Nature synthesis最新文献_第3页

Molecular sublimation enables 2D–3D transformation of orientational FAPbI3 perovskites 分子升华使定向FAPbI3钙钛矿实现2D-3D转化

Nature synthesis Pub Date : 2025-01-02 DOI: 10.1038/s44160-024-00696-1

Zihui Liang, Jinguo Cao, Zezhu Zhou, Lizhi Ren, Haodong Wu, Zhen Wang, Changhai Yi, Dong Yang, Kai Wang, Congcong Wu

{"title":"Molecular sublimation enables 2D–3D transformation of orientational FAPbI3 perovskites","authors":"Zihui Liang, Jinguo Cao, Zezhu Zhou, Lizhi Ren, Haodong Wu, Zhen Wang, Changhai Yi, Dong Yang, Kai Wang, Congcong Wu","doi":"10.1038/s44160-024-00696-1","DOIUrl":"10.1038/s44160-024-00696-1","url":null,"abstract":"The precise alignment and strategic positioning of crystal facets are essential for enhancing the stability and photovoltaic efficacy of perovskite materials. However, the synthesis of preferred facet orientations and the deconstruction of growth mechanisms are challenging due to randomized nucleation upon solvent removal and the consequent uncontrollable crystalline growth in traditional approaches. To mitigate solvent-induced disorder effects, here we introduce an approach involving a two-dimensional (2D) layered perovskite that initiates crystallographically controlled lattice growth upon molecular sublimation. This direct all-solid synthetic pathway is termed ‘2D-to-3D (α)’ and complements the traditional ‘δ-to-α’ phase transformation route. The growth of highly oriented α-formamidinium lead iodide (α-FAPbI3) perovskite films is facilitated, characterized by precise control over facet alignment and minimized lattice mismatch. A solar cell efficiency of 25.01% is achieved and the method offers advantages for the upscaling of perovskite solar cells to module-level manufacturing, demonstrating an efficiency of over 20% for an active area of 70 cm2. The synthesis of perovskite materials with preferred facet orientations is challenging due to randomized nucleation. Here a two-dimensional layered perovskite that initiates controlled lattice growth upon molecular sublimation is synthesized, enabling the formation of large-area films of α-FAPbI3 perovskite with long-range lattice order.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 3","pages":"347-358"},"PeriodicalIF":0.0,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143612624","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

Photocatalytic pathways for hydrochlorination 氢氯化反应的光催化途径

Nature synthesis Pub Date : 2025-01-02 DOI: 10.1038/s44160-024-00703-5

Francisco Juliá-Hernández

引用次数: 0

Ultrathin transition metal oxychalcogenide catalysts for oxygen evolution in acidic media 超薄过渡金属氧硫族化合物在酸性介质中的析氧催化剂

Nature synthesis Pub Date : 2025-01-02 DOI: 10.1038/s44160-024-00694-3

Wenshuo Xu, Yao Wu, Shibo Xi, Yan Wang, Ye Wang, Yuxuan Ke, Lingtong Ding, Xiao Wang, Jieun Yang, Wenjing Zhang, Kian Ping Loh, Feng Ding, Zheng Liu, Manish Chhowalla

{"title":"Ultrathin transition metal oxychalcogenide catalysts for oxygen evolution in acidic media","authors":"Wenshuo Xu, Yao Wu, Shibo Xi, Yan Wang, Ye Wang, Yuxuan Ke, Lingtong Ding, Xiao Wang, Jieun Yang, Wenjing Zhang, Kian Ping Loh, Feng Ding, Zheng Liu, Manish Chhowalla","doi":"10.1038/s44160-024-00694-3","DOIUrl":"10.1038/s44160-024-00694-3","url":null,"abstract":"Two-dimensional transition metal dichalcogenides (TMDs) exfoliated from bulk layered materials possess interesting properties. Most transition metal oxides are not layered and therefore cannot be exfoliated. Here we report the synthesis of a family of ultrathin materials—transition metal oxychalcogenides (TMOCs)—and demonstrate their unique properties. Two-dimensional TMOCs (MXxOy, M = group IV or V transition metal, X = chalcogen, O = oxygen; x, y = 0–2) from bulk transition metal dichalcogenides (MX2) have been fabricated using tetrabutylammonium intercalation. The stoichiometry of TMOCs can be adjusted, which enables control of their optical bandgaps and tunability of electrical conductivity by more than eight orders of magnitude. By tuning the chalcogen-to-oxygen ratio along with local atomic structure in TMOCs, it is possible to impart unexpected properties. For example, in contrast to conventional TMDs, the hybrid structure of TMOCs renders them surprisingly stable and electrochemically active in strong acids, allowing them to be used as proof-of-concept catalysts for the oxygen evolution reaction at pH ≈ 0. The HfS0.52O1.09 catalyst shows high mass activity (103,000 A g−1 at an overpotential of 0.5 V) and exhibits durability in proton exchange membrane water electrolysers. A family of two-dimensional transition metal oxychalcogenides is synthesized from bulk transition metal dichalcogenides by tetrabutylammonium intercalation. The stoichiometry and properties of the two-dimensional transition metal oxychalcogenides can be tuned, enabling high stability and catalytic activity for oxygen evolution in acid.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 3","pages":"327-335"},"PeriodicalIF":0.0,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s44160-024-00694-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143612680","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Anti-Markovnikov hydro- and deuterochlorination of unsaturated hydrocarbons using iron photocatalysis 铁光催化不饱和烃的反马尔可夫尼科夫氢化和去氯化反应

Nature synthesis Pub Date : 2025-01-02 DOI: 10.1038/s44160-024-00698-z

Kang-Jie Bian, David Nemoto Jr, Ying Chen, Yen-Chu Lu, Shih-Chieh Kao, Xiao-Wei Chen, Angel A. Martí, Julian G. West

{"title":"Anti-Markovnikov hydro- and deuterochlorination of unsaturated hydrocarbons using iron photocatalysis","authors":"Kang-Jie Bian, David Nemoto Jr, Ying Chen, Yen-Chu Lu, Shih-Chieh Kao, Xiao-Wei Chen, Angel A. Martí, Julian G. West","doi":"10.1038/s44160-024-00698-z","DOIUrl":"10.1038/s44160-024-00698-z","url":null,"abstract":"The hydrochlorination of unsaturated hydrocarbons is a fundamental reaction in organic synthesis. Traditional acid-mediated approaches proceed with Markovnikov selectivity, but direct access to anti-Markovnikov hydrochlorination products is still a longstanding pursuit. Previous methods are restricted by the need for multiple synthetic steps, stoichiometric chlorine and hydride sources and/or highly oxidative photocatalysis, resulting in limited scope and, in some cases, low regioselectivity. So, the development of redox-neutral hydrochlorination with high anti-Markovnikov regioselectivity compatible with both alkenes and alkynes remains important. Here we report a photocatalytic anti-Markovnikov hydro- and deuterochlorination of unsaturated hydrocarbons enabling access to diverse alkyl and alkenyl chlorides regio- and stereoselectively. Broad scope (125 examples), mild conditions and regio- and isotopo-divergent syntheses are demonstrated. Key to this method is the combination use of ligand-to-metal charge transfer photoreactivity of earth-abundant iron and hydrogen atom transfer reactivity of redox-active thiol. This cooperative system offers a powerful strategy for anti-Markovnikov hydrofunctionalization of unsaturated hydrocarbons. Methods for the anti-Markovnikov-selective hydrochlorination of unsaturated C–C bonds are limited by the need for stoichiometric reagents, highly oxidizing photocatalysts and multiple synthetic steps. Now the combination of ligand-to-metal charge transfer and hydrogen atom transfer reactivity enables the anti-Markovnikov-selective hydro- and deuterochlorination of unsaturated hydrocarbons using iron photocatalysis.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 3","pages":"314-326"},"PeriodicalIF":0.0,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143612648","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

Low-symmetry coordination cages enable recognition specificity and selective enrichment of higher fullerene isomers 低对称配位笼使识别特异性和选择性富集更高的富勒烯异构体

Nature synthesis Pub Date : 2025-01-02 DOI: 10.1038/s44160-024-00697-0

Xiao-Qing Guo, Pengwei Yu, Li-Peng Zhou, Shao-Jun Hu, Xiao-Fang Duan, Li-Xuan Cai, Lipiao Bao, Xing Lu, Qing-Fu Sun

{"title":"Low-symmetry coordination cages enable recognition specificity and selective enrichment of higher fullerene isomers","authors":"Xiao-Qing Guo, Pengwei Yu, Li-Peng Zhou, Shao-Jun Hu, Xiao-Fang Duan, Li-Xuan Cai, Lipiao Bao, Xing Lu, Qing-Fu Sun","doi":"10.1038/s44160-024-00697-0","DOIUrl":"10.1038/s44160-024-00697-0","url":null,"abstract":"The discovery of buckminsterfullerene (C60) marked a milestone in exploring three-dimensional carbon materials. However, with the exponential increase in the number of isomers for higher fullerenes, it has become challenging to realize the enrichment of the isomers by molecular recognition. Here we report two pseudo-cubic metal–organic cages, T and S4, with distinct cavity microenvironments, that showcase recognition specificity towards higher fullerene isomers. Compared with cage T, a symmetry shift from S4 to C2 emerges upon encapsulating an ellipsoidal D2-C76 guest, owing to the precise shape matching that curtails guest rotation. Furthermore, the low-symmetry cage S4 shows exceptional sensitivity in distinguishing between closely related isomers, such as a pair of C2v-symmetric C78 isomers, and shows promise for the selective enrichment of higher fullerenes. The approach of reducing symmetry positions metal–organic cages as promising candidates for encapsulating and identifying a broader spectrum of fullerene isomers, paralleling the specificity observed in biological systems. Symmetry reduction from T to S4 in coordination cages enables selective recognition of higher fullerene isomers, including D2-C76, C2v(2)-C78 and C2v(3)-C78, presenting a promising approach for fullerene identification and enrichment.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 3","pages":"359-369"},"PeriodicalIF":0.0,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143612671","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 high-entropy materials 作者更正：高熵材料的合成

Nature synthesis Pub Date : 2024-12-24 DOI: 10.1038/s44160-024-00725-z

Yifan Sun, Sheng Dai

引用次数: 0

Carbon quantum dots from supercritical fluid 超临界流体中的碳量子点

Nature synthesis Pub Date : 2024-12-06 DOI: 10.1038/s44160-024-00709-z

Peter W. Seavill

引用次数: 0

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