Nature MaterialsPub Date : 2023-11-06DOI: 10.1038/s41563-023-01700-3
Corey M. Efaw, Qisheng Wu, Ningshengjie Gao, Yugang Zhang, Haoyu Zhu, Kevin Gering, Michael F. Hurley, Hui Xiong, Enyuan Hu, Xia Cao, Wu Xu, Ji-Guang Zhang, Eric J. Dufek, Jie Xiao, Xiao-Qing Yang, Jun Liu, Yue Qi, Bin Li
{"title":"Localized high-concentration electrolytes get more localized through micelle-like structures","authors":"Corey M. Efaw, Qisheng Wu, Ningshengjie Gao, Yugang Zhang, Haoyu Zhu, Kevin Gering, Michael F. Hurley, Hui Xiong, Enyuan Hu, Xia Cao, Wu Xu, Ji-Guang Zhang, Eric J. Dufek, Jie Xiao, Xiao-Qing Yang, Jun Liu, Yue Qi, Bin Li","doi":"10.1038/s41563-023-01700-3","DOIUrl":"10.1038/s41563-023-01700-3","url":null,"abstract":"Liquid electrolytes in batteries are typically treated as macroscopically homogeneous ionic transport media despite having a complex chemical composition and atomistic solvation structures, leaving a knowledge gap of the microstructural characteristics. Here, we reveal a unique micelle-like structure in a localized high-concentration electrolyte, in which the solvent acts as a surfactant between an insoluble salt in a diluent. The miscibility of the solvent with the diluent and simultaneous solubility of the salt results in a micelle-like structure with a smeared interface and an increased salt concentration at the centre of the salt–solvent clusters that extends the salt solubility. These intermingling miscibility effects have temperature dependencies, wherein a typical localized high-concentration electrolyte peaks in localized cluster salt concentration near room temperature and is used to form a stable solid–electrolyte interphase on a Li metal anode. These findings serve as a guide to predicting a stable ternary phase diagram and connecting the electrolyte microstructure with electrolyte formulation and formation protocols of solid–electrolyte interphases for enhanced battery cyclability. Liquid electrolytes in batteries are considered to be macroscopically homogeneous ionic transport media despite having a complex chemical composition and atomistic solvation structures. A micelle-like structure in a localized high-concentration electrolyte for which the solvent acts as a surfactant is reported.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"22 12","pages":"1531-1539"},"PeriodicalIF":41.2,"publicationDate":"2023-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71483992","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nature MaterialsPub Date : 2023-11-02DOI: 10.1038/s41563-023-01706-x
Wenjie Zhou, Yein Lim, Haixin Lin, Sangmin Lee, Yuanwei Li, Ziyin Huang, Jingshan S. Du, Byeongdu Lee, Shunzhi Wang, Ana Sánchez-Iglesias, Marek Grzelczak, Luis M. Liz-Marzán, Sharon C. Glotzer, Chad A. Mirkin
{"title":"Colloidal quasicrystals engineered with DNA","authors":"Wenjie Zhou, Yein Lim, Haixin Lin, Sangmin Lee, Yuanwei Li, Ziyin Huang, Jingshan S. Du, Byeongdu Lee, Shunzhi Wang, Ana Sánchez-Iglesias, Marek Grzelczak, Luis M. Liz-Marzán, Sharon C. Glotzer, Chad A. Mirkin","doi":"10.1038/s41563-023-01706-x","DOIUrl":"10.1038/s41563-023-01706-x","url":null,"abstract":"In principle, designing and synthesizing almost any class of colloidal crystal is possible. Nonetheless, the deliberate and rational formation of colloidal quasicrystals has been difficult to achieve. Here we describe the assembly of colloidal quasicrystals by exploiting the geometry of nanoscale decahedra and the programmable bonding characteristics of DNA immobilized on their facets. This process is enthalpy-driven, works over a range of particle sizes and DNA lengths, and is made possible by the energetic preference of the system to maximize DNA duplex formation and favour facet alignment, generating local five- and six-coordinated motifs. This class of axial structures is defined by a square–triangle tiling with rhombus defects and successive on-average quasiperiodic layers exhibiting stacking disorder which provides the entropy necessary for thermodynamic stability. Taken together, these results establish an engineering milestone in the deliberate design of programmable matter. The rational design and assembly of colloidal quasicrystals is achieved by exploring the hybridization of nanoscale decahedra nanoparticles functionalized with DNA linkers.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"23 3","pages":"424-428"},"PeriodicalIF":41.2,"publicationDate":"2023-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71425261","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Compact angle-resolved metasurface spectrometer","authors":"Guiyi Cai, Yanhao Li, Yao Zhang, Xiong Jiang, Yimu Chen, Geyang Qu, Xudong Zhang, Shumin Xiao, Jiecai Han, Shaohua Yu, Yuri Kivshar, Qinghai Song","doi":"10.1038/s41563-023-01710-1","DOIUrl":"10.1038/s41563-023-01710-1","url":null,"abstract":"Light scattered or radiated from a material carries valuable information on the said material. Such information can be uncovered by measuring the light field at different angles and frequencies. However, this technique typically requires a large optical apparatus, hampering the widespread use of angle-resolved spectroscopy beyond the lab. Here we demonstrate compact angle-resolved spectral imaging by combining a tunable metasurface-based spectrometer array and a metalens. With this approach, even with a miniaturized spectrometer footprint of only 4 × 4 μm2, we demonstrate a wavelength accuracy of 0.17 nm, spectral resolution of 0.4 nm and a linear dynamic range of 149 dB. Moreover, our spectrometer has a detection limit of 1.2 fJ, and can be patterned to an array for spectral imaging. Placing such a spectrometer array directly at the back focal plane of a metalens, we achieve an angular resolution of 4.88 × 10−3 rad. Our angle-resolved spectrometers empowered by metalenses can be employed towards enhancing advanced optical imaging and spectral analysis applications. Employing a miniaturized spectrometer that combines a metasurface-based spectrometer array and a metalens, angle-resolved spectral imaging is achieved with a wavelength accuracy of 0.17 nm, spectral resolution of 0.40 nm and angular resolution of 4.88 × 10−3 rad for a spectrometer with a 4 × 4 μm2 footprint.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"23 1","pages":"71-78"},"PeriodicalIF":41.2,"publicationDate":"2023-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71425262","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nature MaterialsPub Date : 2023-11-02DOI: 10.1038/s41563-023-01707-w
Junseok Moon, Wiktor Beker, Marta Siek, Jiheon Kim, Hyeon Seok Lee, Taeghwan Hyeon, Bartosz A. Grzybowski
{"title":"Active learning guides discovery of a champion four-metal perovskite oxide for oxygen evolution electrocatalysis","authors":"Junseok Moon, Wiktor Beker, Marta Siek, Jiheon Kim, Hyeon Seok Lee, Taeghwan Hyeon, Bartosz A. Grzybowski","doi":"10.1038/s41563-023-01707-w","DOIUrl":"10.1038/s41563-023-01707-w","url":null,"abstract":"Multi-metal oxides in general and perovskite oxides in particular have attracted considerable attention as oxygen evolution electrocatalysts. Although numerous theoretical studies have been undertaken, the most promising perovskite-based catalysts continue to emerge from human-driven experimental campaigns rather than data-driven machine learning protocols, which are often limited by the scarcity of experimental data on which to train the models. This work promises to break this impasse by demonstrating that active learning on even small datasets—but supplemented by informative structural-characterization data and coupled with closed-loop experimentation—can yield materials of outstanding performance. The model we develop not only reproduces several non-obvious and actively studied experimental trends but also identifies a composition of a perovskite oxide electrocatalyst exhibiting an intrinsic overpotential at 10 mA cm–2oxide of 391 mV, which is among the lowest known of four-metal perovskite oxides. Multi-metal and perovskite oxides are attractive as oxygen evolution electrocatalysts, and thus far the most promising candidates have emerged from experimental methodologies. Active-learning models supplemented by structural-characterization data and closed-loop experimentation can now identify a perovskite oxide with outstanding performance.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"23 1","pages":"108-115"},"PeriodicalIF":41.2,"publicationDate":"2023-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71425185","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nature MaterialsPub Date : 2023-10-31DOI: 10.1038/s41563-023-01731-w
{"title":"Electronics can be more sustainable","authors":"","doi":"10.1038/s41563-023-01731-w","DOIUrl":"10.1038/s41563-023-01731-w","url":null,"abstract":"Integrated design assisted by materials and technology innovations can help a transition from traditional to sustainable electronics.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"22 11","pages":"1273-1273"},"PeriodicalIF":41.2,"publicationDate":"2023-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41563-023-01731-w.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71417642","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Percolation-induced gel–gel phase separation in a dilute polymer network","authors":"Shohei Ishikawa, Yasuhide Iwanaga, Takashi Uneyama, Xiang Li, Hironori Hojo, Ikuo Fujinaga, Takuya Katashima, Taku Saito, Yasushi Okada, Ung-il Chung, Naoyuki Sakumichi, Takamasa Sakai","doi":"10.1038/s41563-023-01712-z","DOIUrl":"10.1038/s41563-023-01712-z","url":null,"abstract":"Cosmic large-scale structures, animal flocks and living tissues can be considered non-equilibrium organized systems created by dissipative processes. Replicating such properties in artificial systems is still difficult. Herein we report a dissipative network formation process in a dilute polymer–water mixture that leads to percolation-induced gel–gel phase separation. The dilute system, which forms a monophase structure at the percolation threshold, spontaneously separates into two co-continuous gel phases with a submillimetre scale (a dilute-percolated gel) during the deswelling process after the completion of the gelation reaction. The dilute-percolated gel, which contains 99% water, exhibits unexpected hydrophobicity and induces the development of adipose-like tissues in subcutaneous tissues. These findings support the development of dissipative structures with advanced functionalities for distinct applications, ranging from physical chemistry to tissue engineering. A dilute water–polymer mixture exhibits a percolation-induced gel–gel phase separation, resulting in a two gel co-continuous substrate, which is used for adipose tissue development.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"22 12","pages":"1564-1570"},"PeriodicalIF":41.2,"publicationDate":"2023-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71413184","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nature MaterialsPub Date : 2023-10-30DOI: 10.1038/s41563-023-01705-y
Jian Xu, Hao Chen, Luke Grater, Cheng Liu, Yi Yang, Sam Teale, Aidan Maxwell, Suhas Mahesh, Haoyue Wan, Yuxin Chang, Bin Chen, Benjamin Rehl, So Min Park, Mercouri G. Kanatzidis, Edward H. Sargent
{"title":"Anion optimization for bifunctional surface passivation in perovskite solar cells","authors":"Jian Xu, Hao Chen, Luke Grater, Cheng Liu, Yi Yang, Sam Teale, Aidan Maxwell, Suhas Mahesh, Haoyue Wan, Yuxin Chang, Bin Chen, Benjamin Rehl, So Min Park, Mercouri G. Kanatzidis, Edward H. Sargent","doi":"10.1038/s41563-023-01705-y","DOIUrl":"10.1038/s41563-023-01705-y","url":null,"abstract":"Pseudo-halide (PH) anion engineering has emerged as a surface passivation strategy of interest for perovskite-based optoelectronics; but until now, PH anions have led to insufficient defect passivation and thus to undesired deep impurity states. The size of the chemical space of PH anions (>106 molecules) has so far limited attempts to explore the full family of candidate molecules. We created a machine learning workflow to speed up the discovery process using full-density functional theory calculations for training the model. The physics-informed machine learning model allowed us to pinpoint promising molecules with a head group that prevents lattice distortion and anti-site defect formation, and a tail group optimized for strong attachment to the surface. We identified 15 potential bifunctional PH anions with the ability to passivate both donors and acceptors, and through experimentation, discovered that sodium thioglycolate was the most effective passivant. This strategy resulted in a power-conversion efficiency of 24.56% with a high open-circuit voltage of 1.19 volts (24.04% National Renewable Energy Lab-certified quasi-steady-state) in inverted perovskite solar cells. Encapsulated devices maintained 96% of their initial power-conversion energy during 900 hours of one-sun operation at the maximum power point. Pseudo-halide anion engineering is an effective surface passivation strategy for perovskite-based optoelectronics but the large chemical space of molecules limits its potential. Here, the authors create a machine learning workflow to find optimized pseudo-halide anions, which are verified in devices with improved performances.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"22 12","pages":"1507-1514"},"PeriodicalIF":41.2,"publicationDate":"2023-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"71413183","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nature MaterialsPub Date : 2023-10-27DOI: 10.1038/s41563-023-01675-1
Zhigang Shuai
{"title":"Faster holes by delocalization","authors":"Zhigang Shuai","doi":"10.1038/s41563-023-01675-1","DOIUrl":"10.1038/s41563-023-01675-1","url":null,"abstract":"Terahertz photoconductivity measurements coupled with theoretical modelling reveals that thermal transient excitations to more delocalized states enhances hole mobility in organic molecular semiconductors.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"22 11","pages":"1277-1278"},"PeriodicalIF":41.2,"publicationDate":"2023-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"61564244","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nature MaterialsPub Date : 2023-10-27DOI: 10.1038/s41563-023-01701-2
Meghan J. O’Melia, Susan N. Thomas
{"title":"Lymphatics drain nanoparticles from tumours","authors":"Meghan J. O’Melia, Susan N. Thomas","doi":"10.1038/s41563-023-01701-2","DOIUrl":"10.1038/s41563-023-01701-2","url":null,"abstract":"Lymphatic vessels within and near to tumours facilitate nanoparticle transport out of tumours, with ramifications in the design and implementation of next-generation clinical cancer nanomedicines.","PeriodicalId":19058,"journal":{"name":"Nature Materials","volume":"22 11","pages":"1287-1288"},"PeriodicalIF":41.2,"publicationDate":"2023-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"61564245","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}