provide experimental evidence for the origin of CDW in vanadium-based kagome metals.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-9"},"PeriodicalIF":8.6,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00567-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187399","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-13DOI: 10.1038/s41427-024-00565-5
Zhendong Li, Xinxin Wang, Kexin Zeng, Zichao Guo, Chong Li, Xiang Yu, Seeram Ramakrishna, Zhonggang Wang, Yang Lu
In practical engineering, noise and impact hazards are pervasive, indicating the pressing demand for materials that can absorb both sound and stress wave energy simultaneously. However, the rational design of such multifunctional materials remains a challenge. Herein, inspired by cuttlebone, we present bioinspired architected metamaterials with unprecedented sound-absorbing and mechanical properties engineered via a weakly-coupled design. The acoustic elements feature heterogeneous multilayered resonators, whereas the mechanical responses are based on asymmetric cambered cell walls. These metamaterials experimentally demonstrated an average absorption coefficient of 0.80 from 1.0 to 6.0 kHz, with 77% of the data points exceeding the desired 0.75 threshold, all with a compact 21 mm thickness. An absorptance-thickness map is devised for assessing the sound-absorption efficiency. The high-fidelity microstructure-based model reveals the air friction damping mechanism, with broadband behavior attributed to multimodal hybrid resonance. Empowered by the cambered design of cell walls, metamaterials shift catastrophic failure toward a progressive deformation mode characterized by stable stress plateaus and ultrahigh specific energy absorption of 50.7 J/g—a 558.4% increase over the straight-wall design. After the deformation mechanisms are elucidated, a comprehensive research framework for burgeoning acousto-mechanical metamaterials is proposed. Overall, our study broadens the horizon for multifunctional material design. Noise and impact hazards are pervasive in engineering, necessitating materials capable of absorbing both sound and stress wave energy. Here, we present bioinspired metamaterials with exceptional sound-absorbing and mechanical properties using a weakly-coupled design strategy. These materials incorporate multi-layered resonators for superior acoustic performance and cambered cell walls for enhanced structural strength. They achieve an average absorption coefficient of 0.80 across the 1.0 to 6.0 kHz range, all within a sleek 21 mm thickness. Furthermore, the design transitions failure modes from catastrophic to progressive, resulting in a remarkable 558.4% increase in energy absorption compared to conventional designs.
{"title":"Unprecedented mechanical wave energy absorption observed in multifunctional bioinspired architected metamaterials","authors":"Zhendong Li, Xinxin Wang, Kexin Zeng, Zichao Guo, Chong Li, Xiang Yu, Seeram Ramakrishna, Zhonggang Wang, Yang Lu","doi":"10.1038/s41427-024-00565-5","DOIUrl":"10.1038/s41427-024-00565-5","url":null,"abstract":"In practical engineering, noise and impact hazards are pervasive, indicating the pressing demand for materials that can absorb both sound and stress wave energy simultaneously. However, the rational design of such multifunctional materials remains a challenge. Herein, inspired by cuttlebone, we present bioinspired architected metamaterials with unprecedented sound-absorbing and mechanical properties engineered via a weakly-coupled design. The acoustic elements feature heterogeneous multilayered resonators, whereas the mechanical responses are based on asymmetric cambered cell walls. These metamaterials experimentally demonstrated an average absorption coefficient of 0.80 from 1.0 to 6.0 kHz, with 77% of the data points exceeding the desired 0.75 threshold, all with a compact 21 mm thickness. An absorptance-thickness map is devised for assessing the sound-absorption efficiency. The high-fidelity microstructure-based model reveals the air friction damping mechanism, with broadband behavior attributed to multimodal hybrid resonance. Empowered by the cambered design of cell walls, metamaterials shift catastrophic failure toward a progressive deformation mode characterized by stable stress plateaus and ultrahigh specific energy absorption of 50.7 J/g—a 558.4% increase over the straight-wall design. After the deformation mechanisms are elucidated, a comprehensive research framework for burgeoning acousto-mechanical metamaterials is proposed. Overall, our study broadens the horizon for multifunctional material design. Noise and impact hazards are pervasive in engineering, necessitating materials capable of absorbing both sound and stress wave energy. Here, we present bioinspired metamaterials with exceptional sound-absorbing and mechanical properties using a weakly-coupled design strategy. These materials incorporate multi-layered resonators for superior acoustic performance and cambered cell walls for enhanced structural strength. They achieve an average absorption coefficient of 0.80 across the 1.0 to 6.0 kHz range, all within a sleek 21 mm thickness. Furthermore, the design transitions failure modes from catastrophic to progressive, resulting in a remarkable 558.4% increase in energy absorption compared to conventional designs.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-14"},"PeriodicalIF":8.6,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00565-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142216206","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-06DOI: 10.1038/s41427-024-00564-6
Geunyong Kim, Jinyoung Yun, Jinho Yang, Ilkyu Yang, Dirk Wulferding, Roman Movshovich, Gil Young Cho, Ki-Seok Kim, Garam Hahn, Jeehoon Kim
Geometrically confined superconductors often experience a breakdown in the quantization of magnetic flux owing to the incomplete screening of the supercurrent against field penetration. In this study, we report that magnetic field confinement occurs regardless of the dimensionality of the system, even extending to 1D linear potential systems. By using a vector-field magnetic force microscope, we successfully create a vortex‒antivortex pair connected by a 1D unquantized magnetic flux in ultrathin superconducting films. Through an investigation of the manipulation and thermal behavior of the vortex pair, we uncover a long-range interaction mediated by the unquantized magnetic flux. These findings suggest a universal phenomenon of unquantized magnetic flux formation, independent of the geometry of the system. Our results present an experimental route for investigating the impact of confinement on superconducting properties and order parameters in unconventional superconductors characterized by extremely low dimensionality. We demonstrate a 1D linear potential system in superconducting films by creating vortex-antivortex pairs linked by either quantized or unquantized magnetic flux. Our study of vortex pair manipulation and thermal behavior reveals a 1D force mediated by unquantized magnetic flux. This discovery suggests a universal mechanism for forming 1D force systems, offering a new paradigm in the physics of 1D forces.
{"title":"Vortex confinement through an unquantized magnetic flux","authors":"Geunyong Kim, Jinyoung Yun, Jinho Yang, Ilkyu Yang, Dirk Wulferding, Roman Movshovich, Gil Young Cho, Ki-Seok Kim, Garam Hahn, Jeehoon Kim","doi":"10.1038/s41427-024-00564-6","DOIUrl":"10.1038/s41427-024-00564-6","url":null,"abstract":"Geometrically confined superconductors often experience a breakdown in the quantization of magnetic flux owing to the incomplete screening of the supercurrent against field penetration. In this study, we report that magnetic field confinement occurs regardless of the dimensionality of the system, even extending to 1D linear potential systems. By using a vector-field magnetic force microscope, we successfully create a vortex‒antivortex pair connected by a 1D unquantized magnetic flux in ultrathin superconducting films. Through an investigation of the manipulation and thermal behavior of the vortex pair, we uncover a long-range interaction mediated by the unquantized magnetic flux. These findings suggest a universal phenomenon of unquantized magnetic flux formation, independent of the geometry of the system. Our results present an experimental route for investigating the impact of confinement on superconducting properties and order parameters in unconventional superconductors characterized by extremely low dimensionality. We demonstrate a 1D linear potential system in superconducting films by creating vortex-antivortex pairs linked by either quantized or unquantized magnetic flux. Our study of vortex pair manipulation and thermal behavior reveals a 1D force mediated by unquantized magnetic flux. This discovery suggests a universal mechanism for forming 1D force systems, offering a new paradigm in the physics of 1D forces.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-8"},"PeriodicalIF":8.6,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00564-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142216157","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-08-30DOI: 10.1038/s41427-024-00562-8
P. M. Tembo, C. Dyer, V. Subramanian
The current change in battery technology followed by the almost immediate adoption of lithium as a key resource powering our energy needs in various applications is undeniable. Lithium-ion batteries (LIBs) are at the forefront of the industry and offer excellent performance. The application of LIBs is expected to continue to increase. The adoption of renewable energies has spurred this LIB proliferation and resulted in a dramatic increase in LIB waste. In this review, we address waste LIB collection and segregation approaches, waste LIB treatment approaches, and related economics. We have coined a “green score” concept based on a review of several quantitative analyses from the literature to compare the three mainstream recycling processes: pyrometallurgical, hydrometallurgical, and direct recycling. In addition, we analyze the current trends in policymaking and in government incentive development directed toward promoting LIB waste recycling. Future LIB recycling perspectives are analyzed, and opportunities and threats to LIB recycling are presented. Lithium-ion battery (LIB) waste management is an integral part of the LIB circular economy. LIB refurbishing & repurposing and recycling can increase the useful life of LIBs and constituent materials, while serving as effective LIB waste management approaches. A combined effort by governments, industries and end-users will be integral in improving LIB waste collection rates which are largely lacking. A developed pseudo technical green score concept highlights direct recycling as a preferable recycling approach based on various life cycle assessment indicators. Standardized costing for the treatment of end-of-life LIBs shows pyrometallurgy as the least costly recycling approach.
{"title":"Lithium-ion battery recycling—a review of the material supply and policy infrastructure","authors":"P. M. Tembo, C. Dyer, V. Subramanian","doi":"10.1038/s41427-024-00562-8","DOIUrl":"10.1038/s41427-024-00562-8","url":null,"abstract":"The current change in battery technology followed by the almost immediate adoption of lithium as a key resource powering our energy needs in various applications is undeniable. Lithium-ion batteries (LIBs) are at the forefront of the industry and offer excellent performance. The application of LIBs is expected to continue to increase. The adoption of renewable energies has spurred this LIB proliferation and resulted in a dramatic increase in LIB waste. In this review, we address waste LIB collection and segregation approaches, waste LIB treatment approaches, and related economics. We have coined a “green score” concept based on a review of several quantitative analyses from the literature to compare the three mainstream recycling processes: pyrometallurgical, hydrometallurgical, and direct recycling. In addition, we analyze the current trends in policymaking and in government incentive development directed toward promoting LIB waste recycling. Future LIB recycling perspectives are analyzed, and opportunities and threats to LIB recycling are presented. Lithium-ion battery (LIB) waste management is an integral part of the LIB circular economy. LIB refurbishing & repurposing and recycling can increase the useful life of LIBs and constituent materials, while serving as effective LIB waste management approaches. A combined effort by governments, industries and end-users will be integral in improving LIB waste collection rates which are largely lacking. A developed pseudo technical green score concept highlights direct recycling as a preferable recycling approach based on various life cycle assessment indicators. Standardized costing for the treatment of end-of-life LIBs shows pyrometallurgy as the least costly recycling approach.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-20"},"PeriodicalIF":8.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00562-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142216179","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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