Helvetica Chimica Acta最新文献_第2页

Cost-Effective and Scalable Enzyme-Mediated Preparation of Short-Chain Primary Amines 经济高效、可扩展的酶介导短链伯胺制备技术

IF 1.5 4区化学

Helvetica Chimica Acta Pub Date : 2024-06-27 DOI: 10.1002/hlca.202400078

Stefania Gianolio, Beatrice Rassati, Francesca Paradisi

{"title":"Cost-Effective and Scalable Enzyme-Mediated Preparation of Short-Chain Primary Amines","authors":"Stefania Gianolio, Beatrice Rassati, Francesca Paradisi","doi":"10.1002/hlca.202400078","DOIUrl":"10.1002/hlca.202400078","url":null,"abstract":"Amines, crucial components in various industries, play a pivotal role in the synthesis of pharmaceuticals, agrochemicals, and specialty chemicals. Recognizing the environmental impact of conventional methods for their preparation, our study centers on the utilization of abundantly available natural molecules, specifically amino acids, as precursors for short chain amine synthesis. This paper focuses on the biocatalyst, L-valine decarboxylase from Streptomyces viridifaciens (VlmD), delving into the substrate scope, catalytic activity, and cost-effective scalability of an enzymatic process for amine synthesis. Additionally, we investigate the feasibility of immobilizing VlmD, aiming to pave the way for its effective use in industrial applications. Our study exploits the SpinChem system and provides a comprehensive understanding of the potential and limitations of this biocatalyst. Notably, our yields for key amines (8.42 g ⋅ d−1 for isobutylamine, 5.23 g ⋅ d−1 for isoamylamine, 5.16 g ⋅ d−1 for (S)-2-methylbutylamine, 3.78 g ⋅ d−1 for 3-(methylthio)propylamine, and 10.52 g ⋅ d−1 for (R)-1-amino-2-propanol) demonstrate the process efficiency and potential for industrial scalability.","PeriodicalId":12842,"journal":{"name":"Helvetica Chimica Acta","volume":null,"pages":null},"PeriodicalIF":1.5,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/hlca.202400078","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141509277","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A Novel, Industrially-feasible Synthetic Route to (+)-Biotin from L-Cysteine 从 L-半胱氨酸合成 (+)- 生物素的新颖、工业上可行的合成路线

IF 1.5 4区化学

Helvetica Chimica Acta Pub Date : 2024-06-20 DOI: 10.1002/hlca.202400090

Qiongmei Zhang, Kun Peng, Werner Bonrath, Zili Zhang, Zhibin Zhu, Yuehan Xing, Xiaoyan Wang, Bo Gao, Jonathan A. Medlock

引用次数: 0

The Relation between Nature and Stability of H2-Dissociating Sites and Propene Selectivity in Silica-Supported (Ga,Al)2O3 Mixed Oxide Propane Dehydrogenation Catalysts 二氧化硅支撑（Ga,Al）2O3 混合氧化物丙烷脱氢催化剂中 H2 分解位点的性质和稳定性与丙烯选择性之间的关系

IF 1.5 4区化学

Helvetica Chimica Acta Pub Date : 2024-06-18 DOI: 10.1002/hlca.202400076

Pedro Castro-Fernández, Alexander I. Serykh, Melis Yarar, Deni Mance, Paula M. Abdala, Christophe Copéret, Alexey Fedorov, Christoph R. Müller

{"title":"The Relation between Nature and Stability of H2-Dissociating Sites and Propene Selectivity in Silica-Supported (Ga,Al)2O3 Mixed Oxide Propane Dehydrogenation Catalysts","authors":"Pedro Castro-Fernández, Alexander I. Serykh, Melis Yarar, Deni Mance, Paula M. Abdala, Christophe Copéret, Alexey Fedorov, Christoph R. Müller","doi":"10.1002/hlca.202400076","DOIUrl":"https://doi.org/10.1002/hlca.202400076","url":null,"abstract":"Colloidal solutions of gallia-alumina (Ga,Al)2O3(x:y) solid-solution nanoparticles with nominal atomic Ga : Al (x:y) ratios of 1 : 6, 1 : 3, 3 : 1, and 1:0 were used to prepare silica-supported catalysts for propane dehydrogenation (PDH). A comparison of the unsupported and silica-supported catalysts reveals that the dispersion on silica increases the Ga-normalized PDH rates for all catalysts, albeit with a notably lower propene selectivity for (Ga,Al)2O3(1:6)/SiO2. Fourier transform infrared (FTIR) spectroscopy allows contrasting the H2 dissociation sites in the calcined and H2-treated (Ga,Al)2O3(x:y)/SiO2, indicating a transformation of Ga3+ surface sites with Al (mainly) and Ga atoms in the second coordination sphere (Ga(Al/Ga) sites) in the calcined (Ga,Al)2O3(1:6)/SiO2 to predominantly Ga(Ga/Si) surface sites in the H2-treated material. The resulting sites are similarly unselective as in amorphous gallia on silica. H2 produced during the PDH reaction can cause a similar transformation as H2 pretreatment in (Ga,Al)2O3(1:6)/SiO2, rapidly resulting in a notably lowered selectivity. The stable and selective Ga(Al/Ga) surface sites in (Ga,Al)2O3(1:3)/SiO2 yield a Ga−H band at ca. 1990 cm−1 under H2 dissociation conditions while the less selective surface sites, observed for the other Ga : Al ratios, give Ga−H bands at ca. 2040 and 2060 cm−1.","PeriodicalId":12842,"journal":{"name":"Helvetica Chimica Acta","volume":null,"pages":null},"PeriodicalIF":1.5,"publicationDate":"2024-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/hlca.202400076","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142002523","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cover Picture: (Helv. Chim. Acta 6/2024) 封面图片： (Helv. Chim. Acta 6/2024)

IF 1.8 4区化学

Helvetica Chimica Acta Pub Date : 2024-06-14 DOI: 10.1002/hlca.202470601

引用次数: 0

Elastomers Based on Polynorbornene with Polar Polysiloxane Brushes for Soft Transducer Applications 基于聚降冰片烯的弹性体与极性聚硅氧烷刷，用于软传感器应用

IF 1.5 4区化学

Helvetica Chimica Acta Pub Date : 2024-06-10 DOI: 10.1002/hlca.202400032

Yeerlan Adeli, Thulasinath Raman Venkatesan, Frank A. Nüesch, Dorina M. Opris

{"title":"Elastomers Based on Polynorbornene with Polar Polysiloxane Brushes for Soft Transducer Applications","authors":"Yeerlan Adeli, Thulasinath Raman Venkatesan, Frank A. Nüesch, Dorina M. Opris","doi":"10.1002/hlca.202400032","DOIUrl":"10.1002/hlca.202400032","url":null,"abstract":"Elastomers based on cross-linked bottlebrush polymers combine an extreme softness at low strains with a strain-stiffening effect, which makes them attractive as active components in dielectric elastomer actuators (DEA). Their main disadvantage concerns the small relative permittivity, which is about 3.5, requiring relatively high driving voltage in actuators. We synthesized a bottlebrush polymer elastomer with polar brushes, which exhibit an enhanced dielectric permittivity of 4.4. Anionic ring-opening polymerization of a polar cyclosiloxane gave telechelic polar brushes, while ring-opening polymerization of a norbornene macromonomer gave a bottlebrush polymer which was cross-linked to elastomers by a thiol-ene reaction. Elastomers with a small elastic modulus below 100 kPa, strain at break exceeding 100 %, attractive elasticity, and small mechanical loss factors (tanδ) were achieved. Temperature-dependent impedance measurements revealed a transition temperature of −95 °C and an interfacial polarization. The multigram scale synthesis demonstrates the potential for scaling up, which opens the door to broader applications of these materials beyond actuators, such as capacitive sensors, batteries, and electroluminescent devices. Notably, these devices operate at extremely low voltages where the dielectric breakdown does not limit their functionality, but still, the softness and the increased dielectric permittivity are a plus.","PeriodicalId":12842,"journal":{"name":"Helvetica Chimica Acta","volume":null,"pages":null},"PeriodicalIF":1.5,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/hlca.202400032","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141363525","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Nickel(II)-Catalyzed Hydrocarbamoylation of Alkynes with Formamides towards Unsaturated Amides 镍（II）催化的炔烃与甲酰胺的氢氨基化反应，生成不饱和酰胺

IF 1.5 4区化学

Helvetica Chimica Acta Pub Date : 2024-06-03 DOI: 10.1002/hlca.202400020

Tiangui Li, Shiyang Wang, Zongxiang Xia, Jinbo Zhao, Dongyue Zhang, Yuanqi Wu, Yu Liu

引用次数: 0

Diversity of Structures and Bonding in Alkali Metal Ureaphosphanes 碱金属脲膦的结构和键合多样性

IF 1.5 4区化学

Helvetica Chimica Acta Pub Date : 2024-05-28 DOI: 10.1002/hlca.202400077

Michelle H. Crabbe, Alan R. Kennedy, Catherine E. Weetman, Robert E. Mulvey

{"title":"Diversity of Structures and Bonding in Alkali Metal Ureaphosphanes","authors":"Michelle H. Crabbe, Alan R. Kennedy, Catherine E. Weetman, Robert E. Mulvey","doi":"10.1002/hlca.202400077","DOIUrl":"10.1002/hlca.202400077","url":null,"abstract":"While organoelement compounds of lithium, sodium and potassium have been much studied for decades and consequently have found forests of applications, those of the heavier alkali metals, rubidium and caesium would barely manage to fill a tree. However, recently the literature has seen some little growth spurts with these metals, hinting at a possible fertile future in areas such as homogeneous catalysis provided more work is put into their fundamental development. Here we report the synthesis and crystal structures of lithium, rubidium and caesium derivatives of the ureaphosphane Ph2PCH2CH2NHC(=O)NHPh, chosen because it offers O, N, P, and π-coordination sites. Though one may expect such alkali metal compounds to be essentially similar, the caesium complex has novel features where Cs+ engages in a side-on coordination to the C=O bond and in a weak bond to the P centre, both of which are absent in the Rb structure. Less surprisingly, the lithium derivative is tetrameric in contrast to the infinite networks of the rubidium and caesium structures. All alkali metal derivatives were made with deprotonating the ureaphosphane by a suitable base, including the sodium and potassium complexes though these two complexes could not be obtained in a crystalline form.","PeriodicalId":12842,"journal":{"name":"Helvetica Chimica Acta","volume":null,"pages":null},"PeriodicalIF":1.5,"publicationDate":"2024-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/hlca.202400077","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141191595","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cover Picture: (Helv. Chim. Acta 5/2024) 封面图片： (Helv. Chim. Acta 5/2024)

IF 1.8 4区化学

Helvetica Chimica Acta Pub Date : 2024-05-15 DOI: 10.1002/hlca.202470501

引用次数: 0

A Highly Efficient Click Linker for Enrichment of Alkyne-Tagged Proteins in Living Cells 用于活细胞中烯炔标记蛋白质富集的高效点击链接器

IF 1.8 4区化学

Helvetica Chimica Acta Pub Date : 2024-05-10 DOI: 10.1002/hlca.202400031

Guoting Qin, Shara Duong, Yunxin Fu, Chengzhi Cai

引用次数: 0

Fluorescent Membrane Probes Obey the Israelachvili Rules 遵守伊斯拉赫维利规则的荧光膜探针

IF 1.5 4区化学

Helvetica Chimica Acta Pub Date : 2024-05-09 DOI: 10.1002/hlca.202400062

Felix Bayard, Stefan Matile

{"title":"Fluorescent Membrane Probes Obey the Israelachvili Rules","authors":"Felix Bayard, Stefan Matile","doi":"10.1002/hlca.202400062","DOIUrl":"10.1002/hlca.202400062","url":null,"abstract":"When developing fluorescent membrane probes, we naturally tend to focus on the fluorophore itself. In this study, we show that sometimes it can be beneficial to shift attention from the center to the periphery, to maximize multiple interfacing with complex changing environments. Palmitylation for hydrophobic interfacing and glutamate dendrons for hydrophilic interfacing are combined to improve the performance of fluorescent flipper probes. We show that to increase performance in membranes, solubility in water is important, and to increase solubility in water, we increase the hydrophobicity of the flipper probe. These seemingly paradoxical measures are taken to satisfy the Israelachvili rules. They state that only inverted cone amphiphiles form soluble micelles in water, while inverted micelles from cone shaped amphiphiles precipitate into hexagonal 1 supramolecular polymers, and the intermediate cylindrical amphiphiles show intermediate behavior dominated by bilayers and lamellar precipitates. The normal micelles obtained from inverted cone flipper amphiphiles prevent precipitation and prepare for efficient transfer into the lipid bilayer membranes. The results are flippers that break all records set by the 2016 original with regard to effective brightness, responsiveness to membrane order, anchoring in disordered membranes, partitioning into membranes of high order, and stable labeling of membranes of interest. The lessons learned confirm the obvious: The Israelachvili rules apply also to fluorescent membrane probes. They promise literally bright perspectives for fluorescent membrane probes.","PeriodicalId":12842,"journal":{"name":"Helvetica Chimica Acta","volume":null,"pages":null},"PeriodicalIF":1.5,"publicationDate":"2024-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/hlca.202400062","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140937609","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0