Nature Catalysis最新文献_第8页

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-25 DOI: 10.1038/s41929-025-01332-7

Benjamin Martindale

{"title":"Reflecting on interphases","authors":"Benjamin Martindale","doi":"10.1038/s41929-025-01332-7","DOIUrl":"https://doi.org/10.1038/s41929-025-01332-7","url":null,"abstract":"The use of neutron reflectometry is crucial since the light elements lithium and hydrogen are practically invisible to more commonly used X-ray techniques. A number of detailed insights about the exchange of species between the SEI and electrolyte are revealed in a series of experiments. First, the identity of the Li salt has a profound impact of the SEI formation with a more well-defined layer observed in LiBF4 than in LiClO4. Specifically, the structure consists of a thick, diffuse outer layer with a thin compact inner layer at low current density and low cycling that merge into a single layer after increased current cycling. Then, the use of isotopically (deuterium) labelled solvent (THF) and proton donor (ethanol) reveals that the proton donor impacts the inner layer while the solvent controls the outer. In the absence of any proton donor, dendritic growth of Li occurred at the expense of Li3N and LiH. Finally, neutron absorption also allowed the observation of boron incorporation into the SEI in the case of LiBF4.These insights contribute towards explaining the previous observations that the selectivity and stability of Li-mediated N2RR are improved by the use of fluorinated electrolytes. More broadly, it exemplifies the need for deepened understanding of SEI evolution and the power of SEI engineering through electrolyte additives.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"6 1","pages":"284-284"},"PeriodicalIF":37.8,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875966","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

Revealing hidden nanoscale electrocatalysis 揭示隐藏的纳米级电催化

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-25 DOI: 10.1038/s41929-025-01326-5

Steven McIntosh

引用次数: 0

Bridging catalysis 桥接催化

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-25 DOI: 10.1038/s41929-025-01338-1

Francesco Zamberlan

{"title":"Bridging catalysis","authors":"Francesco Zamberlan","doi":"10.1038/s41929-025-01338-1","DOIUrl":"https://doi.org/10.1038/s41929-025-01338-1","url":null,"abstract":"The team first analysed a model liquid phase system for this reaction, composed of acetic acetic-potassium acetate solution with Pd/C, and found that Pd(0) is subjected to corrosion by molecular oxygen. This allows the solubilization of the metal as Pd(II) acetate, with the Pd(II) species then reacting with ethylene to yield VA and metallic Pd(0) as precipitate. They also notice that Pd/C promotes the reaction better than bulk Pd. They also found this is valid also for the electrochemical and thermochemical processes of model VA production in the absence of O2: in all cases, the Pd(II) species is solvated from the solid support upon a corrosion event, but the Pd reoxidation is a heterogeneous process upon which Pd(0) particles are dispersed on the support, as confirmed by TEM measurements, ready for the subsequent corrosion step in the next catalytic cycle. Finally, the same electrochemical behaviour is also observed in a model system of the process’ industrial conditions.Surendranath and co-workers’ investigations point to a dynamic interplay between heterogeneous Pd(0) and homogenous Pd(II) species, with a catalytic system that challenges the current catalytic phase separation paradigm, highlighting the intricate relationship between homogeneous and heterogeneous modes of reaction.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"16 1","pages":"286-286"},"PeriodicalIF":37.8,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875964","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

Oxygen matters 氧气的重要

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-25 DOI: 10.1038/s41929-025-01333-6

Marcal Capdevila-Cortada

{"title":"Oxygen matters","authors":"Marcal Capdevila-Cortada","doi":"10.1038/s41929-025-01333-6","DOIUrl":"https://doi.org/10.1038/s41929-025-01333-6","url":null,"abstract":"Now, Chris-Kriton Skylaris and colleagues, in a collaboration between the University of Southampton and Johnson Matthey, study the impact of oxidation effects on Pt nanoparticles (NPs) to the ORR by computational means. To that end, they perform grand canonical minimization Monte Carlo simulations using the recently developed MACE-MP-0 machine learning interatomic potentials, which allows the treatment of the large Pt NPs (Pt353 plus oxygen atoms, up to a total of 896 atoms) with nearly density functional theory accuracy at a fixed chemical potential.The researchers obtain the Pt NP’s most stable oxygen content at each given voltage and derive a volcano plot that associates a rate-determining step and onset overpotential to each oxygen content. These results are thus a consequence of both thermodynamic considerations and site-blocking effects due to the presence of oxide species. The latter effects are studied in detail via a deletion energy analysis, which reveals the heterogeneity of surface oxide species. In addition, a shift in the d-band centre is found with the oxygen content highlighting two distinct regimes, which is related to the formation of an oxide phase at higher oxygen content. Finally, a kinetic model that includes the above considerations is derived.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"31 1","pages":"285-285"},"PeriodicalIF":37.8,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143875965","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

Regioselective silyl installation for arene diversification 芳烃多样化的区域选择性硅基装置

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-25 DOI: 10.1038/s41929-025-01314-9

引用次数: 0

Rings for interfacial catalysis 用于界面催化的环

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-25 DOI: 10.1038/s41929-025-01331-8

Jan-Stefan Völler

{"title":"Rings for interfacial catalysis","authors":"Jan-Stefan Völler","doi":"10.1038/s41929-025-01331-8","DOIUrl":"https://doi.org/10.1038/s41929-025-01331-8","url":null,"abstract":"Now, Yilin Wang, Bing Liu and co-workers developed a type of emulsion, where the droplets are covered by a densely packed colloidal SiO2 ring monolayer (pictured). Besides enhancing the stability, the SiO2 rings are hollow so that the liquid–liquid interface of the droplets remains largely accessible, enabling efficient diffusion and operation of the catalysts. First, fluorescent rhodamine B was used to visualize the enhanced diffusion through the interface of water-in-cyclohexane ring-stabilized Pickering emulsion (RPE) compared to conventional nanosphere-stabilized PEs (SPE). Having this beneficial feature confirmed the researchers set out to use it for enhancing catalytic reactions. Lipase was added to the water phase of toluene-in water RPE. The enzyme accumulated at the interface and catalysed the hydrolysis of oil-soluble 4-nitrophenyl palmitate to water-soluble p-nitrophenol, which quickly diffused to the water-phase. This set-up outperformed other conventional emulsion systems in terms of reaction conversion and specific activity of lipase. Then, the authors applied the RPE for the haemoglobin-catalysed oxidation of pyrogallol that not only takes place at the interface but also in in the water phase. RPE again showed significantly faster conversion compared to other PE systems, which was attributed to the faster diffusion of the products from the aqueous phase to the organic phase. Finally, a Pd NP-loaded RPE was generated, and it was shown that it performed better than the corresponding SPE system for the oxidation of benzyl alcohol in batch and continuous flow interfacial catalysis due to higher accumulation of Pd NPs at the interface.Taken together, the researchers have successfully addressed the problem of low interface accessibility of particle-stabilized Pickering emulsions and have convincingly demonstrated the advantages of the developed ring-stabilized system for catalytic applications.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 1","pages":"283-283"},"PeriodicalIF":37.8,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876079","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

A highly efficient and regenerable Ir1–Cu1 dual-atom catalyst for low-temperature alkane dehydrogenation 一种高效可再生的Ir1-Cu1双原子烷烃低温脱氢催化剂

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-18 DOI: 10.1038/s41929-025-01328-3

Xiaowen Chen, Maolin Wang, Yurong He, Mi Peng, Jiangyong Diao, Dequan Xiao, Ning Wang, Xiangbin Cai, Hongyang Liu, Ding Ma

{"title":"A highly efficient and regenerable Ir1–Cu1 dual-atom catalyst for low-temperature alkane dehydrogenation","authors":"Xiaowen Chen, Maolin Wang, Yurong He, Mi Peng, Jiangyong Diao, Dequan Xiao, Ning Wang, Xiangbin Cai, Hongyang Liu, Ding Ma","doi":"10.1038/s41929-025-01328-3","DOIUrl":"https://doi.org/10.1038/s41929-025-01328-3","url":null,"abstract":"Alkane dehydrogenation as a direct route to produce olefins receives widespread attention from industry and academia. However, high temperatures (>550 °C) are often needed to break C–H bonds, leading to deleterious side reactions in the alkane dehydrogenation process. Here we reduce the reaction temperature of n-butane dehydrogenation by fabricating a robust and regenerable Ir1–Cu1 dual-atom catalyst. The so-prepared system shows a turnover frequency of 2.45 s−1 at 450 °C, which is 6.3 times higher than the single-atom Ir1/ND@G catalyst, while, at he same time, achieving a high C4 olefin selectivity of 98%. Importantly, key for the success of the Ir1–Cu1 dual-atom catalyst are the sterically favourable geometric configuration and the modulated electronic property, which can lower the reaction barrier for C–H activation, shift the rate-determining step and facilitate the desorption of the product. Thus, a remarkable activity can be achieved for n-butane dehydrogenation at relatively low temperature (≤450 °C).<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"263 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846671","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

Retrobiosynthesis of unnatural lactams via reprogrammed polyketide synthase 通过重编程聚酮合成酶逆转录合成非天然内酰胺

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-18 DOI: 10.1038/s41929-025-01325-6

Namil Lee, Matthias Schmidt, Chenyi Li, Connor J. Filbin, Sarah Klass, Allison Yaguchi, Anna Lisa Fear, Tyler W. H. Backman, Brooks A. Abel, Young-Mo Kim, Woojoo E. Kim, Christopher W. Johnson, Yan Chen, Jennifer W. Gin, Christopher J. Petzold, Edward E. K. Baidoo, Yuqian Gao, Meagan C. Burnet, Gyorgy Babnigg, Philip D. Laible, Christine A. Singer, William E. Michener, Davinia Salvachúa, Hector Garcia Martin, Robert W. Haushalter, Jay D. Keasling

{"title":"Retrobiosynthesis of unnatural lactams via reprogrammed polyketide synthase","authors":"Namil Lee, Matthias Schmidt, Chenyi Li, Connor J. Filbin, Sarah Klass, Allison Yaguchi, Anna Lisa Fear, Tyler W. H. Backman, Brooks A. Abel, Young-Mo Kim, Woojoo E. Kim, Christopher W. Johnson, Yan Chen, Jennifer W. Gin, Christopher J. Petzold, Edward E. K. Baidoo, Yuqian Gao, Meagan C. Burnet, Gyorgy Babnigg, Philip D. Laible, Christine A. Singer, William E. Michener, Davinia Salvachúa, Hector Garcia Martin, Robert W. Haushalter, Jay D. Keasling","doi":"10.1038/s41929-025-01325-6","DOIUrl":"https://doi.org/10.1038/s41929-025-01325-6","url":null,"abstract":"Engineered polyketide synthases (PKSs) have great potential as biocatalysts. These unnatural enzymes are capable of synthesizing molecules that are either not amenable to biosynthesis or are extremely challenging to access chemically. PKSs can thus be a powerful platform to expand the chemical landscape beyond the limits of conventional metabolic engineering. Here we employ a retrobiosynthesis approach to design and construct PKSs to produce δ-valerolactam (VL) and three enantiopure α-substituted VL analogues that have no known biosynthetic route. We introduce the engineered PKSs and pathways for various malonyl-CoA derivatives into Pseudomonas putida and use proteomics, metabolomics and culture condition optimization to improve the production of our target compounds. These α-substituted VLs are polymerized into polyamides (nylon-5) or converted into their N-acryloyl derivatives. RAFT polymerization produces bio-derived polymers with potential biomedical applications. Overall, this interdisciplinary effort highlights the versatility and effectiveness of a PKS-based retrobiosynthesis approach in exploring and developing innovative biomaterials.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"88 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143846669","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

Cobaltosilicate zeolite beyond platinum catalysts for propane dehydrogenation 钴硅酸盐沸石超越铂催化剂用于丙烷脱氢

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-11 DOI: 10.1038/s41929-025-01320-x

Hang Zhou, Huan Li, Liang Wang, Shengqi Chu, Lujie Liu, Lu Liu, Jizhen Qi, Zhouhong Ren, Anyu Cai, Yu Hui, Yucai Qin, Lijuan Song, Xuedi Qin, Jiaqi Shi, Jue Hou, Yongqi Ding, Jiabi Ma, Shaodan Xu, Xin Tao, Lina Li, Qi Yang, Bingwen Hu, Xi Liu, Liwei Chen, Jianping Xiao, Feng-Shou Xiao

引用次数: 0

Identifying high-spin hydroxyl-coordinated Fe3+N4 as the active centre for acidic oxygen reduction using molecular model catalysts 用分子模型催化剂鉴定高自旋羟基配位Fe3+N4为酸性氧还原活性中心

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-04-07 DOI: 10.1038/s41929-025-01324-7

Kuang-Min Zhao, Dao-Xiong Wu, Wen-Kun Wu, Jia-Bao Nie, Fu-Shan Geng, Guang Li, Hai-Yan Shi, Sheng-Chao Huang, Huan Huang, Jing Zhang, Zhi-You Zhou, Yu-Cheng Wang, Shi-Gang Sun

{"title":"Identifying high-spin hydroxyl-coordinated Fe3+N4 as the active centre for acidic oxygen reduction using molecular model catalysts","authors":"Kuang-Min Zhao, Dao-Xiong Wu, Wen-Kun Wu, Jia-Bao Nie, Fu-Shan Geng, Guang Li, Hai-Yan Shi, Sheng-Chao Huang, Huan Huang, Jing Zhang, Zhi-You Zhou, Yu-Cheng Wang, Shi-Gang Sun","doi":"10.1038/s41929-025-01324-7","DOIUrl":"https://doi.org/10.1038/s41929-025-01324-7","url":null,"abstract":"Fe–N–C catalysts are the most promising alternative to Pt for the acidic oxygen reduction reaction (ORR), yet the electronic structure of their active centres remains elusive. Here we synthesize and characterize a conjugate-bridged iron phthalocyanine (FePc) dimer model catalyst with identical Fe sites and catalytic activity comparable to actual catalysts. A high-spin trivalent FeN4 with an axial hydroxyl ligand, denoted as OH–Fe3+N4 (S = 5/2), is identified as the active state. By contrast, monomer and non-conjugated dimer manifest the OH–Fe3+N4 (S = 3/2) state with an excessive adsorption energy of ORR intermediates. Polymerized FePc is composed of 35% of the S = 5/2 state and 65% of the Fe2+N4 (S = 0 or 1) state, showing a general weaker adsorption energy. Both overly strong and weak adsorption energy hinder the ORR. Theoretical calculations indicate that π–d interaction between Fe and the conjugated carbon plane dictates the spin state. This study will help to precisely design Fe-based ORR catalysts.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"59 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143790086","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