Pub Date : 2024-08-30DOI: 10.1038/s41427-024-00563-7
Rae-Hyun Lee, Chea-Yun Kang, Jong-Kyu Lee, Bong-Soo Jin, Kyong-Nam Kim, Hyun-Soo Kim, Jung-Rag Yoon, Seung-Hwan Lee
Garnet-type Li6.1Ga0.3La3Zr2O12 (LGLZO) exhibits high ionic conductivity and extremely low electronic conductivity. The electrochemical properties strongly depend on the characteristics of the grain boundaries and pores in the oxide–ceramic electrolyte. Currently, the main issue of LGLZO is its large grain boundary resistance due to high-temperature sintering. Herein, we propose an effective method for reinforcing the chemical and structural characteristics of the grain boundaries using a Li2O-B2O3-Al2O3 (LBA) sintering aid. In this study, the LBA sintering aid is critical because it fills grain boundaries and void spaces. As a result, LGLZO solid-state electrolytes with sintering aids significantly enhance the ionic conductivity and reduce the activation energy, especially in the grain boundary region. Another crucial issue is the formation of Li dendrites in LGLZO. Since dendritic Li propagates along the grain boundaries, the optimized LGLZO solid-state electrolyte demonstrates excellent stability against Li metals. Overall, the LGLZO electrolyte with the LBA sintering aid exhibits stable long-term cycling performance due to the well-designed grain boundaries. The addition of Li2O-B2O3-Al2O3 (LBA) sintering aid to Li6.1Ga0.3La3Zr2O12 (LGLZO) solid electrolytes enhances grain boundary characteristics and reduces porosity. This modification leads to a substantial increase in ionic conductivity and mechanical stability, while effectively preventing Li dendrite formation. The optimized LGLZO sample with LBA exhibits improved long-term cycling performance, making it a promising candidate for high-performance all-solid-state batteries. These findings underscore the critical role of grain boundary engineering in enhancing the electrochemical properties of garnet-type electrolytes.
{"title":"Tailoring the grain boundary structure and chemistry of the dendrite-free garnet solid electrolyte Li6.1Ga0.3La3Zr2O12","authors":"Rae-Hyun Lee, Chea-Yun Kang, Jong-Kyu Lee, Bong-Soo Jin, Kyong-Nam Kim, Hyun-Soo Kim, Jung-Rag Yoon, Seung-Hwan Lee","doi":"10.1038/s41427-024-00563-7","DOIUrl":"10.1038/s41427-024-00563-7","url":null,"abstract":"Garnet-type Li6.1Ga0.3La3Zr2O12 (LGLZO) exhibits high ionic conductivity and extremely low electronic conductivity. The electrochemical properties strongly depend on the characteristics of the grain boundaries and pores in the oxide–ceramic electrolyte. Currently, the main issue of LGLZO is its large grain boundary resistance due to high-temperature sintering. Herein, we propose an effective method for reinforcing the chemical and structural characteristics of the grain boundaries using a Li2O-B2O3-Al2O3 (LBA) sintering aid. In this study, the LBA sintering aid is critical because it fills grain boundaries and void spaces. As a result, LGLZO solid-state electrolytes with sintering aids significantly enhance the ionic conductivity and reduce the activation energy, especially in the grain boundary region. Another crucial issue is the formation of Li dendrites in LGLZO. Since dendritic Li propagates along the grain boundaries, the optimized LGLZO solid-state electrolyte demonstrates excellent stability against Li metals. Overall, the LGLZO electrolyte with the LBA sintering aid exhibits stable long-term cycling performance due to the well-designed grain boundaries. The addition of Li2O-B2O3-Al2O3 (LBA) sintering aid to Li6.1Ga0.3La3Zr2O12 (LGLZO) solid electrolytes enhances grain boundary characteristics and reduces porosity. This modification leads to a substantial increase in ionic conductivity and mechanical stability, while effectively preventing Li dendrite formation. The optimized LGLZO sample with LBA exhibits improved long-term cycling performance, making it a promising candidate for high-performance all-solid-state batteries. These findings underscore the critical role of grain boundary engineering in enhancing the electrochemical properties of garnet-type electrolytes.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-12"},"PeriodicalIF":8.6,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00563-7.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142216236","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}
Superconducting magnets based on high-temperature superconductors (HTSs) have become critical components in cutting-edge technologies such as advanced medical applications. In HTSs, weak links of superconductivity are inevitable at high-angle grain boundaries (GBs). Thus, two adjacent grains should be crystallographically aligned within the critical angle (θc), for which the intergrain critical current density (Jc) starts to decrease exponentially. The θc of several iron-based superconductors (IBSs) is larger than that of cuprates. However, the decreases in both θc and intergrain Jc under magnetic fields for IBSs are still substantial, hampering their applications in polycrystalline forms. Here, we report that potassium-doped BaFe2As2 (Ba122:K) exhibits superior GB performance to that of previously reported IBSs. A transport Jc of over 0.1 MA/cm2 across [001]-tilt GBs with misorientation angles up to θGB = 24° was recorded even at 28 K, which is a required level for practical applications. Additionally, even in an applied magnetic field, θc was unaltered, and the decay of the intergrain Jc was small. Our results highlight the exceptional potential of Ba122:K for polycrystalline applications and pave the way for next-generation superconducting magnets. We have fabricated artificial grain boundaries in K-doped BaFe2As2 (Ba122:K), one of the Fe-based superconductors. The crystalline orientation map, acquired through the scanning precession electron diffraction measurements, revealed that spontaneous connectivity modification occurred at the grain boundary, which may mitigate weak-link behavior. Specifically, a self-field critical current density Jc of over 0.1 MA/cm2 across the grain boundary with misorientation angles up to 24° was recorded even at 28 K. This performance surpasses the grain boundary properties of hitherto reported Fe-based superconductors. Our results highlight the exceptional potential of Ba122:K for polycrystalline applications and pave the way for next-generation superconducting magnets.
{"title":"High tolerance of the superconducting current to large grain boundary angles in potassium-doped BaFe2As2","authors":"Takafumi Hatano, Dongyi Qin, Kazumasa Iida, Hongye Gao, Zimeng Guo, Hikaru Saito, Satoshi Hata, Yusuke Shimada, Michio Naito, Akiyasu Yamamoto","doi":"10.1038/s41427-024-00561-9","DOIUrl":"10.1038/s41427-024-00561-9","url":null,"abstract":"Superconducting magnets based on high-temperature superconductors (HTSs) have become critical components in cutting-edge technologies such as advanced medical applications. In HTSs, weak links of superconductivity are inevitable at high-angle grain boundaries (GBs). Thus, two adjacent grains should be crystallographically aligned within the critical angle (θc), for which the intergrain critical current density (Jc) starts to decrease exponentially. The θc of several iron-based superconductors (IBSs) is larger than that of cuprates. However, the decreases in both θc and intergrain Jc under magnetic fields for IBSs are still substantial, hampering their applications in polycrystalline forms. Here, we report that potassium-doped BaFe2As2 (Ba122:K) exhibits superior GB performance to that of previously reported IBSs. A transport Jc of over 0.1 MA/cm2 across [001]-tilt GBs with misorientation angles up to θGB = 24° was recorded even at 28 K, which is a required level for practical applications. Additionally, even in an applied magnetic field, θc was unaltered, and the decay of the intergrain Jc was small. Our results highlight the exceptional potential of Ba122:K for polycrystalline applications and pave the way for next-generation superconducting magnets. We have fabricated artificial grain boundaries in K-doped BaFe2As2 (Ba122:K), one of the Fe-based superconductors. The crystalline orientation map, acquired through the scanning precession electron diffraction measurements, revealed that spontaneous connectivity modification occurred at the grain boundary, which may mitigate weak-link behavior. Specifically, a self-field critical current density Jc of over 0.1 MA/cm2 across the grain boundary with misorientation angles up to 24° was recorded even at 28 K. This performance surpasses the grain boundary properties of hitherto reported Fe-based superconductors. Our results highlight the exceptional potential of Ba122:K for polycrystalline applications and pave the way for next-generation superconducting magnets.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-10"},"PeriodicalIF":8.6,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00561-9.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142216238","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 : 2024-08-16DOI: 10.1038/s41427-024-00560-w
Yanhong Chu, LiFeng Wang, Yaohua Ke, Xiaoyu Feng, Wenmei Rao, Wei Ren, Kai Xin, Yan Wang, Lixia Yu, Baorui Liu, Qin Liu
Radiotherapy (RT) is a widely used treatment with strong therapeutic effects, but overcoming challenges related to hypoxia-induced tumor resistance and ineffective antitumor immune responses is crucial for optimal outcomes. In this study, we developed a versatile nanosystem using mesoporous silica nanoparticles (MSNs), R837, and a small quantity of manganese peroxide (Mn/ZnO2). The synthesized MSN@R837-Mn/ZnO2 nanoparticles exhibited precise tumor targeting and accumulation, controlled drug release under acidic conditions, and increased sensitivity in magnetic resonance imaging. These attributes collectively augmented the therapeutic efficacy of RT by alleviating hypoxia and immunosuppression. Tumor cells treated with RT combined with these nanoparticles displayed reduced oxidative stress, alleviated hypoxia, and normalized blood vessel formation. Notably, all mice in the RT + PD-1 + MSN@R837-Mn/ZnO2 group achieved complete tumor regression with extended survival. Safety assessments confirmed the absence of MSN@R837-Mn/ZnO2 toxicity, highlighting its potential as a promising approach with dual functionality for the diagnostic imaging and treatment of cancer. Radiotherapy (RT) faces challenges like hypoxia-induced tumor resistance and weak antitumor immune responses. This study developed a nanosystem using mesoporous silica nanoparticles (MSNs), R837, and manganese peroxide (Mn/ZnO2). The MSN@R837-Mn/ZnO2 nanoparticles showed precise tumor targeting, controlled drug release in acidic conditions, and enhanced MRI sensitivity, boosting RT efficacy by reducing hypoxia and immunosuppression. Tumor cells treated with RT and these nanoparticles had less oxidative stress, improved hypoxia, and normalized blood vessels. Remarkably, all mice in the RT+PD-1+MSN@R837-Mn/ZnO2 group achieved complete tumor regression and extended survival, with no toxicity observed, indicating its potential for cancer imaging and treatment.
{"title":"A multifunctional mesoporous silica drug delivery nanosystem that ameliorates tumor hypoxia and increases radiotherapy efficacy","authors":"Yanhong Chu, LiFeng Wang, Yaohua Ke, Xiaoyu Feng, Wenmei Rao, Wei Ren, Kai Xin, Yan Wang, Lixia Yu, Baorui Liu, Qin Liu","doi":"10.1038/s41427-024-00560-w","DOIUrl":"10.1038/s41427-024-00560-w","url":null,"abstract":"Radiotherapy (RT) is a widely used treatment with strong therapeutic effects, but overcoming challenges related to hypoxia-induced tumor resistance and ineffective antitumor immune responses is crucial for optimal outcomes. In this study, we developed a versatile nanosystem using mesoporous silica nanoparticles (MSNs), R837, and a small quantity of manganese peroxide (Mn/ZnO2). The synthesized MSN@R837-Mn/ZnO2 nanoparticles exhibited precise tumor targeting and accumulation, controlled drug release under acidic conditions, and increased sensitivity in magnetic resonance imaging. These attributes collectively augmented the therapeutic efficacy of RT by alleviating hypoxia and immunosuppression. Tumor cells treated with RT combined with these nanoparticles displayed reduced oxidative stress, alleviated hypoxia, and normalized blood vessel formation. Notably, all mice in the RT + PD-1 + MSN@R837-Mn/ZnO2 group achieved complete tumor regression with extended survival. Safety assessments confirmed the absence of MSN@R837-Mn/ZnO2 toxicity, highlighting its potential as a promising approach with dual functionality for the diagnostic imaging and treatment of cancer. Radiotherapy (RT) faces challenges like hypoxia-induced tumor resistance and weak antitumor immune responses. This study developed a nanosystem using mesoporous silica nanoparticles (MSNs), R837, and manganese peroxide (Mn/ZnO2). The MSN@R837-Mn/ZnO2 nanoparticles showed precise tumor targeting, controlled drug release in acidic conditions, and enhanced MRI sensitivity, boosting RT efficacy by reducing hypoxia and immunosuppression. Tumor cells treated with RT and these nanoparticles had less oxidative stress, improved hypoxia, and normalized blood vessels. Remarkably, all mice in the RT+PD-1+MSN@R837-Mn/ZnO2 group achieved complete tumor regression and extended survival, with no toxicity observed, indicating its potential for cancer imaging and treatment.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-17"},"PeriodicalIF":8.6,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00560-w.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142216239","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 : 2024-08-09DOI: 10.1038/s41427-024-00559-3
Jae Yeon Seo, Sunghyun Lim, Hyun Jun Shin, Ki Won Jeong, Jae Min Hong, Kyungsun Moon, Mi Kyung Kim, Nara Lee, Young Jai Choi
The influence of magnetocrystalline anisotropy (MCA) on antiferromagnetism is elucidated through the characterization of the spin‒flop transition. However, due to a lack of suitable candidates for investigation, a detailed understanding of the preservation of the spin‒flop transition in the presence of low MCA energy remains elusive. In this study, we introduce CrPS4, which is a two-dimensional van der Waals antiferromagnet, as an ideal system to explore the exceedingly weak limit of the thermally-evolved MCA energy. By employing a uniaxially anisotropic spin model and fitting it to the experimental magnetic properties, we quantify the MCA energy and identify the discernible spin configurations in different magnetic phases. Notably, even at the limit of extremely weak MCA, with a mere 0.12% of the interlayer antiferromagnetic exchange interaction at T = 33 K, which is slightly below the Néel temperature (TN) of 38 K, the spin‒flop transition remains intact. We further establish a direct correlation between the visualized spin arrangements and the progressive reversal of magnetic torque induced by rotating magnetic fields. This analysis reveals the essential role of MCA in antiferromagnetism, thus extending our understanding to previously undetected limits and providing valuable insights for the development of spin-processing functionalities based on van der Waals magnets. Though the impact of magnetic anisotropy on antiferromagnetism is manifested in spin-flop transition, understanding the preservation of this transition in weak anisotropy remains elusive. By adopting an anisotropic spin model, we find that the spin-flop transition remains intact in extremely weak anisotropy, with a mere 0.12% of interlayer exchange interaction at 33 K, slightly below the Néel temperature of 38 K. We further establish a direct relationship between the visualized spin arrangements and the progressive reversal of magnetic torque in rotating magnetic fields. Our analysis provides valuable insights for exploring novel phenomena in the realm of low-dimensional magnetism.
{"title":"Probing the weak limit of magnetocrystalline anisotropy through a spin‒flop transition in the van der Waals antiferromagnet CrPS4","authors":"Jae Yeon Seo, Sunghyun Lim, Hyun Jun Shin, Ki Won Jeong, Jae Min Hong, Kyungsun Moon, Mi Kyung Kim, Nara Lee, Young Jai Choi","doi":"10.1038/s41427-024-00559-3","DOIUrl":"10.1038/s41427-024-00559-3","url":null,"abstract":"The influence of magnetocrystalline anisotropy (MCA) on antiferromagnetism is elucidated through the characterization of the spin‒flop transition. However, due to a lack of suitable candidates for investigation, a detailed understanding of the preservation of the spin‒flop transition in the presence of low MCA energy remains elusive. In this study, we introduce CrPS4, which is a two-dimensional van der Waals antiferromagnet, as an ideal system to explore the exceedingly weak limit of the thermally-evolved MCA energy. By employing a uniaxially anisotropic spin model and fitting it to the experimental magnetic properties, we quantify the MCA energy and identify the discernible spin configurations in different magnetic phases. Notably, even at the limit of extremely weak MCA, with a mere 0.12% of the interlayer antiferromagnetic exchange interaction at T = 33 K, which is slightly below the Néel temperature (TN) of 38 K, the spin‒flop transition remains intact. We further establish a direct correlation between the visualized spin arrangements and the progressive reversal of magnetic torque induced by rotating magnetic fields. This analysis reveals the essential role of MCA in antiferromagnetism, thus extending our understanding to previously undetected limits and providing valuable insights for the development of spin-processing functionalities based on van der Waals magnets. Though the impact of magnetic anisotropy on antiferromagnetism is manifested in spin-flop transition, understanding the preservation of this transition in weak anisotropy remains elusive. By adopting an anisotropic spin model, we find that the spin-flop transition remains intact in extremely weak anisotropy, with a mere 0.12% of interlayer exchange interaction at 33 K, slightly below the Néel temperature of 38 K. We further establish a direct relationship between the visualized spin arrangements and the progressive reversal of magnetic torque in rotating magnetic fields. Our analysis provides valuable insights for exploring novel phenomena in the realm of low-dimensional magnetism.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-9"},"PeriodicalIF":8.6,"publicationDate":"2024-08-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00559-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141923705","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 : 2024-07-26DOI: 10.1038/s41427-024-00558-4
Sang-Mi Jeong, Jonguk Yang, Youngsoo Kang, Hee Sung Seo, Keumyoung Seo, Taekyung Lim, Sanghyun Ju
In this paper, we introduce an innovative approach for generating robotic faces with a thermal signature similar to that of humans and equipping prosthetic or robotic hands with a lifelike temperature distribution. This approach enhances their detection via infrared cameras and promotes more natural interactions between humans and robots. This method integrates a temperature regulation system into artificial skin, drawing inspiration from the human body’s natural temperature control via blood flow. Central to this technique is a fiber network simulating blood vessels within the artificial skin. Water flows through these fibers under specific temperature and flow conditions, forming a controlled heat release system. The heat emission can be adjusted by changing the dilation of these fibers, primarily by modulating the frequency of circulation. Our findings indicate that this approach can replicate the varied thermal characteristics of different human faces and hand areas. Consequently, the robotic faces appear more human-like in infrared images, aiding their identification by infrared cameras. At the same time, the prosthetic hands achieve a more natural temperature, reducing the discomfort typically felt in direct contact with synthetic limbs. The aim of this study was to address the challenges faced by the users of prosthetic hands. The results from this study show a promising direction in humanoid robotics, fostering improved tactile interactions and redefining human–robot relationships. This innovative technique facilitates further advancements, blurring the lines between artificial aids and natural biological systems. Robotic faces and hands with human-like thermal infrared emission and physiological temperature are achieved by replicating the circulatory system’s inherent temperature regulation mechanism. The keystone of our development is an intricate system of fibers, reminiscent of blood vessels, embedded within the artificial skin. The fiber network enables controlled heat dissipation by regulating water circulation to mimic human thermal signatures.
{"title":"Thermoregulatory integration in hand prostheses and humanoid robots through blood vessel simulation","authors":"Sang-Mi Jeong, Jonguk Yang, Youngsoo Kang, Hee Sung Seo, Keumyoung Seo, Taekyung Lim, Sanghyun Ju","doi":"10.1038/s41427-024-00558-4","DOIUrl":"10.1038/s41427-024-00558-4","url":null,"abstract":"In this paper, we introduce an innovative approach for generating robotic faces with a thermal signature similar to that of humans and equipping prosthetic or robotic hands with a lifelike temperature distribution. This approach enhances their detection via infrared cameras and promotes more natural interactions between humans and robots. This method integrates a temperature regulation system into artificial skin, drawing inspiration from the human body’s natural temperature control via blood flow. Central to this technique is a fiber network simulating blood vessels within the artificial skin. Water flows through these fibers under specific temperature and flow conditions, forming a controlled heat release system. The heat emission can be adjusted by changing the dilation of these fibers, primarily by modulating the frequency of circulation. Our findings indicate that this approach can replicate the varied thermal characteristics of different human faces and hand areas. Consequently, the robotic faces appear more human-like in infrared images, aiding their identification by infrared cameras. At the same time, the prosthetic hands achieve a more natural temperature, reducing the discomfort typically felt in direct contact with synthetic limbs. The aim of this study was to address the challenges faced by the users of prosthetic hands. The results from this study show a promising direction in humanoid robotics, fostering improved tactile interactions and redefining human–robot relationships. This innovative technique facilitates further advancements, blurring the lines between artificial aids and natural biological systems. Robotic faces and hands with human-like thermal infrared emission and physiological temperature are achieved by replicating the circulatory system’s inherent temperature regulation mechanism. The keystone of our development is an intricate system of fibers, reminiscent of blood vessels, embedded within the artificial skin. The fiber network enables controlled heat dissipation by regulating water circulation to mimic human thermal signatures.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-12"},"PeriodicalIF":8.6,"publicationDate":"2024-07-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00558-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141771071","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 : 2024-07-19DOI: 10.1038/s41427-024-00557-5
P. M. Hari Prasad, G. Malavika, Anuraj Pillai, Sachu Sadan, Zeena S. Pillai
Organic electrode materials (OEMs) possess low discharge potentials and charge‒discharge rates, making them suitable for use as affordable and eco-friendly rechargeable energy storage systems without needing metals such as lithium or sodium. OEMs can provide a sustainable energy economy by their development into stable and efficient next-generation high-power batteries. Despite the presence of several classes of OEMs, such as conducting polymers, 2D and 3D metal-organic frameworks, organolithium derivatives, 2D covalent organic frameworks, aromatic heterocyclic imides, and viologen derivatives, since their introduction in the 1960s, carbonyl-based molecules have maintained low discharge potentials and stable charging/discharging properties. Nevertheless, several redox-active organic molecules, including carbonyl derivatives, show poor electrochemical stability and ionic mobility in standard battery electrolytes, hampering their commercial use. Therefore, with the increased demand for renewable energy, the synthesis and testing of carbonyl-based OEMs continue to be performed in energy research. This review summarizes recent advances in developing carbonyl-based OEMs and their performance in rechargeable batteries. Organic electrode materials have gained considerable interest in the area of energy storage owing to their cost effectiveness, stability, tunable nature and high power. The use of natural ingredients, carbon-based materials and polymers for fabrication impart flexibility and light weight to the gadgets. Organic electrode materials present the potential for biodegradable energy storage solutions in batteries and supercapacitors, fostering innovation in sustainable technology.
{"title":"Emerging organic electrode materials for sustainable batteries","authors":"P. M. Hari Prasad, G. Malavika, Anuraj Pillai, Sachu Sadan, Zeena S. Pillai","doi":"10.1038/s41427-024-00557-5","DOIUrl":"10.1038/s41427-024-00557-5","url":null,"abstract":"Organic electrode materials (OEMs) possess low discharge potentials and charge‒discharge rates, making them suitable for use as affordable and eco-friendly rechargeable energy storage systems without needing metals such as lithium or sodium. OEMs can provide a sustainable energy economy by their development into stable and efficient next-generation high-power batteries. Despite the presence of several classes of OEMs, such as conducting polymers, 2D and 3D metal-organic frameworks, organolithium derivatives, 2D covalent organic frameworks, aromatic heterocyclic imides, and viologen derivatives, since their introduction in the 1960s, carbonyl-based molecules have maintained low discharge potentials and stable charging/discharging properties. Nevertheless, several redox-active organic molecules, including carbonyl derivatives, show poor electrochemical stability and ionic mobility in standard battery electrolytes, hampering their commercial use. Therefore, with the increased demand for renewable energy, the synthesis and testing of carbonyl-based OEMs continue to be performed in energy research. This review summarizes recent advances in developing carbonyl-based OEMs and their performance in rechargeable batteries. Organic electrode materials have gained considerable interest in the area of energy storage owing to their cost effectiveness, stability, tunable nature and high power. The use of natural ingredients, carbon-based materials and polymers for fabrication impart flexibility and light weight to the gadgets. Organic electrode materials present the potential for biodegradable energy storage solutions in batteries and supercapacitors, fostering innovation in sustainable technology.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-19"},"PeriodicalIF":8.6,"publicationDate":"2024-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00557-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141738511","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 : 2024-07-12DOI: 10.1038/s41427-024-00556-6
Jin Hong Kim, Seoung-Hun Kang, Duhee Yoon, Hakseong Kim, Jin-Soo Kim, Mohd Musaib Haidari, Dong Jin Jang, Jin-Yong Ko, Young-Woo Son, Bae Ho Park, Jin Sik Choi
Twisted bilayer graphene (tBLG) with small twist angles has attracted significant attention because of its unique electronic properties arising from the formation of a moiré superlattice. In this study, we systematically characterized the twist-angle-dependent electronic and transport properties of tBLG grown via chemical vapor deposition. This characterization included parameters such as the charge-neutral point voltage, carrier concentration, resistance, and mobility, covering a wide range of twist angles from 0° to 30°. We experimentally demonstrated that these parameters exhibited twist-angle-dependent moiré period trends, with high twist angles exceeding 9°, revealing more practically useful features, including improved mobilities compared to those of single-layer graphene. In addition, we demonstrated that the doping states and work functions were weakly dependent on the twist angles, as confirmed by additional first-principles calculations. This study provides valuable insights into the transport properties of tBLG and its potential for practical applications in the emerging field of twistronics. We systematically characterized the twist-angle-dependent electronic and transport properties of twisted bilayer graphene (tBLG) grown via chemical vapor deposition. Parameters such as charge-neutral point voltage, carrier concentration, resistance, and mobility were examined across a wide range of twist angles from 0° to 30°. Our experimental results demonstrated that these parameters exhibited twist-angle-dependent trends corresponding to the moiré period. Notably, high twist angles exceeding 9° displayed practically useful features, including improved mobilities compared to single-layer graphene. Additionally, we found that the doping states and work functions showed weak dependence on the twist angles, a finding corroborated by first-principles calculations.
{"title":"Twist angle-dependent transport properties of twisted bilayer graphene","authors":"Jin Hong Kim, Seoung-Hun Kang, Duhee Yoon, Hakseong Kim, Jin-Soo Kim, Mohd Musaib Haidari, Dong Jin Jang, Jin-Yong Ko, Young-Woo Son, Bae Ho Park, Jin Sik Choi","doi":"10.1038/s41427-024-00556-6","DOIUrl":"10.1038/s41427-024-00556-6","url":null,"abstract":"Twisted bilayer graphene (tBLG) with small twist angles has attracted significant attention because of its unique electronic properties arising from the formation of a moiré superlattice. In this study, we systematically characterized the twist-angle-dependent electronic and transport properties of tBLG grown via chemical vapor deposition. This characterization included parameters such as the charge-neutral point voltage, carrier concentration, resistance, and mobility, covering a wide range of twist angles from 0° to 30°. We experimentally demonstrated that these parameters exhibited twist-angle-dependent moiré period trends, with high twist angles exceeding 9°, revealing more practically useful features, including improved mobilities compared to those of single-layer graphene. In addition, we demonstrated that the doping states and work functions were weakly dependent on the twist angles, as confirmed by additional first-principles calculations. This study provides valuable insights into the transport properties of tBLG and its potential for practical applications in the emerging field of twistronics. We systematically characterized the twist-angle-dependent electronic and transport properties of twisted bilayer graphene (tBLG) grown via chemical vapor deposition. Parameters such as charge-neutral point voltage, carrier concentration, resistance, and mobility were examined across a wide range of twist angles from 0° to 30°. Our experimental results demonstrated that these parameters exhibited twist-angle-dependent trends corresponding to the moiré period. Notably, high twist angles exceeding 9° displayed practically useful features, including improved mobilities compared to single-layer graphene. Additionally, we found that the doping states and work functions showed weak dependence on the twist angles, a finding corroborated by first-principles calculations.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-9"},"PeriodicalIF":8.6,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00556-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141608630","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 : 2024-07-05DOI: 10.1038/s41427-024-00554-8
Lizhi Guan, Jingbo Fan, Zhi Kai Ng, Edwin Hang Tong Teo, Hortense Le Ferrand
Lightweight electronic packaging that provides mechanical protection, cooling ability, and customizable electromagnetic interference (EMI) shielding effectiveness (SE) is needed for next-generation electronics. Although electronic packaging solutions with excellent EMI SE exist, there is limited research on how hierarchical design can modulate the EMI SE of an electronic packaging material on demand. In this study, the deliberate precise micro/macrostructure design of graphite-based materials using magnetically assisted 3D printing allows tuning of the EMI SE in the X band (8–12 GHz), leading to a maximum total shielding performance of 90 dB. Aligning high-density graphite microplatelets during 3D printing also remarkably amplified the total SE by 200%. Subsequently, rationally designing the oriented microstructure within a geometrical shape increases the reflection and improves the EMI SE from 40 to 60 dB in a specific direction. Our proof-of-concept samples demonstrate the potential of precise micro/macrostructure design for customizing and enhancing electronic packaging’s EMI SE while achieving good heat dissipation and mechanical protection using a versatile 3D printing method. These advances pave the way for more reliable and safer electronic systems. Magnetically assisted 3D printing allows customizable electromagnetic interference (EMI) shielding effectiveness (SE). Aligning high-density graphite microplatelets during the 3D printing parallel or perpendicularly to incident waves leads to their tailored reflection and transmission. Designing the micro/macrostructure of materials allows customization and enhancement of electronic packaging’s EMI SE while achieving good heat dissipation and mechanical protection. These advances pave the way for more reliable and safer electronic systems.
下一代电子产品需要能提供机械保护、冷却能力和可定制电磁干扰（EMI）屏蔽效果（SE）的轻型电子封装。虽然目前已有具有出色电磁干扰屏蔽效果的电子封装解决方案，但有关分层设计如何按需调节电子封装材料的电磁干扰屏蔽效果的研究还很有限。在这项研究中，利用磁辅助三维打印技术对石墨基材料进行有意的精确微/宏观结构设计，可以调整 X 波段（8-12 GHz）的 EMI SE，使总屏蔽性能最大达到 90 dB。在三维打印过程中对齐高密度石墨微板还可将总屏蔽性能显著提高 200%。随后，在几何形状内合理设计定向微结构可增加反射，并将特定方向的 EMI SE 从 40 dB 提高到 60 dB。我们的概念验证样品证明了精确的微/宏观结构设计在定制和增强电子封装的 EMI SE 方面的潜力，同时利用多功能 3D 打印方法实现了良好的散热和机械保护。这些进步为更可靠、更安全的电子系统铺平了道路。
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Pub Date : 2024-06-28DOI: 10.1038/s41427-024-00552-w
Yen-Ting Chen, Zi-Xiang Wen, Chen-Fu Lin, Ming-Hsien Li, Peter Chen
Lead-free Cs3Bi2I9 single crystals have been demonstrated to be promising materials for direct X-ray detectors with remarkable performance. However, their application for 2D X-ray imaging is hindered by their time-consuming preparation and limited crystal size. In this paper, a thick Cs3Bi2I9 perovskite film fabricated via facile spray coating at a low processing temperature, which increases the area of the photoactive film, reduces the processing time, decreases the energy budget and the production cost, and enhances the production yield due to high material utilization, has great potential for commercial applications. Careful control of the processing temperature and intervals during spray coating results in a dense and thick perovskite film with well-stacked perovskite domains. The compact perovskite film enhances the charge transport capability of the Cs3Bi2I9 perovskite film and reduces the dark current density of the X-ray detector. The resultant X-ray detector, prepared through a two-step spray coating process, exhibited a sensitivity of 127.23 μC Gyair−1 cm−2 and a detection limit of 7.4 μGyair s−1. In addition, the device delivers long-term stability with a consistent photoresponse when exposed to consecutive X-ray pulse irradiation. A two-step spray coating process (first step: 20 cycles of spray coating at 110 °C with 40 s intervals; second step: 180 cycles of spray coating at 130 °C with 20 s intervals) was employed to a produce large-area, compact, and thick Cs3Bi2I9 perovskite film for the application of direct X-ray detectors. The fabricated device achieved a large active area of 150 mm2, a sensitivity of 127.23 μC Gyair−1 cm−2, a detection limit of 7.4 μGyairs−1, and durability after long-term X-ray pulse irradiation.
无铅 Cs3Bi2I9 单晶已被证明是性能卓越的直接 X 射线探测器的理想材料。然而，它们在二维 X 射线成像中的应用却因制备耗时和晶体尺寸有限而受到阻碍。本文在低加工温度下通过简便的喷涂方法制备了厚的 Cs3Bi2I9 包晶石薄膜，增加了光活性薄膜的面积，缩短了加工时间，降低了能源预算和生产成本，并因材料利用率高而提高了产量，具有巨大的商业应用潜力。在喷涂过程中，对加工温度和间隔时间的精心控制可获得致密厚实、包晶畴堆积良好的包晶薄膜。致密的包晶薄膜增强了 Cs3Bi2I9 包晶薄膜的电荷传输能力，降低了 X 射线探测器的暗电流密度。通过两步喷涂工艺制备的 X 射线探测器的灵敏度为 127.23 μC Gyair-1 cm-2，探测极限为 7.4 μGyair s-1。此外，该装置在连续接受 X 射线脉冲照射时具有长期稳定性和一致的光响应。
{"title":"Inorganic Cs3Bi2I9 lead-free halide perovskite film for large-area X-ray detector via low-cost ambient spray coating","authors":"Yen-Ting Chen, Zi-Xiang Wen, Chen-Fu Lin, Ming-Hsien Li, Peter Chen","doi":"10.1038/s41427-024-00552-w","DOIUrl":"10.1038/s41427-024-00552-w","url":null,"abstract":"Lead-free Cs3Bi2I9 single crystals have been demonstrated to be promising materials for direct X-ray detectors with remarkable performance. However, their application for 2D X-ray imaging is hindered by their time-consuming preparation and limited crystal size. In this paper, a thick Cs3Bi2I9 perovskite film fabricated via facile spray coating at a low processing temperature, which increases the area of the photoactive film, reduces the processing time, decreases the energy budget and the production cost, and enhances the production yield due to high material utilization, has great potential for commercial applications. Careful control of the processing temperature and intervals during spray coating results in a dense and thick perovskite film with well-stacked perovskite domains. The compact perovskite film enhances the charge transport capability of the Cs3Bi2I9 perovskite film and reduces the dark current density of the X-ray detector. The resultant X-ray detector, prepared through a two-step spray coating process, exhibited a sensitivity of 127.23 μC Gyair−1 cm−2 and a detection limit of 7.4 μGyair s−1. In addition, the device delivers long-term stability with a consistent photoresponse when exposed to consecutive X-ray pulse irradiation. A two-step spray coating process (first step: 20 cycles of spray coating at 110 °C with 40 s intervals; second step: 180 cycles of spray coating at 130 °C with 20 s intervals) was employed to a produce large-area, compact, and thick Cs3Bi2I9 perovskite film for the application of direct X-ray detectors. The fabricated device achieved a large active area of 150 mm2, a sensitivity of 127.23 μC Gyair−1 cm−2, a detection limit of 7.4 μGyairs−1, and durability after long-term X-ray pulse irradiation.","PeriodicalId":19382,"journal":{"name":"Npg Asia Materials","volume":"16 1","pages":"1-15"},"PeriodicalIF":8.6,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41427-024-00552-w.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141504451","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 : 2024-06-21DOI: 10.1038/s41427-024-00551-x
Hiroki Ago, Pablo Solís-Fernández
Research on two-dimensional (2D) materials has made tremendous progress reflecting their unique properties and promising applications. In this perspective, we review the novel concept of “2.5-dimensional (2.5D) materials”, which represent new opportunities to extend the field of materials science beyond 2D materials. This concept consists of controlling van der Waals interactions and using interlayer nanospaces to synthesize new materials and explore their intriguing properties. It also includes combination with other dimensional materials, the fabrication of three-dimensional (3D) architectures of 2D materials, and practical applications in our 3D everyday life. We discuss recent research based on this concept and provide future perspectives. Although atomically thin 2D materials have attracted great interest from their unique properties and promising applications, the integration of multiple 2D materials or their modifications are more exciting because they offer opportunities to explore new frontier of materials science. This perspective illustrates the new concept of “2.5-dimensional (2.5D) materials”, which symbolically represents the great potential offered by different routes to extend the realm of 2D materials. Some examples of 2.5D materials are reviewed, such as multicomponent heterostructures, intercalation, combination with other dimensional materials, functionalization, and application to 3D devices. In this perspective, we present the recent progress of this 2.5D materials research and future outlook.
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