Nature synthesis最新文献_第5页

Catalyst and microenvironment design for more efficient ethanol electrosynthesis 更有效的乙醇电合成催化剂和微环境设计

Nature synthesis Pub Date : 2024-10-04 DOI: 10.1038/s44160-024-00663-w

引用次数: 0

Metal/MXene composites via in situ reduction

Nature synthesis Pub Date : 2024-10-04 DOI: 10.1038/s44160-024-00660-z

Qingxiao Zhang, Jia-ao Wang, Qinghua Yu, Qizhen Li, Runze Fan, Chong Li, Yiyi Fan, Cong Zhao, Weihua Cheng, Peiyi Ji, Jie Sheng, Chenhao Zhang, Songhai Xie, Graeme Henkelman, Hui Li

{"title":"Metal/MXene composites via in situ reduction","authors":"Qingxiao Zhang, Jia-ao Wang, Qinghua Yu, Qizhen Li, Runze Fan, Chong Li, Yiyi Fan, Cong Zhao, Weihua Cheng, Peiyi Ji, Jie Sheng, Chenhao Zhang, Songhai Xie, Graeme Henkelman, Hui Li","doi":"10.1038/s44160-024-00660-z","DOIUrl":"10.1038/s44160-024-00660-z","url":null,"abstract":"Metal/two-dimensional substrate composites offer a rich library of materials that can have application in catalysis, sensing, biotechnology and other fields. In situ reduction deposition provides a scalable method for fabricating metal/MXene composites, but the rational control of metal nanostructures growth on MXene remains difficult. Here a strategy for the in situ reduction deposition of various metals (Au, Pd, Ag, Pt, Rh, Ru and Cu) on Ti3C2Tx MXene is demonstrated. This study uncovers the guiding principles of the metal deposition process on MXene nanosheets, including the influence of redox potential, metal coordination and lattice mismatch. A series of metal/MXene composites with fine-tuned structures were constructed based on these guiding principles, such as Pd@Au-Edge/Ti3C2Tx, Pt@Au-Edge/Ti3C2Tx, Au@Ag@Au-Surface/Ti3C2Tx and Ag@Pd@Au-Edge/Ti3C2Tx. In addition, the in situ reduction strategy can be extended to other MXene materials, such as Mo2CTx, V2CTx, Ti3CNTx, Nb4C3Tx and Mo2TiC2Tx, which allows the creation of metal/MXene composites with versatile and customizable nanostructures for a wide range of applications. In situ reduction deposition is a scalable method for fabricating metal/MXene composites, but rational control remains difficult. Now an in situ reduction strategy for synthesizing metal/MXene composites with precise control over metal size, deposition site and nanostructure has been demonstrated.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 2","pages":"252-261"},"PeriodicalIF":0.0,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143397431","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

Carbon- and energy-efficient ethanol electrosynthesis via interfacial cation enrichment 界面阳离子富集的碳高效乙醇电合成

Nature synthesis Pub Date : 2024-10-04 DOI: 10.1038/s44160-024-00662-x

Ali Shayesteh Zeraati, Feng Li, Tartela Alkayyali, Roham Dorakhan, Erfan Shirzadi, Fatemeh Arabyarmohammadi, Colin P. O’Brien, Christine M. Gabardo, Jonathan Kong, Adnan Ozden, Mohammad Zargartalebi, Yong Zhao, Lizhou Fan, Panagiotis Papangelakis, Dongha Kim, Sungjin Park, Rui Kai Miao, Jonathan P. Edwards, Daniel Young, Alexander H. Ip, Edward H. Sargent, David Sinton

{"title":"Carbon- and energy-efficient ethanol electrosynthesis via interfacial cation enrichment","authors":"Ali Shayesteh Zeraati, Feng Li, Tartela Alkayyali, Roham Dorakhan, Erfan Shirzadi, Fatemeh Arabyarmohammadi, Colin P. O’Brien, Christine M. Gabardo, Jonathan Kong, Adnan Ozden, Mohammad Zargartalebi, Yong Zhao, Lizhou Fan, Panagiotis Papangelakis, Dongha Kim, Sungjin Park, Rui Kai Miao, Jonathan P. Edwards, Daniel Young, Alexander H. Ip, Edward H. Sargent, David Sinton","doi":"10.1038/s44160-024-00662-x","DOIUrl":"10.1038/s44160-024-00662-x","url":null,"abstract":"The use of acidic electrolytes in CO2 reduction avoids costly carbonate loss. However, the energy efficiency of acid-fed electrolysers has been limited by high hydrogen production and operating potentials. We find that these stem from the lack of alkali cations at the catalyst surface, limiting CO2 and CO adsorption. In acid-fed membrane electrode assembly systems, the incorporation of these cations is challenging as there is no flowing catholyte. Here an interfacial cation matrix (ICM)–catalyst heterojunction is designed that directly attaches to the catalyst layer. The negatively charged nature of the ICM enriches the alkali cation concentration near the cathode surface, trapping generated hydroxide ions. This increases the local electric field and pH, increasing multi-carbon production. Integrating the ICM strategy with a tailored copper–silver catalyst enables selective ethanol production through a proton-spillover mechanism. We report a 45% CO2-to-ethanol Faradaic efficiency at 200 mA cm−2, carbon efficiency of 63%, full-cell ethanol energy efficiency of 15% (3-fold improvement over the best previous acidic CO2 reduction value) and energy cost of 260 GJ per tonne ethanol, the lowest among reported ethanol-producing CO2 electrolysers. Acidic CO2 electroreduction is carbon efficient but suffers from low energy efficiency and selectivity. Here an interfacial cation matrix is developed to enrich alkali cations and increase the local pH at a Cu–Ag catalyst surface, improving efficiency. A 45% CO2-to-ethanol Faradaic efficiency and 15% energy efficiency for ethanol production are achieved.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 1","pages":"75-83"},"PeriodicalIF":0.0,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142995947","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

Mechanical exfoliation of non-layered metal oxides into ultrathin flakes 将非层状金属氧化物机械剥离成超薄薄片

Nature synthesis Pub Date : 2024-10-03 DOI: 10.1038/s44160-024-00657-8

Ruijie Li, Zhixin Yao, Zhenjiang Li, Lei Liao, Huacong Sun, Chaonan Cong, Xudan Huang, Kang Wu, Tingjun Wang, Huifeng Tian, PeiChi Liao, Shizhuo Liu, Yihan Wang, Lina Yang Zhang, U Sasaki, Ge Yin, Junjie Guo, Yu Ye, Xiaoding Wei, Xueyun Wang, Jiawang Hong, Jinhai Mao, Lihong Bao, Lifen Wang, Xuedong Bai, Peng Gao, Kaihui Liu, Lei Liao, Jun He, Shulin Bai, Yanfeng Zhang, Yanglong Hou, Ruqiang Zou, Hong-Jun Gao, Yue Zhang, Enge Wang, Lei Liu

{"title":"Mechanical exfoliation of non-layered metal oxides into ultrathin flakes","authors":"Ruijie Li, Zhixin Yao, Zhenjiang Li, Lei Liao, Huacong Sun, Chaonan Cong, Xudan Huang, Kang Wu, Tingjun Wang, Huifeng Tian, PeiChi Liao, Shizhuo Liu, Yihan Wang, Lina Yang Zhang, U Sasaki, Ge Yin, Junjie Guo, Yu Ye, Xiaoding Wei, Xueyun Wang, Jiawang Hong, Jinhai Mao, Lihong Bao, Lifen Wang, Xuedong Bai, Peng Gao, Kaihui Liu, Lei Liao, Jun He, Shulin Bai, Yanfeng Zhang, Yanglong Hou, Ruqiang Zou, Hong-Jun Gao, Yue Zhang, Enge Wang, Lei Liu","doi":"10.1038/s44160-024-00657-8","DOIUrl":"10.1038/s44160-024-00657-8","url":null,"abstract":"The exfoliation of layered crystals can produce diverse two-dimensional (2D) materials and heterostructures. However, the micromechanical cleavage of non-stratified materials into 2D flakes remains challenging due to z-direction consecutive bonding. Here we report a mechanical exfoliation method for producing freestanding 2D metal oxide flakes. By synchronizing the thermal decomposition of metal salts and water-assisted forming, we synthesize large-aspect-ratio lamellae of amorphous and crystalline metal oxides as parent materials, which can exfoliate to ultrathin flakes. The freestanding, transferrable features allow the room temperature integration of high-k metal oxide flakes as top-gate dielectrics in 2D material transistors. We utilize the dual-function Cr-doped AlOx flake as the gating dielectric and component, sensing and storing the visible light by photon-programming floating gate effect, showing an in-sensor computing device. Our results provide a platform to investigate the fundamental properties of ultrathin metal oxides free of substrate clamping and pave the way to metal oxides-based functional devices. A mechanical exfoliation method for producing freestanding metal oxide ultrathin flakes is reported. The flakes can be transferred and integrated with 2D materials, providing a platform to investigate the fundamental properties of ultrathin metal oxides.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 1","pages":"106-115"},"PeriodicalIF":0.0,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142995940","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 氮化薄膜的相位工程

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

Xing Ming, Xiaojun Kuang

引用次数: 0

Carbon isotopic labelling of carboxylic acids enabled by organic photoredox-catalysed cyanation 有机光氧化催化氰化作用下羧酸的碳同位素标记

Nature synthesis Pub Date : 2024-09-27 DOI: 10.1038/s44160-024-00656-9

Zhengbo Zhu, Xuedan Wu, Gerald Thomas Bida, Huaifu Deng, Xinrui Ma, Siran Qian, Zhanhong Wu, Zibo Li, David A. Nicewicz

{"title":"Carbon isotopic labelling of carboxylic acids enabled by organic photoredox-catalysed cyanation","authors":"Zhengbo Zhu, Xuedan Wu, Gerald Thomas Bida, Huaifu Deng, Xinrui Ma, Siran Qian, Zhanhong Wu, Zibo Li, David A. Nicewicz","doi":"10.1038/s44160-024-00656-9","DOIUrl":"10.1038/s44160-024-00656-9","url":null,"abstract":"The application of molecular imaging has advanced personalized medicine and generated a profound impact on patient care. Positron emission tomography and magnetic resonance imaging are among the most widely used imaging modalities, often requiring the isotopic labelling of bioactive molecules to generate the desired imaging probes. Unfortunately, radiochemistry often limits the development of novel agents due to complicated syntheses and the incompatibility of complex molecules. Here, considering the prevalence of carboxylic acids in drug and bioactive molecules, we have developed a method to perform 11/13C labelling through carboxylic acid groups via organic photoredox reactions to generate radiolabelled nitriles. We applied this strategy to a range of aliphatic carboxylic acids, including complex and functionalized drug molecules, amino acids and short peptides. Notably, when benzylic and alkyl carboxylic acids were used as substrates, a copper co-catalyst was required to obtain the labelled nitriles, whereas when α-amino acids and peptides were used as substrates, a copper co-catalyst was not required to form labelled α-amino nitriles. The radiolabelled nitrile products could be easily converted back to radiolabelled carboxylic acids with high radiochemical yields and molar activities. Positron emission tomography and magnetic resonance imaging are two powerful imaging modalities that require the installation of isotopes in biologically relevant molecules. Now an organic photoredox-catalysed method for the conversion of a range of carboxylic acids to their 11C and 13C isotopomers via decarboxylative cyanation is reported.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 1","pages":"97-105"},"PeriodicalIF":0.0,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142995920","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

Palladium-catalysed [2σ + 2π] cycloaddition reactions of bicyclo[1.1.0]butanes with aldehydes 钯催化双环[1.1.0]丁烷与醛的[2σ + 2π]环加成反应

Nature synthesis Pub Date : 2024-09-27 DOI: 10.1038/s44160-024-00659-6

Tianzhu Qin, Mengyang He, Weiwei Zi

{"title":"Palladium-catalysed [2σ + 2π] cycloaddition reactions of bicyclo[1.1.0]butanes with aldehydes","authors":"Tianzhu Qin, Mengyang He, Weiwei Zi","doi":"10.1038/s44160-024-00659-6","DOIUrl":"10.1038/s44160-024-00659-6","url":null,"abstract":"Cycloaddition reactions of bicyclo[1.1.0]butanes (BCBs) with 2π components are a powerful tool for preparing C(sp3)-rich arene bioisosteres. Despite enormous progress in this field, catalytic enantioselective cycloadditions of BCBs that produce enantioenriched three-dimensional bioisosteres are underdeveloped. Here we report a palladium-catalysed [3 + 2] cycloaddition reaction of vinyl-carbonyl-BCBs with carbonyl compounds, including formaldehyde, activated ketones, and aliphatic and aromatic aldehydes. This approach provides quick access to a wide variety of 2-oxabicyclo[2.1.1]hexanes. Density functional theory calculations indicate that the reaction occurs through a zwitterionic mechanism involving σ-bond cleavage, nucleophilic addition and allylic substitution. When (R,R)-ANDEN-phenyl Trost ligand is used, the stereoselectivity of the addition of palladium-zwitterionic enolates to carbonyl can be controlled to achieve enantioselective [3 + 2] cycloadditions. We further demonstrate the practicality of the method by carrying out several downstream transformations of cycloaddition products. Palladium catalysis enables the cycloaddition reaction between vinyl-carbonyl-bicyclo[1.1.0]butanes and aldehydes or ketones for the synthesis of 2-oxabicyclo[2.1.1]hexanes, an arene bioisotere. Enantiocontrol over the zwitterionic [2σ + 2π] cycloaddition process can be achieved using the commercially available (R,R)-ANDEN-phenyl Trost ligand.","PeriodicalId":74251,"journal":{"name":"Nature synthesis","volume":"4 1","pages":"124-133"},"PeriodicalIF":0.0,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142995868","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