Nature synthesisPub Date : 2024-10-31DOI: 10.1038/s44160-024-00669-4
Taehoon Kim, Dongchul Seo, Sungsoon Kim, Gyu Won Kim, Seung-Jae Shin, Se Young Kim, Minwoo Lee, Jihong Bae, Hansol Ra, Minjun Kim, Taeyoung Kim, Soyeon Lee, Seung-Rok Kim, Hyunmin Cho, Han Joo Lee, Jaehyeok Choi, Seongil Im, Jin-Woo Park, Jinwoo Cheon, Joon Sang Lee, Aron Walsh, Wooyoung Shim
{"title":"Anomalous in-plane electrical anisotropy in elemental metal nanosheets","authors":"Taehoon Kim, Dongchul Seo, Sungsoon Kim, Gyu Won Kim, Seung-Jae Shin, Se Young Kim, Minwoo Lee, Jihong Bae, Hansol Ra, Minjun Kim, Taeyoung Kim, Soyeon Lee, Seung-Rok Kim, Hyunmin Cho, Han Joo Lee, Jaehyeok Choi, Seongil Im, Jin-Woo Park, Jinwoo Cheon, Joon Sang Lee, Aron Walsh, Wooyoung Shim","doi":"10.1038/s44160-024-00669-4","DOIUrl":"10.1038/s44160-024-00669-4","url":null,"abstract":"Two-dimensional (2D) elemental metals, often overlooked owing to their lack of switching or dielectric properties, have the potential to exhibit unique properties unachievable by their bulk counterparts if their microstructure can be controlled. Here we propose an electrodeposition method that utilizes a confined 2D template to prepare elemental metal nanosheets with an aligned grain orientation, resulting in an exceptionally high in-plane electrical anisotropy of >103. Heterogeneous nucleation is initiated and the directed growth of the metal at the cathode is controlled within a channel whose size is smaller than the critical size of the nuclei. This leads to the formation of anisotropic microstructures, and consequently, the nanosheets exhibit anisotropic electrical properties. Unlike conventional field-effect transistors, devices employing a channel with two orthogonally separated conduction paths yield an exceptional on–off switching ratio exceeding 104. Our approach offers a promising route to produce various 2D elemental metals with properties different from those observed in their bulk counterparts and highlights the potential of anisotropic metallic nanosheets as switching elements. An electrodeposition method is proposed for the growth of elemental metal nanosheets with aligned grain orientation using a confined 2D template. Nucleation and growth are controlled within a confined 2D channel, resulting in nanosheets with high in-plane electrical anisotropy (>103), highlighting their potential as switching elements.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 1","pages":"31-42"},"PeriodicalIF":0.0,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142995874","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}
Nature synthesisPub Date : 2024-10-31DOI: 10.1038/s44160-024-00674-7
Yuanjun Chen, Edward H. Sargent
{"title":"Extended-release capsule-inspired electrocatalyst design","authors":"Yuanjun Chen, Edward H. Sargent","doi":"10.1038/s44160-024-00674-7","DOIUrl":"10.1038/s44160-024-00674-7","url":null,"abstract":"Inspired by pharmaceutical capsules, an extended-release shell to regulate catalyst surface reconstruction is developed, generating highly active sites and leading to enhanced CO2 electroreduction performance.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 1","pages":"9-10"},"PeriodicalIF":0.0,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142995876","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}
Nature synthesisPub Date : 2024-10-25DOI: 10.1038/s44160-024-00684-5
Peter W. Seavill
{"title":"Electrochemical etherification and amination","authors":"Peter W. Seavill","doi":"10.1038/s44160-024-00684-5","DOIUrl":"10.1038/s44160-024-00684-5","url":null,"abstract":"","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 11","pages":"1313-1313"},"PeriodicalIF":0.0,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142596139","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}
Nature synthesisPub Date : 2024-10-25DOI: 10.1038/s44160-024-00673-8
Kai-Liang Tao, Xing Wang, Huan Liu, Wen-Qing Chen, Yi Sun, Yun-Qian Zhang, Yu-Xi Li, Zhen-Yu Wang, Yang Ye, Hui Xu, Lefu Lan, Hui-Xiong Dai
{"title":"Multisite modifications of arenes using ketones as removable handles enabled by Pd and norbornene cooperative catalysis","authors":"Kai-Liang Tao, Xing Wang, Huan Liu, Wen-Qing Chen, Yi Sun, Yun-Qian Zhang, Yu-Xi Li, Zhen-Yu Wang, Yang Ye, Hui Xu, Lefu Lan, Hui-Xiong Dai","doi":"10.1038/s44160-024-00673-8","DOIUrl":"10.1038/s44160-024-00673-8","url":null,"abstract":"Natural products serve as crucial sources for new drugs and play an indispensable role in drug discovery. Late-stage functionalization of natural products is an efficient method for diversifying their structures, fine-tuning their biological properties and rapidly constructing molecular libraries. Polysubstituted arenes serve as structural cores in pharmaceuticals derived from natural products. However, programmable multisite arene modification remains a largely unmet challenge. Here, using commercially available and easy-to-synthesize aryl ketones as substrates, we present the programmable multifunctionalization of natural products via a palladium- and norbornene-catalysed Catellani-type reaction. Given the ease of installing an acyl group and using it as a relay, this protocol enables the incorporation of a variety of bioactive molecules into natural products via successive acylation and deacylation processes. Furthermore, this strategy was applied to the construction of a molecular library based on dehydroabietic acid. Multiple molecules with substantially increased activity were obtained through antimicrobial activity screening. Polysubstituted arenes are ubiquitous structural cores in natural products and drugs but their synthesis through programmable arene modification remains a challenge. Now, a palladium- and norbornene-catalysed Catellani-type reaction of aryl ketones, through successive acylation and deacylation, allows the synthesis of polysubstituted arenes.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 2","pages":"209-218"},"PeriodicalIF":0.0,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143397416","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}
Nature synthesisPub Date : 2024-10-25DOI: 10.1038/s44160-024-00683-6
Alison Stoddart
{"title":"Predicting enantioselectivity for diverse substrates","authors":"Alison Stoddart","doi":"10.1038/s44160-024-00683-6","DOIUrl":"10.1038/s44160-024-00683-6","url":null,"abstract":"","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 11","pages":"1315-1315"},"PeriodicalIF":0.0,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142596137","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}
Nature synthesisPub Date : 2024-10-23DOI: 10.1038/s44160-024-00676-5
Jingyang Qin, Christopher J. Teskey
{"title":"Reshaping amino acids","authors":"Jingyang Qin, Christopher J. Teskey","doi":"10.1038/s44160-024-00676-5","DOIUrl":"10.1038/s44160-024-00676-5","url":null,"abstract":"Two catalysts working together under light irradiation selectively dehydrogenate proteinogenic amino acids to yield intermediates that can be diversified into non-canonical amino acids.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 12","pages":"1451-1452"},"PeriodicalIF":0.0,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142798585","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}
Nature synthesisPub Date : 2024-10-21DOI: 10.1038/s44160-024-00680-9
Alexandra R. Groves
{"title":"Polyhedral expansion of closo-hexaboranes","authors":"Alexandra R. Groves","doi":"10.1038/s44160-024-00680-9","DOIUrl":"10.1038/s44160-024-00680-9","url":null,"abstract":"","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 11","pages":"1316-1316"},"PeriodicalIF":0.0,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142596111","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}
Nature synthesisPub Date : 2024-10-16DOI: 10.1038/s44160-024-00665-8
Kalyan Biswas, Jesús Janeiro, Aurelio Gallardo, Marco Lozano, Ana Barragán, Berta Álvarez, Diego Soler-Polo, Oleksandr Stetsovych, Andrés Pinar Solé, Koen Lauwaet, José M. Gallego, Dolores Pérez, Rodolfo Miranda, José I. Urgel, Pavel Jelínek, Diego Peña, David Écija
{"title":"Designing highly delocalized solitons by harnessing the structural parity of π-conjugated polymers","authors":"Kalyan Biswas, Jesús Janeiro, Aurelio Gallardo, Marco Lozano, Ana Barragán, Berta Álvarez, Diego Soler-Polo, Oleksandr Stetsovych, Andrés Pinar Solé, Koen Lauwaet, José M. Gallego, Dolores Pérez, Rodolfo Miranda, José I. Urgel, Pavel Jelínek, Diego Peña, David Écija","doi":"10.1038/s44160-024-00665-8","DOIUrl":"10.1038/s44160-024-00665-8","url":null,"abstract":"π-Conjugated polymers are a class of materials featuring an alternation of single and double bonds along their backbone, a configuration that can result in delocalized π-electrons. The unique electronic structure of these polymers makes them vital in applications such as organic electronics, solar cells and light-emitting diodes. A key feature in such materials is the emergence of topological quasiparticles, termed solitons, which are crucial for their observed high electrical conductivity. By using on-surface synthesis, we present a chemical reaction based on the regio- and stereoselective coupling of indenyl moieties for fabricating π-conjugated acenoindenylidene polymers, which feature a longitudinal polyacetylene backbone, on a Au(111) surface. The relationship between structural parity and electronic properties is investigated. We discover that odd-membered polymers exhibit an in-gap soliton state, which, due to their low bandgaps, spatially extends several nanometres along the longitudinal polyacetylene backbone. Our findings pave the way for the design of π-conjugated polymers that are able to host intrinsic solitons through chemical design by exploiting structural parity, without the need for external doping. An on-surface synthetic route for the regio- and stereoselective coupling of indenyl moieties, affording the design of π-conjugated acenoindenylidene polymers on Au(111), is reported. The relationship between the structural parity of the polymers and their electronic properties reveals the emergence of highly delocalized soliton quasiparticles in odd-membered polymers.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 2","pages":"233-242"},"PeriodicalIF":0.0,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143397419","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}
Nature synthesisPub Date : 2024-10-10DOI: 10.1038/s44160-024-00649-8
Richard B. Canty, Milad Abolhasani
{"title":"Reproducibility in automated chemistry laboratories using computer science abstractions","authors":"Richard B. Canty, Milad Abolhasani","doi":"10.1038/s44160-024-00649-8","DOIUrl":"10.1038/s44160-024-00649-8","url":null,"abstract":"While abstraction is critical for the transferability of automated laboratory science in (bio)chemical and materials sciences, its improper implementation is a technical debt taken against the reproducibility of experimental results. Over the decades, computer science has developed guidelines and strategies for how abstractions are captured in programming languages—particularly concerning the substitutability of implementations of abstracted ideas and the clear definition of the contexts in which abstractions are used. However, few programming languages developed for automated experiments fully leverage the wisdom learned in computer science. To achieve collaborative sharing of scientific knowledge via automated laboratories, the way that experimental protocols are codified and interpreted by machine agents must use abstractions responsibly and with reproducibility, rather than solely transferability, at its core. This Review discusses how computer science principles of abstraction can be translated to create more reproducible automation as an enabler for the acceleration of collaborative research with self-driving laboratories. Digital workflow representations in automated and autonomous chemistry laboratories can achieve transferability by using abstract concepts. However, such abstractions must abide by certain rules to ensure reproducibility. Lessons learned from computer science for responsible abstraction are translated into an automated chemistry laboratory context to guide digital workflow development towards reproducibility.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 11","pages":"1327-1339"},"PeriodicalIF":0.0,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142596131","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}