The rational design of efficient thermal‐photo CO 2 reduction catalysts necessitates synergistic integration of structural modulation and reactant activation strategies. Herein, a Mg‐doped Bi nanosphere catalyst is reported, engineered for efficient CO 2 reduction under H 2 O‐H 2 co‐feeding conditions. Mg doping not only optimizes the nanostructure by reducing the particle size but also modifies the surface charge distribution and enhances water adsorption, thereby promoting CO 2 activation and catalytic performance. Crucially, under H 2 OH 2 co‐feeding, H 2 O interacts with Bi to generate hydroxylated BiOH sites that promote CO 2 chemisorption, while H 2 supplies hydrogen species (*H) for CO 2 reduction. In situ diffuse reflectance infrared Fourier transform spectroscopy reveals a cooperative mechanism: CO 2 adsorbs on BiOH to form *CO 32− intermediates, which undergo sequential reduction facilitated by H 2 activation. This synergy achieves a CO production rate of 55.32 μmol·g −1 ·h −1 under 420 nm illumination with 100% selectivity, which is 2.4 times higher than that under a pure H 2 atmosphere. The work highlights the critical role of dopant‐driven active site engineering and reactant synergies (H 2 OH 2 ) in CO 2 valorization, providing a scalable strategy for catalytic performance enhancement.
{"title":"Enhancing Thermal‐Photocatalytic Reduction of CO 2 via H 2 O‐H 2 Co‐Feeding in Mg‐Doped Bismuth Catalysts","authors":"Haonan Li, Weimin Ma, Pei Kang, Yingxuan Li","doi":"10.1002/adsc.70239","DOIUrl":"https://doi.org/10.1002/adsc.70239","url":null,"abstract":"The rational design of efficient thermal‐photo CO <jats:sub>2</jats:sub> reduction catalysts necessitates synergistic integration of structural modulation and reactant activation strategies. Herein, a Mg‐doped Bi nanosphere catalyst is reported, engineered for efficient CO <jats:sub>2</jats:sub> reduction under H <jats:sub>2</jats:sub> O‐H <jats:sub>2</jats:sub> co‐feeding conditions. Mg doping not only optimizes the nanostructure by reducing the particle size but also modifies the surface charge distribution and enhances water adsorption, thereby promoting CO <jats:sub>2</jats:sub> activation and catalytic performance. Crucially, under H <jats:sub>2</jats:sub> OH <jats:sub>2</jats:sub> co‐feeding, H <jats:sub>2</jats:sub> O interacts with Bi to generate hydroxylated BiOH sites that promote CO <jats:sub>2</jats:sub> chemisorption, while H <jats:sub>2</jats:sub> supplies hydrogen species (*H) for CO <jats:sub>2</jats:sub> reduction. In situ diffuse reflectance infrared Fourier transform spectroscopy reveals a cooperative mechanism: CO <jats:sub>2</jats:sub> adsorbs on BiOH to form *CO <jats:sub>3</jats:sub> <jats:sup>2−</jats:sup> intermediates, which undergo sequential reduction facilitated by H <jats:sub>2</jats:sub> activation. This synergy achieves a CO production rate of 55.32 μmol·g <jats:sup>−1</jats:sup> ·h <jats:sup>−1</jats:sup> under 420 nm illumination with 100% selectivity, which is 2.4 times higher than that under a pure H <jats:sub>2</jats:sub> atmosphere. The work highlights the critical role of dopant‐driven active site engineering and reactant synergies (H <jats:sub>2</jats:sub> OH <jats:sub>2</jats:sub> ) in CO <jats:sub>2</jats:sub> valorization, providing a scalable strategy for catalytic performance enhancement.","PeriodicalId":118,"journal":{"name":"Advanced Synthesis & Catalysis","volume":"41 1","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145594173","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Natalia Kulbacka, Wangyu Shi, Sophie M. Guillaume, Jean‐François Carpentier, Jordi Benet‐Buchholz, Arjan W. Kleij
We report a method for the base‐mediated transformation of ether‐tethered acrylic ester‐based cyclic carbonates into functionalized cyclic acetals. The protocol builds on the use of hydroxyalkyl‐substituted cyclic carbonates that undergo an oxa ‐Michael addition reaction in the presence of alkyl propiolates thereby forging ( E )‐configured acrylic ether intermediates. The scope of the reaction involves the use of both five‐ and six‐membered cyclic carbonates, and correspondingly, both five‐ and six‐membered cyclic acetals can be prepared. The amount of reagents, the purification method, and the type of ester substrate all contribute to the efficiency of the transformation. Mechanistic control reactions point at the intermediacy of an alkoxide that induces an intramolecular Michael addition onto the acrylic double bond following alkoxide‐mediated formation of both an alcohol and ester in the final product. These functional groups, among others, further enable easy diversification of acetal‐based synthons.
{"title":"Domino Synthesis of Functionalized Cyclic Acetals From Organic Carbonates","authors":"Natalia Kulbacka, Wangyu Shi, Sophie M. Guillaume, Jean‐François Carpentier, Jordi Benet‐Buchholz, Arjan W. Kleij","doi":"10.1002/adsc.70248","DOIUrl":"https://doi.org/10.1002/adsc.70248","url":null,"abstract":"We report a method for the base‐mediated transformation of ether‐tethered acrylic ester‐based cyclic carbonates into functionalized cyclic acetals. The protocol builds on the use of hydroxyalkyl‐substituted cyclic carbonates that undergo an <jats:italic>oxa</jats:italic> ‐Michael addition reaction in the presence of alkyl propiolates thereby forging ( <jats:italic>E</jats:italic> )‐configured acrylic ether intermediates. The scope of the reaction involves the use of both five‐ and six‐membered cyclic carbonates, and correspondingly, both five‐ and six‐membered cyclic acetals can be prepared. The amount of reagents, the purification method, and the type of ester substrate all contribute to the efficiency of the transformation. Mechanistic control reactions point at the intermediacy of an alkoxide that induces an intramolecular Michael addition onto the acrylic double bond following alkoxide‐mediated formation of both an alcohol and ester in the final product. These functional groups, among others, further enable easy diversification of acetal‐based synthons.","PeriodicalId":118,"journal":{"name":"Advanced Synthesis & Catalysis","volume":"20 1","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145593780","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Elisabeth Söderberg, Marianne R. Molenaar, Katarzyna Zaczyk, Magnus Johansson, Martin A. Hayes, Per‐Olof Syrén
Amide bond formation is a basal transformation in synthetic chemistry and the pharmaceutical industry that is traditionally performed under harsh conditions, using excess amounts of amine and relying on coupling agents. Biocatalysis shows great potential in contributing to milder and more sustainable amide bond formation in water, in particular using the emerging family of amide bond synthetase (ABS) enzymes. Here, we use molecular dynamics, biocatalysis, and enzyme engineering to study amide bond formation in extant and ancestral ABS from Marinactinospora thermotolerans (McbA). Our results show that while being more thermostable, the C‐terminal domain that delivers the amine substrate to the adenylated acid intermediate is more flexible in ancestral McbA, presumably leading to an extended amine scope as observed experimentally from a small panel of aliphatic and aromatic substrates. An engineered ancestor of McbA harboring a single mutation that presumptively represent a catalytic shift residue when going from ancestral to modern biocatalyst, show two to ten‐fold improved conversions over its ancestral template while maintaining high thermostability, highlighting ancestral sequence reconstruction as a potent method in protein engineering. Kinetic experiments showed that the engineered ancestral enzyme had 2‐fold higher apparent kcat values in amide formation compared to extant enzyme, concomitant with relaxed substrate inhibition and loss‐of‐dependency on magnesium. Finally, we optimize ATP recycling utilizing a single polyphosphate kinase to showcase how engineered ancestral McbA together with reaction optimization is amenable for pharmacophore synthesis at a preparative scale.
{"title":"Engineering of an Ancestral McbA with Enhanced Domain Mobility Extends Biocatalytic Amide Synthesis Scope","authors":"Elisabeth Söderberg, Marianne R. Molenaar, Katarzyna Zaczyk, Magnus Johansson, Martin A. Hayes, Per‐Olof Syrén","doi":"10.1002/adsc.70232","DOIUrl":"https://doi.org/10.1002/adsc.70232","url":null,"abstract":"Amide bond formation is a basal transformation in synthetic chemistry and the pharmaceutical industry that is traditionally performed under harsh conditions, using excess amounts of amine and relying on coupling agents. Biocatalysis shows great potential in contributing to milder and more sustainable amide bond formation in water, in particular using the emerging family of amide bond synthetase (ABS) enzymes. Here, we use molecular dynamics, biocatalysis, and enzyme engineering to study amide bond formation in extant and ancestral ABS from <jats:italic>Marinactinospora thermotolerans</jats:italic> (McbA). Our results show that while being more thermostable, the C‐terminal domain that delivers the amine substrate to the adenylated acid intermediate is more flexible in ancestral McbA, presumably leading to an extended amine scope as observed experimentally from a small panel of aliphatic and aromatic substrates. An engineered ancestor of McbA harboring a single mutation that presumptively represent a catalytic shift residue when going from ancestral to modern biocatalyst, show two to ten‐fold improved conversions over its ancestral template while maintaining high thermostability, highlighting ancestral sequence reconstruction as a potent method in protein engineering. Kinetic experiments showed that the engineered ancestral enzyme had 2‐fold higher apparent <jats:italic>k</jats:italic> <jats:sub>cat</jats:sub> values in amide formation compared to extant enzyme, concomitant with relaxed substrate inhibition and loss‐of‐dependency on magnesium. Finally, we optimize ATP recycling utilizing a single polyphosphate kinase to showcase how engineered ancestral McbA together with reaction optimization is amenable for pharmacophore synthesis at a preparative scale.","PeriodicalId":118,"journal":{"name":"Advanced Synthesis & Catalysis","volume":"63 1","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145593971","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A P 4 S 10 ‐promoted [5 + 1] spiroannulation of 2‐(2‐nitrophenyl)‐indoles with cyclic ketones for the preparation of spirocyclic tetrahydrocarbolines has been described. The present approach afforded a series of structurally valuable spirocyclic tetrahydrocarbolines in moderate to good yields under metal‐free conditions. In this work, nitro reduction, C–N condensation, and spiroannulation were realized in one pot.
{"title":"P 4 S 10 ‐Promoted [5+1] Spiroannulation of 2‐(2‐Nitrophenyl)‐indoles with Cyclic Ketones to Access Spirocyclic Tetrahydrocarbolines","authors":"Qi Yin, Bin Tan, Jiao Liu, Xueao Wang, Yuhe Liu, Guo‐Jun Deng, Shanping Chen","doi":"10.1002/adsc.70244","DOIUrl":"https://doi.org/10.1002/adsc.70244","url":null,"abstract":"A P <jats:sub>4</jats:sub> S <jats:sub>10</jats:sub> ‐promoted [5 + 1] spiroannulation of 2‐(2‐nitrophenyl)‐indoles with cyclic ketones for the preparation of spirocyclic tetrahydrocarbolines has been described. The present approach afforded a series of structurally valuable spirocyclic tetrahydrocarbolines in moderate to good yields under metal‐free conditions. In this work, nitro reduction, C–N condensation, and spiroannulation were realized in one pot.","PeriodicalId":118,"journal":{"name":"Advanced Synthesis & Catalysis","volume":"48 4 1","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145593779","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A general, chemoenzymatic one‐pot procedure for the transformation of alcohols or amines to the corresponding alkene products in aqueous media has been reported. The procedure is based on the laccase‐TEMPO‐mediated oxidations of substrates and subsequent Wittig reaction. In this way, a one‐pot sequence of two consecutive reactions has been developed, which has a number of advantages such as (a) no need of purification of the intermediate products, (b) application of water as green solvent and an enzyme‐laccase as natural catalyst, (c) application of molecular oxygen as final green oxidant, and (d) formation of water as a byproduct of the oxidation step.
报道了一种在水介质中将醇或胺转化为相应的烯烃产物的一般化学酶一锅程序。该程序是基于漆酶- TEMPO -介导的底物氧化和随后的Wittig反应。通过这种方式，一个由两个连续反应组成的一锅序列已经被开发出来，它具有许多优点，例如(a)不需要对中间产物进行纯化，(b)使用水作为绿色溶剂和酶-漆酶作为天然催化剂，(c)使用分子氧作为最终绿色氧化剂，以及(d)形成水作为氧化步骤的副产物。
{"title":"Chemoenzymatic Synthesis of Alkenes from Alcohols or Amines by One‐Pot Laccase‐Mediated Oxidations and Wittig Reaction in Water","authors":"Ignacy Janicki, Piotr Kiełbasiński","doi":"10.1002/adsc.70233","DOIUrl":"https://doi.org/10.1002/adsc.70233","url":null,"abstract":"A general, chemoenzymatic one‐pot procedure for the transformation of alcohols or amines to the corresponding alkene products in aqueous media has been reported. The procedure is based on the laccase‐TEMPO‐mediated oxidations of substrates and subsequent Wittig reaction. In this way, a one‐pot sequence of two consecutive reactions has been developed, which has a number of advantages such as (a) no need of purification of the intermediate products, (b) application of water as green solvent and an enzyme‐laccase as natural catalyst, (c) application of molecular oxygen as final green oxidant, and (d) formation of water as a byproduct of the oxidation step.","PeriodicalId":118,"journal":{"name":"Advanced Synthesis & Catalysis","volume":"89 1","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145583245","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A mild and green photocatalytic strategy for synthesizing α ‐hydroxy ketones through N‐chlorosuccinimide (NCS)‐assisted decarboxylation of α ‐keto acids, followed by radical coupling and hydrogen atom transfer has been reported. The method operates at room temperature under visible light irradiation without metal catalysts, bases, or oxidants. A wide range of aromatic α ‐keto acids were smoothly converted into the expected products. The feasibility of scale‐up and sunlight‐driven reactions further highlighted its practicality. The ultraviolet–visible absorption spectra experiments ruled out the formation of electron donor–acceptor complexes, and Stern–Volmer experiments demonstrated the facilitative role of NCS in the photoinduced generation of acyl radical.
{"title":"Visible‐Light‐Induced Synthesis of α ‐Hydroxy Ketones From α ‐Keto Acids Under Mild Conditions","authors":"Wen‐Hui Yang, Ying Tong, Chen Li, Ming‐Qi Yang, Jia‐Yao Feng, Dong‐Qing Yang, Xi‐Ni Luo, Guo‐Ping Ge, Jun‐Qi Zhang, Wen‐Ting Wei","doi":"10.1002/adsc.70217","DOIUrl":"https://doi.org/10.1002/adsc.70217","url":null,"abstract":"A mild and green photocatalytic strategy for synthesizing <jats:italic>α</jats:italic> ‐hydroxy ketones through N‐chlorosuccinimide (NCS)‐assisted decarboxylation of <jats:italic>α</jats:italic> ‐keto acids, followed by radical coupling and hydrogen atom transfer has been reported. The method operates at room temperature under visible light irradiation without metal catalysts, bases, or oxidants. A wide range of aromatic <jats:italic>α</jats:italic> ‐keto acids were smoothly converted into the expected products. The feasibility of scale‐up and sunlight‐driven reactions further highlighted its practicality. The ultraviolet–visible absorption spectra experiments ruled out the formation of electron donor–acceptor complexes, and Stern–Volmer experiments demonstrated the facilitative role of NCS in the photoinduced generation of acyl radical.","PeriodicalId":118,"journal":{"name":"Advanced Synthesis & Catalysis","volume":"107 1","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145583244","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Peng Guo, Guoliang Pu, Lin‐Yuan Zeng, Man Chen, Pan Wang, Jia Jia, Xuefei Li, Pan–Pan Zhou, Chun‐Yang He
α‐CF 3 ‐substituted alkenes are a class of highly important building blocks. Herein, a new phenol‐based catalytic system is developed that facilitates the elimination of trifluoromethylated alkyl bromides to produce trifluoromethylated alkenes‐a process previously deemed challenging. This method is distinguished by its mild reaction conditions, extensive substrate compatibility, and high chemo‐selectivity and regioselectivity. This facile elimination can be plausibly attributed to phenoxide anion–secondary trifluoromethylated alkyl bromides weak interactions.
{"title":"Phenoxide‐Catalyzed Synthesis of Trifluoromethylated Alkenes from Trifluoromethylated Alkyl Bromides","authors":"Peng Guo, Guoliang Pu, Lin‐Yuan Zeng, Man Chen, Pan Wang, Jia Jia, Xuefei Li, Pan–Pan Zhou, Chun‐Yang He","doi":"10.1002/adsc.70175","DOIUrl":"https://doi.org/10.1002/adsc.70175","url":null,"abstract":"α‐CF <jats:sub>3</jats:sub> ‐substituted alkenes are a class of highly important building blocks. Herein, a new phenol‐based catalytic system is developed that facilitates the elimination of trifluoromethylated alkyl bromides to produce trifluoromethylated alkenes‐a process previously deemed challenging. This method is distinguished by its mild reaction conditions, extensive substrate compatibility, and high chemo‐selectivity and regioselectivity. This facile elimination can be plausibly attributed to phenoxide anion–secondary trifluoromethylated alkyl bromides weak interactions.","PeriodicalId":118,"journal":{"name":"Advanced Synthesis & Catalysis","volume":"223 1","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145583246","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yan Cao, Jing Wang, Wei Chen, Jianwei Wang, Linqi Wang, Xiaolong Wang, Jun Ying
A novel palladium‐catalyzed four‐component tandem sulfonylation and carbonylation of 1,6‐enynes has been developed for the rapid construction of succinimide, sulfone, and carbonyl motifs simultaneously. In the presence of very low palladium catalyst loading, the reaction of 1,6‐enynes with nucleophiles proceeded smoothly to afford a wide range of sulfone‐ and carbonyl‐containing succinimide derivatives with high yields and excellent selectivity. Notably, modifications of bioactive molecules were also demonstrated by using this method.
{"title":"Palladium‐Catalyzed Four‐Component Tandem Sulfonylation and Carbonylation of 1,6‐Enynes","authors":"Yan Cao, Jing Wang, Wei Chen, Jianwei Wang, Linqi Wang, Xiaolong Wang, Jun Ying","doi":"10.1002/adsc.70226","DOIUrl":"https://doi.org/10.1002/adsc.70226","url":null,"abstract":"A novel palladium‐catalyzed four‐component tandem sulfonylation and carbonylation of 1,6‐enynes has been developed for the rapid construction of succinimide, sulfone, and carbonyl motifs simultaneously. In the presence of very low palladium catalyst loading, the reaction of 1,6‐enynes with nucleophiles proceeded smoothly to afford a wide range of sulfone‐ and carbonyl‐containing succinimide derivatives with high yields and excellent selectivity. Notably, modifications of bioactive molecules were also demonstrated by using this method.","PeriodicalId":118,"journal":{"name":"Advanced Synthesis & Catalysis","volume":"1 1","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145567410","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The global demand for amino acids continues to rise, yet traditional synthesis methods face environmental and safety challenges. To contribute to a sustainable future vision, we herein report a novel cofactor‐neutral in vitro multienzyme cascade that directly converts methanol, a renewable C1 feedstock, into glycine under mild conditions. A two‐step strategy achieves 82.2% methanol‐to‐glycolaldehyde and 86.0% glycolaldehyde‐to‐glycine conversion, respectively. At 500 mM methanol, it yields 18.8 mM glycine after 6 h, which represents a 26.8‐fold improvement over the one‐pot approach. These results demonstrate the potential of modular in vitro multienzyme catalysis for efficient C1‐to‐amino acid transformation and establish a foundation for the synthesis of many other complex nitrogen‐containing molecules.
全球对氨基酸的需求持续增长，但传统的合成方法面临环境和安全挑战。为了促进可持续的未来愿景，我们在此报道了一种新的辅助因子中性体外多酶级联，可在温和条件下直接将甲醇（一种可再生的C1原料）转化为甘氨酸。两步策略分别实现了82.2%的甲醇制乙醇醛和86.0%的乙醇醛制甘氨酸的转化率。在500 mM的甲醇条件下，6小时后产生18.8 mM的甘氨酸，这比单罐方法提高了26.8倍。这些结果证明了模块化体外多酶催化高效C1 - to -氨基酸转化的潜力，并为许多其他复杂含氮分子的合成奠定了基础。
{"title":"Glycine Synthesis From Methanol by a Cofactor‐Neutral In Vitro Multienzyme Cascade","authors":"Ranran Wu, Fei Li, Kaiyang Lian, Dingyu Liu, Huifeng Jiang, Zhiguang Zhu","doi":"10.1002/adsc.70238","DOIUrl":"https://doi.org/10.1002/adsc.70238","url":null,"abstract":"The global demand for amino acids continues to rise, yet traditional synthesis methods face environmental and safety challenges. To contribute to a sustainable future vision, we herein report a novel cofactor‐neutral in vitro multienzyme cascade that directly converts methanol, a renewable C1 feedstock, into glycine under mild conditions. A two‐step strategy achieves 82.2% methanol‐to‐glycolaldehyde and 86.0% glycolaldehyde‐to‐glycine conversion, respectively. At 500 mM methanol, it yields 18.8 mM glycine after 6 h, which represents a 26.8‐fold improvement over the one‐pot approach. These results demonstrate the potential of modular in vitro multienzyme catalysis for efficient C1‐to‐amino acid transformation and establish a foundation for the synthesis of many other complex nitrogen‐containing molecules.","PeriodicalId":118,"journal":{"name":"Advanced Synthesis & Catalysis","volume":"1 1","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554631","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tehmina Akram, Chuang Niu, Wen‐Jie Qiu, Guan‐Wu Wang
Skeletal editing has been achieved through triflic anhydride‐mediated O‐to‐N swapping reaction of 3,3‐diarylbenzofuranones with benzonitriles/benzyl/alkyl nitriles, successfully affording 3,3‐diarylisoindolinones. A possible reaction mechanism with triflic anhydride serving as a key mediator is proposed to explain this conversion. The present reaction features a broad substrate scope, excellent functional group tolerance and high yields, expanding the structural diversity of isoindolinones.
骨架编辑是通过三酸酐介导的3,3 -二芳基苯并呋喃酮与苯并腈/苄基/烷基腈的O - to - N交换反应实现的，成功地生成3,3 -二芳基异吲哚酮。提出了一种以三酸酐为主要介质的反应机理来解释这种转化。该反应具有底物范围广、官能团耐受性好、产率高等特点，扩大了异吲哚酮的结构多样性。
{"title":"An O‐to‐N Swapping Reaction via Triflic Anhydride‐Mediated Lactamization of 3,3‐Diarylbenzofuranones with Nitriles","authors":"Tehmina Akram, Chuang Niu, Wen‐Jie Qiu, Guan‐Wu Wang","doi":"10.1002/adsc.70230","DOIUrl":"https://doi.org/10.1002/adsc.70230","url":null,"abstract":"Skeletal editing has been achieved through triflic anhydride‐mediated O‐to‐N swapping reaction of 3,3‐diarylbenzofuranones with benzonitriles/benzyl/alkyl nitriles, successfully affording 3,3‐diarylisoindolinones. A possible reaction mechanism with triflic anhydride serving as a key mediator is proposed to explain this conversion. The present reaction features a broad substrate scope, excellent functional group tolerance and high yields, expanding the structural diversity of isoindolinones.","PeriodicalId":118,"journal":{"name":"Advanced Synthesis & Catalysis","volume":"103 1","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554633","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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