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Enhancing Photocatalytic Redox Activity of Polymeric Carbon Nitride for Valuable Fluorinated Heterocycles through Fast-Track Electron Highways 通过快速电子高速公路增强聚合氮化碳的光催化氧化还原活性,以生产有价值的氟化杂环化合物
IF 12.9 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-15 DOI: 10.1021/acscatal.4c02395
Chong Wang, Shiru Lin, Yichun Lu, Yuchen Hou, Oleksandr Savateev, Jiajia Cheng
The ionic structure of poly(heptazine imides) has a strong implication in photocatalytic hydrogen generation. From numerous reports, it is evident that these materials are also superior to covalent carbon nitrides in various organic transformations. However, the reason has been remaining vague. Herein, we report the design of a molten-salt carbon nitride (MCN) featuring ionic structure represented by negatively charged organic polymeric scaffold and K+ counterions and application of this material as the photocatalyst in synthesis of pharmaceutically relevant fluorinated heterocycles under visible light under the redox neutral conditions. K+ ions serve as the sites for sorption of ethyl bromodifluoroacetate, while the electronically excited state of MCN acts as the single electron transfer agent, enabling generation of difluoroalkyl radicals from the substrate. Combination of these two features endows a material that outperforms homogeneous photocatalysts and covalent carbon nitrides. Our protocol expands the application of carbon nitrides in synthesis of organic compounds with complex structure and provides fresh perspectives on the factors contributing to the enhanced photocatalytic efficiency of poly(heptazine imides).
聚(庚嗪酰亚胺)的离子结构对光催化制氢具有重要意义。从大量报告中可以看出,这些材料在各种有机物转化中也优于共价碳氮化物。然而,其中的原因却一直模糊不清。在此,我们报告了以带负电荷的有机聚合物支架和 K+ 反离子为离子结构的熔盐氮化碳(MCN)的设计,以及在氧化还原中性条件下将该材料作为光催化剂在可见光下合成与制药相关的氟化杂环的应用。K+ 离子是二氟溴乙酸乙酯的吸附位点,而 MCN 的电子激发态则是单电子传递剂,能够从底物中生成二氟烷基自由基。这两种特性的结合使这种材料的性能优于均相光催化剂和共价碳氮化物。我们的方案拓展了碳氮化物在合成结构复杂的有机化合物中的应用,并为聚(庚嗪亚胺)光催化效率的提高提供了新的视角。
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引用次数: 0
Ru(II)-Catalyzed Deformylative C–C Activation and Carbene Insertion: Empowering Diversity-Oriented Synthesis of Unsymmetrical Biaryldiols and Heterobiaryl Amino Alcohols Ru(II)-Catalyzed Deformylative C-C Activation and Carbene Insertion:以多样性为导向合成不对称联二醇和杂二芳基氨基醇
IF 12.9 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-15 DOI: 10.1021/acscatal.4c02889
Chandan Kumar Giri, Tejender Singh, Sudeshna Mondal, Soumya Ghosh, Mahiuddin Baidya
While 1,1′-biaryl diols and amino alcohols are privileged scaffolds, their streamlined catalytic synthesis with unsymmetrical substitution patterns remains a daunting challenge. Herein, we describe a ruthenium(II)-catalyzed synthesis of unsymmetrical 1,1′-biaryl-2,2′-diols via deformylative coupling of ortho-hydroxy aromatic aldehydes with diverse cyclic diazo compounds. The protocol is operationally simple and scalable and involves intriguing C–C bond activation and carbene insertion cascade to produce a range of diversely functionalized biaryldiols in very high yields and regioselectivity. The methodology is also suitable to access heterobiaryl amino alcohols bearing indole motif, applicable in challenging 2-fold C–C activation leading to valuable tetrahydroxy bis-biaryls, and retains efficacy in the site-selective modification of pharmaceutical agents. DFT studies have also been conducted to illustrate the intricacy of this catalytic cycle.
虽然 1,1′-联二醇和氨基醇是一种特殊的支架,但它们与不对称取代模式的简化催化合成仍然是一项艰巨的挑战。在此,我们介绍了一种钌(II)催化的非对称 1,1′-联二-2,2′-二元醇的合成方法,该方法是通过正羟基芳香醛与多种环重氮化合物的变形偶联来实现的。该方案操作简单、可扩展,涉及引人入胜的 C-C 键活化和碳烯插入级联反应,能以极高的产率和区域选择性生成一系列不同官能度的双芳基二醇。该方法还适用于获得含有吲哚基团的杂芳基氨基醇,适用于具有挑战性的 2 倍 C-C 活化,从而获得有价值的四羟基双芳基,并在药物制剂的位点选择性修饰方面保持高效。我们还进行了 DFT 研究,以说明这一催化循环的复杂性。
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引用次数: 0
Epsilon-Iron Carbide for the Hydrogenation of Carbonyl Groups in Esters 用于酯中羰基氢化的碳化ε铁
IF 12.9 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-15 DOI: 10.1021/acscatal.4c02212
Huijiang Huang, Xin Shang, Xin Li, Qiao Han, Qiang Wang, Junhu Wang, Shengping Wang, Peng Jin, Yujun Zhao, Xinbin Ma
The synthesis of ethanol (EtOH) via hydrogenation of dimethyl oxalate (DMO) from syngas has gained wide attention, but its practical application is still limited by the poor selectivity on conventional Cu-based catalysts. This work developed an efficient Fe2C catalyst confined in the ordered mesoporous carbon (Fe/CMK-3) for the hydrogenation of DMO to EtOH. The formation of epsilon-carbide phase was favored by moderate carbonization process via stepwise methanol dissociation in a confined redox microenvironment. The lower energy barriers of the epsilon-carbide phase for C═O activation enhanced the intrinsic activity of Fe/CMK-3 in the deep hydrogenation of MA to EtOH, which was the rate-determining step of DMO hydrogenation. In addition, the confined effect of ordered mesoporous carbon allowed a high dispersion of the iron carbonates, which further boosted the EtOH production. On this catalyst, a high EtOH yield of 97.6%, an unprecedent space time yield of 1004 gEtOH kgcat–1 h–1, and a durability of 120 h were successfully achieved, which could provide an alternative route for the industrial production of ethanol from syngas conversion.
从合成气中通过草酸二甲酯(DMO)加氢合成乙醇(EtOH)的方法已受到广泛关注,但其实际应用仍受到传统铜基催化剂选择性差的限制。本研究开发了一种封闭在有序介孔碳(Fe/CMK-3)中的高效 Fe2C 催化剂,用于将 DMO 加氢转化为 EtOH。在封闭的氧化还原微环境中,通过逐步解离甲醇的温和碳化过程,有利于ε-碳化物相的形成。ε-碳化物相活化 C═O 的能垒较低,增强了 Fe/CMK-3 在 MA 深度氢化为 EtOH 过程中的内在活性,而这正是 DMO 氢化的决定性步骤。此外,有序介孔碳的封闭效应使碳酸铁高度分散,进一步提高了 EtOH 的产量。在这种催化剂上,成功实现了 97.6% 的高 EtOH 产率、1004 gEtOH kgcat-1 h-1 的史无前例的时空产率和 120 h 的耐久性,为合成气转化生产乙醇的工业化生产提供了另一条途径。
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引用次数: 0
Insights into Substituent Effects on the Fundamental Photocatalytic Processes of Covalent Organic Frameworks toward H2 Evolution and H2O2 Production Reactions 深入了解取代基对共价有机框架产生 H2 和 H2O2 反应的基本光催化过程的影响
IF 12.9 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-13 DOI: 10.1021/acscatal.4c02827
Ying-Ying Gu, Junxia Wang, Qingqing Tang, Hongtao Wei, Jing Ning, Xuefang Lan, Xuefeng Wang, Xuehui Li, Yonggang Jia, Shaobin Wang, Long Hao
Covalent organic frameworks (COFs) have demonstrated enormous potential in photocatalysis. To construct more efficient COF-based photocatalysts, it is essential to delve into the relationship between molecular-level structure of the COF and the fundamental photocatalytic processes. COF is built by small molecular monomers, so the classic substitution effect on small molecules should be accumulated in the COF. However, to accurately investigate the substituent effect, the other structural parameters of the COF should be kept as unchanged as possible. This work designed and constructed COFs with identical skeleton but different substituents (−H, –CH3, and –OH) at the same position, which displayed very similar crystallinity, surface area, pore size distribution, and morphology, but completely different photocatalytic H2 evolution or H2O2 production performances. Comparative analyses of the fundamental photocatalytic processes indicated that −OH-containing COF possessed broader visible light absorption, higher charge separation efficiency, and more rational surface properties for the reactions compared with –H and −Me-containing COFs, thus resulting in superior photocatalytic performances. This study reveals that a small change in the substituent will lead to big differences in the photocatalytic processes and thus the final photocatalytic performances, which have instructive significance for the structural design and performance evaluation of COF-based photocatalysts.
共价有机框架(COFs)在光催化领域展现出巨大的潜力。要构建更高效的 COF 光催化剂,就必须深入研究 COF 分子级结构与基本光催化过程之间的关系。COF 由小分子单体构建而成,因此小分子的经典取代效应应该在 COF 中积累。然而,为了准确研究取代基效应,COF 的其他结构参数应尽可能保持不变。本研究设计并构建了骨架相同但在相同位置上具有不同取代基(-H、-CH3 和 -OH)的 COF,它们的结晶度、比表面积、孔径分布和形貌非常相似,但光催化 H2 演化或 H2O2 生成的性能却完全不同。对基本光催化过程的比较分析表明,与含-H和-Me的COF相比,含-OH的COF具有更广泛的可见光吸收、更高的电荷分离效率和更合理的反应表面性质,因而具有更优越的光催化性能。该研究揭示了取代基的微小变化会导致光催化过程的巨大差异,进而影响最终的光催化性能,对 COF 基光催化剂的结构设计和性能评价具有指导意义。
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引用次数: 0
Surface Engineering on Ag-Decorated Co3O4 Electrocatalysts for Boosting Nitrate Reduction to Ammonia 促进硝酸盐还原成氨的 Ag-Decorated Co3O4 电催化剂的表面工程技术
IF 12.9 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acscatal.4c01510
Ming Zhang, Zhipeng Ma, Shujie Zhou, Chen Han, Varun Kundi, Priyank V. Kumar, Lars Thomsen, Bernt Johannessen, Lingyi Peng, Yihao Shan, Constantine Tsounis, Yuwei Yang, Jian Pan, Rose Amal
Electrochemical nitrate reduction reaction (NO3RR) offers an alternative pathway toward ambient ammonia production and nitrogen balance restoration, requiring efficient catalysts. In this study, a silver-decorated cobalt oxide (Ag–Co3O4) catalyst was shown to enhance ammonia production during NO3RR in an alkaline electrolyte. Specifically, the Ag–Co3O4 catalyst delivers an ammonia (NH3) yield rate of 52 μmol h–1 cm–2 with a Faradaic efficiency of 88% at −0.32 V versus RHE. The activity is 6 times higher than that of the conventional Co3O4 catalyst (8.8 μmol h–1 cm–2). The catalytic activity and selectivity of Ag–Co3O4 originate from the interaction between atomically dispersed Ag and Co3O4, resulting in the formation of active octahedral Co2+ species (Co2+Oh) with an unpaired eg electron, which facilitates the activation and adsorption of NO3 ion and promotes the *NO2 adsorption, along with its transformation to *NO intermediate. This leads to efficient NH4+ production, as evidenced by combined experimental and theoretical studies.
电化学硝酸盐还原反应(NO3-RR)为环境产氨和恢复氮平衡提供了另一种途径,但需要高效的催化剂。在这项研究中,银装饰氧化钴(Ag-Co3O4)催化剂在碱性电解质中的 NO3-RR 反应中提高了氨的生成。具体而言,Ag-Co3O4 催化剂在 -0.32 V 相对于 RHE 时的氨 (NH3) 产率为 52 μmol h-1 cm-2,法拉第效率为 88%。其活性是传统 Co3O4 催化剂(8.8 μmol h-1 cm-2)的 6 倍。Ag-Co3O4 的催化活性和选择性源于原子分散的 Ag 与 Co3O4 之间的相互作用,从而形成了带有一个未配对电子的活性八面体 Co2+ 物种(Co2+Oh),这有利于 NO3- 离子的活化和吸附,并促进*NO2 的吸附,同时将其转化为*NO 中间体。综合实验和理论研究证明,这将导致 NH4+ 的高效生成。
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引用次数: 0
Promoted Surface-Interface Catalysis over Mn–Cr Incorporated Cu-Based Catalysts for Efficient Hydrogen Production from Methanol Decomposition 促进锰铬结合铜基催化剂的表面-界面催化,从甲醇分解中高效制氢
IF 12.9 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acscatal.4c02918
Zhineng Tan, Guoli Fan, Lirong Zheng, Feng Li
To solve the safety problems and economic inefficiency of transporting and storing gaseous hydrogen, developing efficient catalytic decomposition of liquid organic hydrogen carriers for in situ hydrogen production is attracting more and more attention. Here, a series of Cr-doped, Mn-promoted Cu-based catalysts for methanol decomposition were fabricated from quaternary Cu–Mn–Cr–Al layered double hydroxides. It was demonstrated that Mn incorporation promoted the reduction and dispersion of copper species and regulated the electronic properties of surface metallic Cu sites, and an appropriate amount of Cr doping facilitated the generation of smaller Cu particles and reduced the surface acidity over catalysts, thereby favoring the construction of generous interfacial Cu+ sites in the form of Cu+–Ov–Mn and Cu+–O–M structures (Ov: oxygen vacancy; M = Mn or Cr). The Cu-based catalyst bearing a Cr:Mn molar ratio of 0.4 achieved a high hydrogen selectivity of 84.3% at complete methanol conversion, along with long-term stability during 80 h of reaction. Through various exhaustive characterization studies, in situ diffuse reflectance infrared Fourier transform spectra of methanol adsorption and desorption, and density functional theory calculations, it was revealed that abundant interfacial Cu+–Ov–Mn and Cu+–O–M structures and favorable Cu+–Cu0 synergistic effects in Cu-based catalysts efficiently promoted a series of dehydrogenation processes of methanol and reaction intermediates, thus boosting hydrogen production. This study provides effective methods for the construction of Cu-based catalysts by engineering surficial and interfacial sites conducive to the efficient hydrogen production through methanol decomposition.
为了解决运输和储存气态氢的安全问题和经济效益低下的问题,开发高效催化分解液态有机氢载体以就地制氢的技术越来越受到人们的关注。本文利用四元 Cu-Mn-Cr-Al 层状双氢氧化物制备了一系列铬掺杂、锰促进的 Cu 基甲醇分解催化剂。研究表明,锰的掺入促进了铜物种的还原和分散,并调节了表面金属 Cu 位点的电子特性,而适量的铬掺杂则有利于生成更小的 Cu 颗粒,并降低催化剂的表面酸度,从而有利于以 Cu+-Ov-Mn 和 Cu+-O-M 结构(Ov:氧空位;M = 锰或铬)的形式构建宽松的界面 Cu+ 位点。铬锰摩尔比为 0.4 的铜基催化剂在完全转化甲醇时的氢气选择性高达 84.3%,并且在 80 小时的反应过程中具有长期稳定性。通过各种详尽的表征研究、甲醇吸附和解吸的原位漫反射红外傅立叶变换光谱以及密度泛函理论计算,发现铜基催化剂中丰富的界面 Cu+-Ov-Mn 和 Cu+-O-M 结构以及有利的 Cu+-Cu0 协同效应能有效促进甲醇和反应中间产物的一系列脱氢过程,从而提高氢气产量。该研究通过设计有利于甲醇分解高效制氢的表面和界面位点,为构建铜基催化剂提供了有效方法。
{"title":"Promoted Surface-Interface Catalysis over Mn–Cr Incorporated Cu-Based Catalysts for Efficient Hydrogen Production from Methanol Decomposition","authors":"Zhineng Tan, Guoli Fan, Lirong Zheng, Feng Li","doi":"10.1021/acscatal.4c02918","DOIUrl":"https://doi.org/10.1021/acscatal.4c02918","url":null,"abstract":"To solve the safety problems and economic inefficiency of transporting and storing gaseous hydrogen, developing efficient catalytic decomposition of liquid organic hydrogen carriers for in situ hydrogen production is attracting more and more attention. Here, a series of Cr-doped, Mn-promoted Cu-based catalysts for methanol decomposition were fabricated from quaternary Cu–Mn–Cr–Al layered double hydroxides. It was demonstrated that Mn incorporation promoted the reduction and dispersion of copper species and regulated the electronic properties of surface metallic Cu sites, and an appropriate amount of Cr doping facilitated the generation of smaller Cu particles and reduced the surface acidity over catalysts, thereby favoring the construction of generous interfacial Cu<sup>+</sup> sites in the form of Cu<sup>+</sup>–O<sub>v</sub>–Mn and Cu<sup>+</sup>–O–M structures (O<sub>v</sub>: oxygen vacancy; M = Mn or Cr). The Cu-based catalyst bearing a Cr:Mn molar ratio of 0.4 achieved a high hydrogen selectivity of 84.3% at complete methanol conversion, along with long-term stability during 80 h of reaction. Through various exhaustive characterization studies, in situ diffuse reflectance infrared Fourier transform spectra of methanol adsorption and desorption, and density functional theory calculations, it was revealed that abundant interfacial Cu<sup>+</sup>–O<sub>v</sub>–Mn and Cu<sup>+</sup>–O–M structures and favorable Cu<sup>+</sup>–Cu<sup>0</sup> synergistic effects in Cu-based catalysts efficiently promoted a series of dehydrogenation processes of methanol and reaction intermediates, thus boosting hydrogen production. This study provides effective methods for the construction of Cu-based catalysts by engineering surficial and interfacial sites conducive to the efficient hydrogen production through methanol decomposition.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597432","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Operando Soft X-ray Absorption of LaMn1–xCoxO3 Perovskites for CO Oxidation 用于 CO 氧化的 LaMn1-xCoxO3 Perovskites 的操作性软 X 射线吸收
IF 12.9 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acscatal.4c03259
Qijun Che, Mahnaz Ghiasi, Luca Braglia, Matt L. J. Peerlings, Silvia Mauri, Piero Torelli, Petra de Jongh, Frank M. F. de Groot
We employed operando soft X-ray absorption spectroscopy (XAS) to monitor the changes in the valence states and spin properties of LaMn1–xCoxO3 catalysts subjected to a mixture of CO and O2 at ambient pressure. Guided by simulations based on charge transfer multiplet theory, we quantitatively analyze the Mn and Co 2p XAS as well as the oxygen K-edge XAS spectra during the reaction process. The Mn sites are particularly sensitive to the catalytic reaction, displaying dynamics in their oxidation state. When Co doping is introduced (x ≤ 0.5), Mn oxidizes from Mn2+ to Mn3+ and Mn4+, while Co largely maintains a valence state of Co2+. In the case of LaCoO3, we identify high-spin and low-spin Co3+ species combined with Co2+. Our investigation underscores the importance to consider the spin and valence states of catalyst materials under operando conditions.
我们采用操作软 X 射线吸收光谱 (XAS) 来监测 LaMn1-xCoxO3 催化剂在环境压力下与 CO 和 O2 混合反应时的价态和自旋特性的变化。在基于电荷转移多重理论的模拟指导下,我们定量分析了反应过程中 Mn 和 Co 2p XAS 以及氧 K 边 XAS 光谱。锰位点对催化反应特别敏感,其氧化态呈现出动态变化。当引入 Co 掺杂(x ≤ 0.5)时,锰从 Mn2+ 氧化成 Mn3+ 和 Mn4+,而 Co 则基本保持 Co2+ 的价态。在 LaCoO3 中,我们发现了与 Co2+ 结合的高自旋和低自旋 Co3+ 物种。我们的研究强调了在操作条件下考虑催化剂材料的自旋和价态的重要性。
{"title":"Operando Soft X-ray Absorption of LaMn1–xCoxO3 Perovskites for CO Oxidation","authors":"Qijun Che, Mahnaz Ghiasi, Luca Braglia, Matt L. J. Peerlings, Silvia Mauri, Piero Torelli, Petra de Jongh, Frank M. F. de Groot","doi":"10.1021/acscatal.4c03259","DOIUrl":"https://doi.org/10.1021/acscatal.4c03259","url":null,"abstract":"We employed operando soft X-ray absorption spectroscopy (XAS) to monitor the changes in the valence states and spin properties of LaMn<sub>1–<i>x</i></sub>Co<sub><i>x</i></sub>O<sub>3</sub> catalysts subjected to a mixture of CO and O<sub>2</sub> at ambient pressure. Guided by simulations based on charge transfer multiplet theory, we quantitatively analyze the Mn and Co 2p XAS as well as the oxygen K-edge XAS spectra during the reaction process. The Mn sites are particularly sensitive to the catalytic reaction, displaying dynamics in their oxidation state. When Co doping is introduced (<i>x</i> ≤ 0.5), Mn oxidizes from Mn<sup>2+</sup> to Mn<sup>3+</sup> and Mn<sup>4+</sup>, while Co largely maintains a valence state of Co<sup>2+</sup>. In the case of LaCoO<sub>3</sub>, we identify high-spin and low-spin Co<sup>3+</sup> species combined with Co<sup>2+</sup>. Our investigation underscores the importance to consider the spin and valence states of catalyst materials under operando conditions.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597435","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Decatungstate/Cobalt Dual Catalyzed Dehydrogenation of Ketones Enabled by Polarity-Matched Site-Selective Activation 通过极性匹配的位点选择性活化实现癸钨酸盐/钴双催化酮的脱氢反应
IF 12.9 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-11 DOI: 10.1021/acscatal.4c02956
Bin Sun, Jiayin Wang, Shuangshuang Zhou, Jiaxing Xu, Xiaohui Zhuang, Zehui Meng, Yifan Xu, Zhiguo Zhang, Can Jin
The direct dehydrogenation of ketones has been widely utilized in both academic and industrial settings as the most efficient means of constructing unsaturated ketones and phenols. In contrast to the induction of dehydrogenation at the α-site of carbonyl by enol activation, direct and efficient activation of the carbonyl β-C(sp3)-H bond to form unsaturated ketones remains unexplored. Herein, we report a polarity-matching-based activation strategy for the carbonyl β-C(sp3)-H bond, enabling the photoinduced intramolecular dehydrogenation of ketones without prefunctionalization via the merger of photoredox and cobalt catalysis. This photoinduced mode employs a benign and mild approach to construct unsaturated ketone and phenol skeletons via acceptorless catalytic dehydrogenation, showcasing potential applications in the field of drug synthesis.
酮的直接脱氢作为构建不饱和酮和酚的最有效方法,在学术界和工业界都得到了广泛应用。与通过烯醇活化诱导羰基 α 位点的脱氢反应不同,直接有效地活化羰基 β-C(sp3)-H 键以形成不饱和酮的方法仍有待探索。在此,我们报告了一种基于极性匹配的羰基β-C(sp3)-H 键活化策略,通过合并光氧化和钴催化,实现了酮的光诱导分子内脱氢,而无需预官能化。这种光诱导模式采用了一种良性、温和的方法,通过无受体催化脱氢来构建不饱和酮和酚骨架,在药物合成领域具有潜在的应用前景。
{"title":"Decatungstate/Cobalt Dual Catalyzed Dehydrogenation of Ketones Enabled by Polarity-Matched Site-Selective Activation","authors":"Bin Sun, Jiayin Wang, Shuangshuang Zhou, Jiaxing Xu, Xiaohui Zhuang, Zehui Meng, Yifan Xu, Zhiguo Zhang, Can Jin","doi":"10.1021/acscatal.4c02956","DOIUrl":"https://doi.org/10.1021/acscatal.4c02956","url":null,"abstract":"The direct dehydrogenation of ketones has been widely utilized in both academic and industrial settings as the most efficient means of constructing unsaturated ketones and phenols. In contrast to the induction of dehydrogenation at the α-site of carbonyl by enol activation, direct and efficient activation of the carbonyl β-C(sp<sup>3</sup>)-H bond to form unsaturated ketones remains unexplored. Herein, we report a polarity-matching-based activation strategy for the carbonyl β-C(sp<sup>3</sup>)-H bond, enabling the photoinduced intramolecular dehydrogenation of ketones without prefunctionalization via the merger of photoredox and cobalt catalysis. This photoinduced mode employs a benign and mild approach to construct unsaturated ketone and phenol skeletons via acceptorless catalytic dehydrogenation, showcasing potential applications in the field of drug synthesis.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141588838","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Elucidation of the Stereochemical Mechanism of Cystathionine γ-Lyase Reveals How Substrate Specificity Constrains Catalysis 阐明胱硫醚γ-赖氨酸酶的立体化学机制揭示底物特异性如何制约催化作用
IF 12.9 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-11 DOI: 10.1021/acscatal.4c02281
Anna Zmich, Lydia J. Perkins, Craig Bingman, Andrew R. Buller
Pyridoxal phosphate (PLP)-dependent enzymes play essential roles in metabolism and have found applications for organic synthesis and as enzyme therapeutics. The vinylglycine ketimine (VGK) subfamily hosts a growing set of enzymes that play diverse roles in primary and secondary metabolism. However, the molecular determinants of substrate specificity and the complex acid–base chemistry that enables VGK catalysis remain enigmatic. We use a recently discovered amino acid γ-lyase as a model system to probe catalysis in this enzyme family. We discovered that two stereochemically distinct proton transfer pathways occur. Combined kinetic and spectroscopic analysis revealed that progression through the catalytic cycle is correlated with the presence of an H-bond donor after Cγ of an amino acid substrate, suggesting that substrate binding is kinetically coupled to a conformational change. High-resolution X-ray crystallography shows that cystathionine-γ-lyases generate an s-trans intermediate and that this geometry is likely conserved throughout the VGK family. An H-bond acceptor in the active site templates substrate binding but does so by preorganizing substrates away from catalytically productive orientations. Mutagenesis eliminates this preorganization, such that there is a relaxation of the substrate specificity but an increase in kcat for diverse substrates. We exploit this information to perform a preparative-scale α,β,β-trideuteration of polar amino acids. Together, these data untangle a complex mode of substrate specificity and provide a foundation for the future study and applications of VGK enzymes.
依赖磷酸吡哆醛(PLP)的酶在新陈代谢中发挥着重要作用,并被应用于有机合成和酶疗法。乙烯基甘氨酸酮亚胺(VGK)亚家族拥有越来越多的酶,它们在初级和次级代谢中发挥着不同的作用。然而,底物特异性的分子决定因素以及 VGK 催化所需的复杂酸碱化学性质仍然是个谜。我们以最近发现的一种氨基酸γ-裂解酶为模型系统,探究该酶家族的催化作用。我们发现存在两种立体化学上截然不同的质子转移途径。结合动力学和光谱分析发现,催化循环的进展与氨基酸底物 Cγ 后是否存在 H 键供体相关,这表明底物结合在动力学上与构象变化相关。高分辨率 X 射线晶体学研究表明,胱硫醚-γ-裂解酶会产生一种 s-trans 中间体,而且这种几何形状在整个 VGK 家族中可能是保守的。活性位点中的一个 H 键受体为底物结合提供了模板,但这种模板是通过预组织底物使其远离催化生产方向来实现的。突变消除了这种预组织,因此底物特异性有所放松,但对不同底物的 kcat 却有所增加。我们利用这一信息对极性氨基酸进行了制备规模的α,β,β-三uteration反应。这些数据共同揭示了底物特异性的复杂模式,为 VGK 酶未来的研究和应用奠定了基础。
{"title":"Elucidation of the Stereochemical Mechanism of Cystathionine γ-Lyase Reveals How Substrate Specificity Constrains Catalysis","authors":"Anna Zmich, Lydia J. Perkins, Craig Bingman, Andrew R. Buller","doi":"10.1021/acscatal.4c02281","DOIUrl":"https://doi.org/10.1021/acscatal.4c02281","url":null,"abstract":"Pyridoxal phosphate (PLP)-dependent enzymes play essential roles in metabolism and have found applications for organic synthesis and as enzyme therapeutics. The vinylglycine ketimine (VGK) subfamily hosts a growing set of enzymes that play diverse roles in primary and secondary metabolism. However, the molecular determinants of substrate specificity and the complex acid–base chemistry that enables VGK catalysis remain enigmatic. We use a recently discovered amino acid γ-lyase as a model system to probe catalysis in this enzyme family. We discovered that two stereochemically distinct proton transfer pathways occur. Combined kinetic and spectroscopic analysis revealed that progression through the catalytic cycle is correlated with the presence of an H-bond donor after Cγ of an amino acid substrate, suggesting that substrate binding is kinetically coupled to a conformational change. High-resolution X-ray crystallography shows that cystathionine-γ-lyases generate an <i>s-trans</i> intermediate and that this geometry is likely conserved throughout the VGK family. An H-bond acceptor in the active site templates substrate binding but does so by preorganizing substrates <i>away</i> from catalytically productive orientations. Mutagenesis eliminates this preorganization, such that there is a relaxation of the substrate specificity but an increase in <i>k</i><sub>cat</sub> for diverse substrates. We exploit this information to perform a preparative-scale α,β,β-trideuteration of polar amino acids. Together, these data untangle a complex mode of substrate specificity and provide a foundation for the future study and applications of VGK enzymes.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141597437","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Anionic Olefin Metathesis Catalysts Enable Modification of Unprotected Biomolecules in Water 阴离子烯烃官能团催化剂可在水中修饰未受保护的生物分子
IF 12.9 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-11 DOI: 10.1021/acscatal.4c02811
Christian O. Blanco, Richard Ramos Castellanos, Deryn E. Fogg
Stability problems have limited the uptake of cationic olefin metathesis catalysts in chemical biology. Described herein are anionic catalysts that improve water-solubility, robustness, and compatibility with biomolecules such as DNA. A sulfonate tag is installed on the cyclic (alkyl)(amino) carbene (CAAC) ligand platform, chosen for resistance to degradation by nucleophiles, base, water, and β-elimination. Hoveyda–Grubbs catalysts bearing the sulfonated CAAC ligands deliver record productivity in metathesis of unprotected carbohydrates and nucleosides at neutral pH. Decomposed catalyst has negligible impact on metathesis selectivity, whereas N-heterocyclic carbene (NHC) catalysts degrade rapidly in water and cause extensive C=C migration.
稳定性问题限制了阳离子烯烃偏合成催化剂在化学生物学中的应用。本文介绍的阴离子催化剂可提高水溶性、稳定性以及与 DNA 等生物大分子的兼容性。环(烷基)(氨基)碳烯(CAAC)配体平台上安装了磺酸盐标签,该标签具有耐亲核物、碱、水和β-消除降解的特性。带有磺化 CAAC 配体的 Hoveyda-Grubbs 催化剂在中性 pH 下进行无保护碳水化合物和核苷的复分解反应时,具有创纪录的生产率。分解催化剂对元合成选择性的影响可以忽略不计,而 N-杂环碳烯(NHC)催化剂在水中会迅速降解,并导致大量 C=C 迁移。
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引用次数: 0
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ACS Catalysis
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