Nature synthesis最新文献_第2页

Reproducibility in automated chemistry laboratories using computer science abstractions 利用计算机科学抽象技术实现自动化化学实验室的可重复性

Nature synthesis Pub Date : 2024-10-10 DOI: 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}

引用次数: 0

C–N coupling with cobalt 与钴的 C-N 耦合

Nature synthesis Pub Date : 2024-10-01 DOI: 10.1038/s44160-024-00668-5

Thomas West

引用次数: 0

Nitrogenated products from polyolefins 聚烯烃氮化产品

Nature synthesis Pub Date : 2024-10-01 DOI: 10.1038/s44160-024-00667-6

Peter W. Seavill

引用次数: 0

Selective coupling on molecular catalysts 分子催化剂上的选择性偶联

Nature synthesis Pub Date : 2024-10-01 DOI: 10.1038/s44160-024-00670-x

Alexandra R. Groves

引用次数: 0

Phase engineering of nitride thin films

Nature synthesis Pub Date : 2024-09-30 DOI: 10.1038/s44160-024-00666-7

Xing Ming, Xiaojun Kuang

引用次数: 0

Enhanced hydrogen peroxide photosynthesis in covalent organic frameworks through induced asymmetric electron distribution 通过诱导不对称电子分布增强共价有机框架中的过氧化氢光合作用

Nature synthesis Pub Date : 2024-09-19 DOI: 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":"Covalent organic frameworks (COFs) can be used as photocatalysts for the direct photosynthesis of hydrogen peroxide (H2O2) from oxygen, water and sunlight. However, their highly symmetric structure can lead to weak adsorption of O2 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 O2 species, which promotes photocatalytic H2O2 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 O2 adsorption interaction and a record-breaking solar-to-chemical conversion efficiency of 1.22% for direct photosynthesis of H2O2 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.<figure></figure>","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"23 1","pages":""},"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}

引用次数: 0

A singly bonded gallanediyl with redox-active and redox-inert reactivity 具有氧化还原活性和氧化还原惰性的单键加兰二基

Nature synthesis Pub Date : 2024-09-19 DOI: 10.1038/s44160-024-00639-w

Simon H. F. Schreiner, Tobias Rüffer, Robert Kretschmer

引用次数: 0

External forces align supramolecular materials 外力调整超分子材料

Nature synthesis Pub Date : 2024-09-16 DOI: 10.1038/s44160-024-00647-w

Matthew J. Harrington

引用次数: 0

Interfacially coupled Cu-cluster/GaN photocathode for efficient CO2 to ethylene conversion 用于将二氧化碳高效转化为乙烯的簇间耦合铜/氮化镓光电阴极

Nature synthesis Pub Date : 2024-09-12 DOI: 10.1038/s44160-024-00648-9

Bingxing Zhang, Peng Zhou, Zhengwei Ye, Ishtiaque Ahmed Navid, Yuyang Pan, Yixin Xiao, Kai Sun, Zetian Mi

{"title":"Interfacially coupled Cu-cluster/GaN photocathode for efficient CO2 to ethylene conversion","authors":"Bingxing Zhang, Peng Zhou, Zhengwei Ye, Ishtiaque Ahmed Navid, Yuyang Pan, Yixin Xiao, Kai Sun, Zetian Mi","doi":"10.1038/s44160-024-00648-9","DOIUrl":"10.1038/s44160-024-00648-9","url":null,"abstract":"The photoelectrochemical synthesis of valuable multicarbon products from carbon dioxide, sunlight and water is a promising pathway for clean energy generation and carbon neutrality. However, it is challenging to create and stabilize efficient C–C coupling sites to achieve multicarbon products with high selectivity, yield and stability. Here we designed a low-coordinated copper-cluster catalyst interfacially coupled in situ with a GaN nanowire photocathode, achieving a high ethylene Faradaic efficiency of ∼61% and a partial current density of 14.2 mA cm−2, with a robust stability of ∼116 h. The in situ self-optimized Ga–N–O interface was confirmed to facilitate and stabilize the interfacially oxidized copper species of copper clusters, which function as efficient C–C coupling sites for ethylene production. Furthermore, the hydrogen-feeding effect of GaN for promoting CO hydrogenation also guides the facile CHO-involved C–C coupling pathway. This work sheds light on the interface design and understanding of efficient and stable (photo)electrosynthesis of highly valuable fuels from CO2. An interfacially coupled Cu-cluster/GaN photocathode is designed to overcome the efficiency and stability bottlenecks in photoelectrochemical CO2 reduction to multicarbon products. The self-optimized Ga–N–O interface facilitates and stabilizes interfacially oxidized copper species of copper clusters, which function as efficient C–C coupling sites for ethylene production.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 12","pages":"1567-1576"},"PeriodicalIF":0.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195611","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

Computational analysis of modular diazotransfer reactions for the development of predictive reactivity models and diazotransfer reagents 对模块重氮转移反应进行计算分析，以开发预测性反应模型和重氮转移试剂

Nature synthesis Pub Date : 2024-09-10 DOI: 10.1038/s44160-024-00633-2

Meng-Meng Zheng, Liu Cai, Tiancheng Ma, Hao-Dong Tan, Xiaoyu Lai, Jiajia Dong, Xiao-Song Xue

{"title":"Computational analysis of modular diazotransfer reactions for the development of predictive reactivity models and diazotransfer reagents","authors":"Meng-Meng Zheng, Liu Cai, Tiancheng Ma, Hao-Dong Tan, Xiaoyu Lai, Jiajia Dong, Xiao-Song Xue","doi":"10.1038/s44160-024-00633-2","DOIUrl":"10.1038/s44160-024-00633-2","url":null,"abstract":"The development of the sulfur(VI)–fluoride exchange (SuFEx) and modular diazotransfer (MoDAT) reactions represent important milestones in the evolution of click chemistry. However, their reactivity profiles, chemoselectivity origins and underlying mechanisms remain unclear. Here we report a computational study of the MoDAT and SuFEx pathways, focusing on the reaction between the diazotransfer reagent fluorosulfuryl azide and primary amines. Our calculations reveal that the MoDAT reaction possesses a small kinetic barrier and a strong driving force, making it kinetically and thermodynamically more favourable than the SuFEx reaction. Through mechanistic scrutiny and structure–activity relationship studies, we have formulated predictive models for the reactivity and selectivity of the MoDAT reaction. Leveraging these insights, an easy-to-prepare and easily handled diazotransfer reagent with excellent reactivity has been developed, which holds broad promise for applications in chemistry and biology. Computational analysis of competing sulfur(VI)–fluoride exchange and modular diazotransfer pathways in the reaction between primary amines and fluorosulfuryl azide reveals that diazotransfer is more kinetically and thermodynamically favoured. Predictive models are formulated by combining mechanistic analysis and structure–activity relationship studies, enabling the development of an easy-to-prepare and highly reactive diazotransfer reagent.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"3 12","pages":"1507-1517"},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142195626","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