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":null,"pages":null},"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/s44160-024-00683-6
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":null,"pages":null},"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 : 2024-10-21DOI: 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":null,"pages":null},"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 : 2024-10-10DOI: 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":null,"pages":null},"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}
Nature synthesisPub Date : 2024-10-01DOI: 10.1038/s44160-024-00667-6
Peter W. Seavill
{"title":"Nitrogenated products from polyolefins","authors":"Peter W. Seavill","doi":"10.1038/s44160-024-00667-6","DOIUrl":"10.1038/s44160-024-00667-6","url":null,"abstract":"","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142415410","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 : 2024-10-01DOI: 10.1038/s44160-024-00670-x
Alexandra R. Groves
{"title":"Selective coupling on molecular catalysts","authors":"Alexandra R. Groves","doi":"10.1038/s44160-024-00670-x","DOIUrl":"10.1038/s44160-024-00670-x","url":null,"abstract":"","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142415397","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 : 2024-09-19DOI: 10.1038/s44160-024-00644-z
Youxing Liu, Lu Li, Zhiyuan Sang, Hao Tan, Na Ye, Chenglong Sun, Zongqiang Sun, Mingchuan Luo, Shaojun Guo
{"title":"Enhanced hydrogen peroxide photosynthesis in covalent organic frameworks through induced asymmetric electron distribution","authors":"Youxing Liu, Lu Li, Zhiyuan Sang, Hao Tan, Na Ye, Chenglong Sun, Zongqiang Sun, Mingchuan Luo, Shaojun Guo","doi":"10.1038/s44160-024-00644-z","DOIUrl":"https://doi.org/10.1038/s44160-024-00644-z","url":null,"abstract":"<p>Covalent organic frameworks (COFs) can be used as photocatalysts for the direct photosynthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) from oxygen, water and sunlight. However, their highly symmetric structure can lead to weak adsorption of O<sub>2</sub> and, therefore, unsatisfactory photocatalytic performance. Here we explore the local asymmetric electron distribution induced by Pauli and electron–electron repulsion in COFs to construct localized bonding sites for O<sub>2</sub> species, which promotes photocatalytic H<sub>2</sub>O<sub>2</sub> production. Experimental results and theoretical calculations reveal that TAPT–FTPB COFs (where TAPT is 1,3,5-tris-(4-aminophenyl) triazine and FTPB is 5-(5-formylthiophen-2-yl)thiophene-2-carbaldehyde) with an asymmetric electron distribution show strong O<sub>2</sub> adsorption interaction and a record-breaking solar-to-chemical conversion efficiency of 1.22% for direct photosynthesis of H<sub>2</sub>O<sub>2</sub> from oxygen and water, which is higher than in the photosynthesis of plants (~0.1%). A flow-type photocatalytic microreactor integrated with TAPT–FTPB COFs exhibits 100% sterilization efficiency for killing bacteria and 97.8% conversion for photocatalytic 2-thiophene methylamine coupling. This work reports a strategy for manipulating the local electron distribution in COFs, opening the door for research on the rational design of high-performance photocatalysis with a local asymmetric electron distribution.</p><figure></figure>","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251972","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 : 2024-09-19DOI: 10.1038/s44160-024-00639-w
Simon H. F. Schreiner, Tobias Rüffer, Robert Kretschmer
{"title":"A singly bonded gallanediyl with redox-active and redox-inert reactivity","authors":"Simon H. F. Schreiner, Tobias Rüffer, Robert Kretschmer","doi":"10.1038/s44160-024-00639-w","DOIUrl":"https://doi.org/10.1038/s44160-024-00639-w","url":null,"abstract":"<p>Singly bonded metallylenes (R–M:) of the group 13 elements feature a non-bonding pair of electrons together with two vacant orbitals, which makes them highly reactive ambiphiles that readily activate small molecules by oxidative addition. As a consequence of their pronounced reactivity, examples of organometallics with singly bonded aluminium(I) and gallium(I) centres remain rare. Here we report the one-step synthesis of a monomeric gallium(I) compound that readily undergoes oxidative addition reactions and, more remarkably, carbometalation reactions with alkynes by retention of the low +I oxidation state and the singly bonded nature of gallium. This observation contrasts with common reports on the reactivity of low-valent main-group compounds, which are regularly oxidized to compounds in a more stable higher oxidation state. This approach provides access to low-valent main-group compounds and paves the way for the development of bond-functionalization strategies that may enable the discovery of catalytic processes in the future.</p><figure></figure>","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142251973","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}
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