Nature synthesis最新文献_第10页

Ligand-induced self-assembly of twisted two-dimensional halide perovskites 扭曲二维卤化物钙钛矿的配体诱导自组装

IF 2

Nature synthesis Pub Date : 2025-03-28 DOI: 10.1038/s44160-025-00780-0

Jonghee Yang, Addis S. Fuhr, Subeom Shin, Kevin M. Roccapriore, Bogdan Dryzhakov, Bin Hu, Byeongjoo Kang, Hyungju Ahn, Woojae Kim, Bobby G. Sumpter, Sergei V. Kalinin, Mahshid Ahmadi

{"title":"Ligand-induced self-assembly of twisted two-dimensional halide perovskites","authors":"Jonghee Yang, Addis S. Fuhr, Subeom Shin, Kevin M. Roccapriore, Bogdan Dryzhakov, Bin Hu, Byeongjoo Kang, Hyungju Ahn, Woojae Kim, Bobby G. Sumpter, Sergei V. Kalinin, Mahshid Ahmadi","doi":"10.1038/s44160-025-00780-0","DOIUrl":"10.1038/s44160-025-00780-0","url":null,"abstract":"Two-dimensional (2D) halide perovskites (HPs) exhibit intriguing optoelectronic functionalities. Conventionally, 2D HPs have been synthesized with linear and planar molecular spacers, resulting in nominal modifications of their optoelectronic properties. In contrast, lower-dimensional HPs (0D and 1D) have proved accommodating to the incorporation of bulky molecular spacers. Fundamental insights into the incorporation of bulky molecular spacers in 2D HP structures remains elusive. Here, by implementing a high-throughput autonomous exploration workflow, the crystallization behaviours of 2D HPs based on a bulky 3,3-diphenylpropylammonium (DPA) spacer are comprehensively explored. Counterintuitive to conventional HP chemistry, synthesis of 2D DPA2PbI4 HPs is indeed feasible when the steric hindrance is mediated by minute incorporation of 3D HP precursors. Furthermore, a moiré superlattice is observed from the DPA2PbI4 flakes, indicating the spontaneous formation of twisted stacks of 2D HPs. We hypothesize that the unconventional van der Waals surface of DPA2PbI4 facilitates the self-assembly of the twisted stacks of 2D HPs. This work exemplifies how high-throughput experimentation can discover unconventional material systems in which the synthetic principle lies beyond conventional chemical intuition. Furthermore, these findings provide hints for how to chemically manipulate the twist stacking in 2D HPs, thus rendering a straightforward way for bespoke realization of functionalities in exotic materials systems via a bottom-up approach. High-throughput automated synthesis is used to investigate the crystallization behaviour of two-dimensional (2D) halide perovskites (HPs) based on a bulky ligand cation, 3,3-diphenylpropylammonium. The solution-processed 2D HP flakes realize a moiré superlattice, indicating the formation of a twisted 2D stack via self-assembly action.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 9","pages":"1068-1077"},"PeriodicalIF":20.0,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145123701","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 reactions using iron–sodium pairs 铁钠对偶联反应

IF 2

Nature synthesis Pub Date : 2025-03-26 DOI: 10.1038/s44160-025-00779-7

Jos Briggs-Pritchard, Michael L. Neidig

引用次数: 0

Water-stable nanocrystals in a single step 单步制备水稳定纳米晶体

IF 2

Nature synthesis Pub Date : 2025-03-26 DOI: 10.1038/s44160-025-00768-w

引用次数: 0

Iron-catalysed direct coupling of organosodium compounds 铁催化有机钠化合物的直接偶联。

IF 2

Nature synthesis Pub Date : 2025-03-25 DOI: 10.1038/s44160-025-00771-1

Ikko Takahashi, Andreu Tortajada, David E. Anderson, Laurean Ilies, Eva Hevia, Sobi Asako

{"title":"Iron-catalysed direct coupling of organosodium compounds","authors":"Ikko Takahashi, Andreu Tortajada, David E. Anderson, Laurean Ilies, Eva Hevia, Sobi Asako","doi":"10.1038/s44160-025-00771-1","DOIUrl":"10.1038/s44160-025-00771-1","url":null,"abstract":"Sodium is one of the most abundant elements on Earth and a sustainable alternative to less sustainable metals such as lithium, which is becoming increasingly depleted and expensive. Traditionally, however, organosodium reagents have been considered highly reactive, engaging in uncontrollable reactions, and as a result, they have been scarcely used in organic synthesis, especially in combination with transition-metal catalysis. Here we report the use of organosodium compounds as C(sp2)–Na nucleophilic partners in iron-catalysed oxidative homocoupling and cross-coupling with alkyl halides. Mechanistic investigations based on the preparation and characterization of putative organoiron intermediates reveal that a bidentate additive coordinates both sodium and the iron centre, exerting control over the catalytic reactivity. This combination of two abundant and non-toxic metals, powered by molecular-level mechanistic understanding, is expected to open new avenues for the use of sustainable organometallic reagents in organic synthesis. Despite the abundance and non-toxic nature of sodium, organosodium reagents have rarely been used in organic synthesis. Now iron-catalysed homocoupling and C(sp2)–C(sp3) cross-coupling reactions of arylsodium compounds are reported. The observed C(sp2)–C(sp3) cross-coupling reactivity of arylsodium reagents is enabled by Lewis donor additive N,N,N′,N′-tetramethylethylenediamine.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 7","pages":"816-825"},"PeriodicalIF":20.0,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12254037/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144627972","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

Scalable and precise synthesis of polymer nanoparticles 可扩展和精确合成聚合物纳米颗粒

IF 2

Nature synthesis Pub Date : 2025-03-24 DOI: 10.1038/s44160-025-00778-8

Chun Feng

引用次数: 0

Industrial-level CO2 to formate conversion on Turing-structured electrocatalysts 工业水平的二氧化碳在图灵结构的电催化剂上形成转化

IF 2

Nature synthesis Pub Date : 2025-03-20 DOI: 10.1038/s44160-025-00769-9

Na Ye, Kai Wang, Yingjun Tan, Zhengyi Qian, Hongyu Guo, Changshuai Shang, Zheng Lin, Qizheng Huang, Youxing Liu, Lu Li, Yu Gu, Ying Han, Chenhui Zhou, Mingchuan Luo, Shaojun Guo

{"title":"Industrial-level CO2 to formate conversion on Turing-structured electrocatalysts","authors":"Na Ye, Kai Wang, Yingjun Tan, Zhengyi Qian, Hongyu Guo, Changshuai Shang, Zheng Lin, Qizheng Huang, Youxing Liu, Lu Li, Yu Gu, Ying Han, Chenhui Zhou, Mingchuan Luo, Shaojun Guo","doi":"10.1038/s44160-025-00769-9","DOIUrl":"10.1038/s44160-025-00769-9","url":null,"abstract":"Industrializing the electrosynthesis of formate from CO2 reduction in membrane electrode assembly (MEA) electrolysers necessitates tuning both electrocatalysts and the interfacial water microenvironment. Here we cast a series of Turing-structured topology electrocatalysts, which can control the reorientation of interfacial water through the tuning of surface oxophilicity, for industrial-level conversion of CO2 to formate. Experimental and theoretical results verify the precisely modulated reorientation of interfacial water, with the ratios of four-coordinated to two-coordinated hydrogen-bonded interfacial water ranging from 0.26 to 3.10 over Turing-structured topology catalysts. We further demonstrate the efficiency of these strategies in sustaining high-rate formate electrosynthesis across a wide range of industrial-level current densities (300–1,000 mA cm−2) and formulate a volcano relationship to describe the relation. The optimal Turing Sb0.1Sn0.9O2 catalyst achieves a formate Faradaic efficiency of 92.0% at 1,000 mA cm-2 and exhibits a stability of 200 h at 500 mA cm-2 in a membrane electrode assembly electrolyser. Our findings highlight the prospect of topology-mediated tunings of the interfacial water microenvironment for electrifying the conversion of CO2 to formate, with promising implications for the electrosynthesis of other valuable chemicals. Turing-structured topology electrocatalysts are reported to control the reorientation of interfacial water through the tuning of surface oxophilicity. The optimal Turing catalyst achieves a formate Faradaic efficiency of 92.0% at 1,000 mA cm−2.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 7","pages":"799-807"},"PeriodicalIF":20.0,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145123091","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

Unassisted electrochemical H2O2 production coupled to glycerol oxidation 与甘油氧化耦合的无辅助电化学H2O2生产

IF 2

Nature synthesis Pub Date : 2025-03-20 DOI: 10.1038/s44160-025-00774-y

Dongrak Oh, Seon Woo Hwang, Dong Yeon Kim, Jesse E. Matthews, Jinyoung Lee, Jaime E. Avilés Acosta, Sang-Won Lee, Yi Xu, Ara Cho, Dong Un Lee, Thomas F. Jaramillo, Dong-Hwa Seo, Ji-Wook Jang

{"title":"Unassisted electrochemical H2O2 production coupled to glycerol oxidation","authors":"Dongrak Oh, Seon Woo Hwang, Dong Yeon Kim, Jesse E. Matthews, Jinyoung Lee, Jaime E. Avilés Acosta, Sang-Won Lee, Yi Xu, Ara Cho, Dong Un Lee, Thomas F. Jaramillo, Dong-Hwa Seo, Ji-Wook Jang","doi":"10.1038/s44160-025-00774-y","DOIUrl":"10.1038/s44160-025-00774-y","url":null,"abstract":"Hydrogen peroxide (H2O2) is not only a key eco-friendly oxidizer but also a promising energy carrier with an energy density comparable to that of compressed hydrogen. The industrial production of H2O2 relies on the energy-intensive and environmentally detrimental anthraquinone process, necessitating the exploration of greener alternatives. Here we demonstrate sustainable and unassisted electrochemical H2O2 production (via the two-electron oxygen reduction reaction) coupled to the oxidative valorization of glycerol, a biomass energy by-product, operating without external electric or solar energy inputs. We applied bismuth-loaded Pt and oxidized carbon nanotube electrocatalysts, for glycerol oxidation reaction and two-electron oxygen reduction reaction, respectively, which possess onset potentials close to the theoretical values for the electrochemical reactions. With this system, we achieved a high H2O2 production rate of approximately 8.475 μmol cm−2 min−1 and high glycerate selectivity for in situ glycerol oxidation reaction (74%), while producing renewable electricity on-site. Hydrogen peroxide (H2O2) is an eco-friendly oxidizer and a promising energy carrier, but it is primarily synthesized through the energy-intensive anthraquinone process. Here sustainable and unassisted electrochemical H2O2 production coupled to glycerol oxidation is reported, operating without an external bias or solar energy input.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 8","pages":"931-939"},"PeriodicalIF":20.0,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145123617","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

Nanocrystal synthesis with alkoxy reagents for dispersion in polar and non-polar solvents 用烷氧基试剂合成纳米晶体，用于极性和非极性溶剂的分散。

IF 2

Nature synthesis Pub Date : 2025-03-20 DOI: 10.1038/s44160-025-00764-0

Suresh Sarkar, Opeyemi H. Arogundade, Yuxiao Cui, Erick I. Hernandez Alvarez, André Schleife, Andrew M. Smith

{"title":"Nanocrystal synthesis with alkoxy reagents for dispersion in polar and non-polar solvents","authors":"Suresh Sarkar, Opeyemi H. Arogundade, Yuxiao Cui, Erick I. Hernandez Alvarez, André Schleife, Andrew M. Smith","doi":"10.1038/s44160-025-00764-0","DOIUrl":"10.1038/s44160-025-00764-0","url":null,"abstract":"Applications of colloidal nanocrystals in polar solvents often require nanocrystals synthesized in non-polar solvents. However, solvent transfer processes are problematic and deteriorate nanocrystal quality. Here we report syntheses of nanocrystals with nearly universal solvent dispersibility using ligands and solvents with alkoxy repeating units. Core syntheses, shell deposition and cation exchange proceed similarly to traditional methods while products are more stable in aqueous solution than those generated by solvent transfer. (CdSe)CdZnS nanocrystals retain photoluminescence in cells for single-particle tracking experiments and outperform other nanocrystal classes in diffusion metrics reflecting stability and resistance to non-specific binding. Distinct reaction classes yield nanocrystals with either methoxy or hydroxy ligand terminations, both of which can be purified by aqueous methods that are chemically greener than traditional methods. These reactions can further generate nanocrystals with diverse oxide, sulfide and selenide compositions, shapes and spectral bands with wide dispersibility that may make applications in polar solvents more widely accessible. Nanocrystals are synthesized with long-term colloidal stability in both polar and non-polar solvents without the need for ligand exchange. During synthesis, conventional coordinating ligands and solvents with long alkyl chains are replaced with those bearing alkoxy repeating units.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 7","pages":"826-835"},"PeriodicalIF":20.0,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144981685","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

Sintering protonic zirconate cells with enhanced electrolysis stability and Faradaic efficiency 烧结具有增强电解稳定性和法拉第效率的质子锆酸盐电池

IF 2

Nature synthesis Pub Date : 2025-03-14 DOI: 10.1038/s44160-025-00765-z

Wei Tang, Wenjuan Bian, Hanping Ding, Yong Ding, Zeyu Zhao, Quanwen Sun, Samuel Koomson, You Wang, Boshen Xu, Pei Dong, Dongchang Chen, Joshua Y. Gomez, Wuxiang Feng, Wei Wu, Meng Zhou, Yanhao Dong, Hongmei Luo, Ju Li, Dong Ding

{"title":"Sintering protonic zirconate cells with enhanced electrolysis stability and Faradaic efficiency","authors":"Wei Tang, Wenjuan Bian, Hanping Ding, Yong Ding, Zeyu Zhao, Quanwen Sun, Samuel Koomson, You Wang, Boshen Xu, Pei Dong, Dongchang Chen, Joshua Y. Gomez, Wuxiang Feng, Wei Wu, Meng Zhou, Yanhao Dong, Hongmei Luo, Ju Li, Dong Ding","doi":"10.1038/s44160-025-00765-z","DOIUrl":"10.1038/s44160-025-00765-z","url":null,"abstract":"The emerging applications of steam electrolysis and electrochemical synthesis at 300–600 °C set stringent requirements on the stability of protonic ceramic cells, which cannot be met by Ce-rich electrolytes. A promising candidate is Ce-free BaZr0.8Y0.2O3−δ, but its usage has long been hindered due to the high sintering temperatures required for protonic devices. Here we resolved the issue through a co-sintering process, in which the shrinkage stress of a readily sinterable support layer helps to densify the pure BaZr0.8Y0.2O3–δ electrolyte membrane at low temperatures. This approach eliminates Ce and harmful sintering aids in the dense zirconate electrolyte membrane, thereby enhancing the Faradaic efficiency and electrochemical stability, especially under harsh operating conditions. The protonic zirconate cells have exceptional performance and demonstrate stable high-steam pressure electrolysis up to 0.7 atm steam pressure, −2 A cm−2 current density and over 800 h of dynamic operation at 600 °C. Our processing breakthrough enables stabilized protonic cells for demanding applications in future energy infrastructure. Emerging applications of steam electrolysis and electrochemical synthesis for future hydrogen technologies at intermediate temperatures set stringent requirements on the stability of protonic ceramic cells. Now a sintering approach enables densified Ce-free protonic zirconate cells with enhanced Faradaic efficiency and exceptional stability under harsh operating conditions.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 5","pages":"592-602"},"PeriodicalIF":20.0,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145123065","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

Direct preparation of two-dimensional platelets from polymers enabled by accelerated seed formation 由加速种子形成的聚合物直接制备二维血小板

IF 2

Nature synthesis Pub Date : 2025-03-14 DOI: 10.1038/s44160-025-00767-x

Laihui Xiao, Tianlai Xia, Jian Zhang, Sam J. Parkinson, Julia Y. Rho, Andrew P. Dove, Rachel K. O’ Reilly

{"title":"Direct preparation of two-dimensional platelets from polymers enabled by accelerated seed formation","authors":"Laihui Xiao, Tianlai Xia, Jian Zhang, Sam J. Parkinson, Julia Y. Rho, Andrew P. Dove, Rachel K. O’ Reilly","doi":"10.1038/s44160-025-00767-x","DOIUrl":"10.1038/s44160-025-00767-x","url":null,"abstract":"Crystallization-driven self-assembly (CDSA) presents a facile method to access well-defined nanostructures. However, nanostructure preparation via CDSA has been constrained by prolonged processing time and limited throughput, primarily due to seed preparation and confinement to small batch scales. In turn, this limits the potential to scale up CDSA to enable application of the resultant particles. Here we report a rapid seed preparation method that drives uniform seed micelle formation by supersaturating polymer solutions in a flow system. This leads to a large reduction in processing time, from a week down to minutes. Importantly, the modular flow cascade applied can integrate both seed preparation and living CDSA, enabling end-to-end production of nanostructures directly from polymers in 3 min. The attained throughput of 132 mg h−1 surpasses that of other reported methods by orders of magnitude and, in turn, provides a step forward for the scaling-up of precision nanomaterials. Crystallization-driven self-assembly is a powerful method for accessing well-defined nanostructures, but prolonged processing times and limited throughput constrain its application. Now a flow-based strategy is introduced for the preparation of self-assembled 2D platelets from various crystallizable polymers with a reduced processing time and enhanced throughput.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 7","pages":"808-815"},"PeriodicalIF":20.0,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s44160-025-00767-x.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145123088","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