Nature synthesis最新文献_第4页

Programmable phase switching and exfoliation 可编程相位开关和去角质

Nature synthesis Pub Date : 2024-12-05 DOI: 10.1038/s44160-024-00702-6

Qingdong Ou, Qiaoliang Bao

引用次数: 0

Synthesis of isolated Ru–O3 sites on hexagonal close-packed intermetallic penta-metallene for hydrogen oxidation electrocatalysis 六方密排五金属间烯上钌- o3分离位点的合成及其氢氧化电催化作用

Nature synthesis Pub Date : 2024-12-03 DOI: 10.1038/s44160-024-00685-4

Fangxu Lin, Heng Luo, Lu Li, Fan Lv, Yanyan Chen, Qinghua Zhang, Xiaocang Han, Dawei Wang, Menggang Li, Yan Luo, Kai Wang, Lin Gu, Qian Wang, Xiaoxu Zhao, Mingchuan Luo, Shaojun Guo

{"title":"Synthesis of isolated Ru–O3 sites on hexagonal close-packed intermetallic penta-metallene for hydrogen oxidation electrocatalysis","authors":"Fangxu Lin, Heng Luo, Lu Li, Fan Lv, Yanyan Chen, Qinghua Zhang, Xiaocang Han, Dawei Wang, Menggang Li, Yan Luo, Kai Wang, Lin Gu, Qian Wang, Xiaoxu Zhao, Mingchuan Luo, Shaojun Guo","doi":"10.1038/s44160-024-00685-4","DOIUrl":"10.1038/s44160-024-00685-4","url":null,"abstract":"Atomically thin two-dimensional alloys are interesting for electrocatalysis but suffer from poor functional robustness and wide active-site heterogeneity. Here the synthesis of an unconventional hexagonal close-packed-phase intermetallic Pd-based multi-metallene, on which isolated Ru–O3 atomic sites are homogeneously dispersed, overcomes these obstacles. This structure exhibits excellent hydrogen oxidation reaction (HOR) activity, durability and anti-CO poisoning performance. The mass activity and exchange current density reach 11.5 mA μg−1 and 1.0 mA cm−2, respectively, showing some of the fastest reaction kinetics reported for Pd-based HOR catalysts. In situ Raman spectroscopy and theoretical investigations confirm that the intensified ligand effect derived from orderly atomic arrangement tends to strengthen the adsorption of hydroxyl and water, while the homogeneous Ru–O3 sites contribute to weakened binding of HOR-involved intermediates (*H, *OH and *H2O), leading to a favourable reaction pathway. This work demonstrates the importance of high-valence Ru and surface O species in enhancing the synergetic process and water reorganization. Atomically thin alloys are promising electrocatalysts but suffer from poor homogeneity. Here a multi-element metallene system is synthesized using an auto-catalytic method. The hexagonal close-packed intermetallic structure and isolated surface Ru–O3 sites provide optimal adsorption of intermediates, contributing to high hydrogen oxidation activity and stability.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 3","pages":"399-409"},"PeriodicalIF":0.0,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143612663","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Synthesis of high-entropy materials 高熵材料的合成

Nature synthesis Pub Date : 2024-12-03 DOI: 10.1038/s44160-024-00690-7

Yifan Sun, Sheng Dai

{"title":"Synthesis of high-entropy materials","authors":"Yifan Sun, Sheng Dai","doi":"10.1038/s44160-024-00690-7","DOIUrl":"10.1038/s44160-024-00690-7","url":null,"abstract":"High-entropy materials (HEMs) exhibit compelling behaviours that are distinct from those in conventional solid solutions. Such disordered multicomponent systems bring unprecedented compositional and structural complexities that hinder a thorough understanding of entropy stabilization and its impact on phase selection and property optimization. The controlled fabrication of HEMs, ideally reaching the same level of detail as traditional alloy design, is desirable. The past decade has witnessed the development of advanced synthesis methodologies and techniques to introduce various degrees of control to this class of inherently disordered materials. Here we discuss the emerging rationales for synthesizing bulk and nanostructured HEMs with tunable microstructures, extended compositions and tailored atomic configurations. Case studies of formation pathways and stabilization mechanisms of different types of HEM reveal insightful synthesis guidelines. This progress enables predictable and rational manipulation of atomic order in the chemically disordered lattice, laying the foundations for exceptional functionalities. The emergence of high-entropy materials affords opportunities to harmonize precision and disorder for materials design. This Review highlights the synthesis principles and strategies towards controllable and predictive fabrication of high-entropy materials with complex chemical compositions, engineered microstructures and tailored atomic configurations.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 12","pages":"1457-1470"},"PeriodicalIF":0.0,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798592","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Electrochemical fragmentation for alkene difunctionalization 烯烃双官能化的电化学破碎

Nature synthesis Pub Date : 2024-11-27 DOI: 10.1038/s44160-024-00701-7

Thomas West

引用次数: 0

Electronic structure modulation of black phosphorus 黑磷的电子结构调制

Nature synthesis Pub Date : 2024-11-27 DOI: 10.1038/s44160-024-00708-0

Alexandra R. Groves

引用次数: 0

Atomic-level Cu active sites enable energy-efficient CO2 electroreduction to multicarbon products in strong acid 原子水平的Cu活性位点使高能效的CO2电还原到强酸中的多碳产品

Nature synthesis Pub Date : 2024-11-26 DOI: 10.1038/s44160-024-00689-0

Lizhou Fan, Feng Li, Tianqi Liu, Jianan Erick Huang, Rui Kai Miao, Yu Yan, Shihui Feng, Cheuk-Wai Tai, Sung-Fu Hung, Hsin-Jung Tsai, Meng-Cheng Chen, Yang Bai, Dongha Kim, Sungjin Park, Panos Papangelakis, Chengqian Wu, Ali Shayesteh Zeraati, Roham Dorakhan, Licheng Sun, David Sinton, Edward Sargent

{"title":"Atomic-level Cu active sites enable energy-efficient CO2 electroreduction to multicarbon products in strong acid","authors":"Lizhou Fan, Feng Li, Tianqi Liu, Jianan Erick Huang, Rui Kai Miao, Yu Yan, Shihui Feng, Cheuk-Wai Tai, Sung-Fu Hung, Hsin-Jung Tsai, Meng-Cheng Chen, Yang Bai, Dongha Kim, Sungjin Park, Panos Papangelakis, Chengqian Wu, Ali Shayesteh Zeraati, Roham Dorakhan, Licheng Sun, David Sinton, Edward Sargent","doi":"10.1038/s44160-024-00689-0","DOIUrl":"10.1038/s44160-024-00689-0","url":null,"abstract":"Electrochemical CO2 reduction provides a promising strategy to synthesize C2+ compounds with reduced carbon intensity; however, high overall energy consumption restricts practical implementation. Using acidic media enables high CO2 utilization and low liquid product crossover, but to date has suffered low C2+ product selectivity. Here we hypothesize that adjacent pairs of atomic-copper active sites may favour C–C coupling, thus facilitating C2+ product formation. We construct tandem electrocatalysts with two distinct classes of active sites, the first for CO2 to CO, and the second, a dual-atomic-site catalyst, for CO to C2+. This leads to an ethanol Faradaic efficiency of 46% and a C2+ product Faradaic efficiency of 91% at 150 mA cm−2 in an acidic CO2 reduction reaction. We document a CO2 single-pass utilization of 78% and an energy efficiency of 30% towards C2+ products; an ethanol crossover rate of 5%; and an ethanol product concentration of 4.5%, resulting in an exceptionally low projected energy cost of 249 GJ t−1 for the electrosynthesis of ethanol via the CO2 reduction reaction. Tandem electrocatalysts are developed for acidic CO2 electroreduction. The catalyst contains planar-copper for CO2 reduction to CO, and a dual-copper-active-site layer for CO reduction to C2+ products. An ethanol Faradaic efficiency of 46% and a C2+ Faradaic efficiency of 91% are achieved in acidic electrolyte at 150 mA cm−2.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 2","pages":"262-270"},"PeriodicalIF":0.0,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143397437","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Author Correction: Synthesis of goldene comprising single-atom layer gold 作者更正：含单原子层金的金的合成

Nature synthesis Pub Date : 2024-11-25 DOI: 10.1038/s44160-024-00700-8

Shun Kashiwaya, Yuchen Shi, Jun Lu, Davide G. Sangiovanni, Grzegorz Greczynski, Martin Magnuson, Mike Andersson, Johanna Rosen, Lars Hultman

引用次数: 0

Simultaneous mechanical and chemical synthesis of long-range-ordered perovskites 长程有序钙钛矿的同时机械和化学合成

Nature synthesis Pub Date : 2024-11-22 DOI: 10.1038/s44160-024-00687-2

Hong Liu, Haodong Wu, Zezhu Zhou, Lizhi Ren, Yi Yang, Aiping Zhang, Jin Qian, Shashank Priya, Bed Poudel, Chang Liu, Dong Yang, Kai Wang, Congcong Wu

{"title":"Simultaneous mechanical and chemical synthesis of long-range-ordered perovskites","authors":"Hong Liu, Haodong Wu, Zezhu Zhou, Lizhi Ren, Yi Yang, Aiping Zhang, Jin Qian, Shashank Priya, Bed Poudel, Chang Liu, Dong Yang, Kai Wang, Congcong Wu","doi":"10.1038/s44160-024-00687-2","DOIUrl":"10.1038/s44160-024-00687-2","url":null,"abstract":"Combining mechanical and chemical effects during the synthesis of crystals can lead to unexpected material attributes. The role of mechanical effects during the wet chemical synthesis of halide perovskite remains insufficiently explored, mainly due to its temporal asynchronization with the typical slower solvent evaporation-motivated chemical changes. Here we introduce stress from mechanical shearing into a short temporal window of crystal synthesis by using a fast-crystallizing precursor ink, which causes mechanical shearing effects to occur simultaneously with the atomic assembly of perovskite. This protocol allows macroscopic dynamic shearing to impact the atomic lattice rearrangement, growth and facet orientation. Such an effect is consistently observed across atomic to centimetre scales, culminating in films with long-range uniformity. These perovskite films exhibit exceptional crystalline orientation and structural uniformity, demonstrating a Herman’s orientation factor of −0.3135 and leading to a remarkable power conversion efficiency of 25.90% on small-area cells and exceeding 21% in a 70 cm2 solar module. This synthetic approach exemplifies the use of mechanical shearing to foster the assembly of long-range-ordered crystallographic lattices, thereby providing a scalable synthesis for high-quality perovskite films. Controlling crystal growth in perovskite syntheses that rely solely on chemical processes is challenging. Now, a synthesis protocol that integrates mechanical and chemical effects achieves enhanced crystalline orientation and uniformity.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 2","pages":"196-208"},"PeriodicalIF":0.0,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143397395","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Coupling of mechanical and chemical effects to synthesize highly oriented perovskite films 机械与化学耦合作用合成高取向钙钛矿薄膜

Nature synthesis Pub Date : 2024-11-22 DOI: 10.1038/s44160-024-00688-1

引用次数: 0

A burst of light for mechanochemistry 机械化学的一束光

Nature synthesis Pub Date : 2024-11-22 DOI: 10.1038/s44160-024-00693-4

Roman Boulatov

引用次数: 0