Nature Catalysis最新文献_第3页

The critical role of local microenvironments 局部微环境的关键作用

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-08-22 DOI: 10.1038/s41929-025-01395-6

Hao-Fei Geng, Yi-Fan Bao, Xiang Wang, Bin Ren

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Morphological and chemical state effects in pulsed CO2 electroreduction on Cu(100) unveiled by correlated spectro-microscopy 相关光谱显微镜揭示了脉冲CO2电还原对Cu（100）的形态和化学状态影响

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-08-20 DOI: 10.1038/s41929-025-01387-6

Liviu C. Tănase, Mauricio J. Prieto, Lucas de Souza Caldas, Aarti Tiwari, Fabian Scholten, Philipp Grosse, Andrea Martini, Janis Timoshenko, Thomas Schmidt, Beatriz Roldan Cuenya

{"title":"Morphological and chemical state effects in pulsed CO2 electroreduction on Cu(100) unveiled by correlated spectro-microscopy","authors":"Liviu C. Tănase, Mauricio J. Prieto, Lucas de Souza Caldas, Aarti Tiwari, Fabian Scholten, Philipp Grosse, Andrea Martini, Janis Timoshenko, Thomas Schmidt, Beatriz Roldan Cuenya","doi":"10.1038/s41929-025-01387-6","DOIUrl":"10.1038/s41929-025-01387-6","url":null,"abstract":"Subjecting copper to short anodic pulses during the electrocatalytic reduction of carbon dioxide (CO2RR) has been shown to improve the activity and selectivity towards hydrocarbons and alcohols. Nonetheless, the nature of the active sites is still unclear. Here the evolution of the morphology, chemical state and crystal structure of Cu(100) exposed to potential pulses during the CO2RR was resolved by a combination of spectroscopy, microscopy and diffraction methods applied concurrently. Under anodic potential pulses, (n10) facets were formed. Moreover, alternating anodic to cathodic potential pulses during the CO2RR also lead to the stabilization of copper oxide species located either at the surface or directly underneath ultrathin metallic copper layers, depending on the specific pulse potential treatment applied. Both findings are key for the enhanced ethylene and ethanol production reported during pulsed CO2RR. Anodic pulsing during electrocatalytic CO2 reduction has been shown to enhance activity and selectivity towards hydrocarbons and alcohols on copper yet the nature of the active sites remains unclear. Here, correlated spectro-microscopy in a quasi in situ experimental set-up provides information on the formation of specific facets and oxidation states under reactive conditions.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 9","pages":"881-890"},"PeriodicalIF":44.6,"publicationDate":"2025-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-025-01387-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144901711","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Resolving non-covalent interactions between surface hydroxyl on Cu and interfacial water in alkaline CO electroreduction 碱性CO电还原中Cu表面羟基与界面水的非共价相互作用

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-08-19 DOI: 10.1038/s41929-025-01396-5

Qiliang Liu, Wenxing Yang

{"title":"Resolving non-covalent interactions between surface hydroxyl on Cu and interfacial water in alkaline CO electroreduction","authors":"Qiliang Liu, Wenxing Yang","doi":"10.1038/s41929-025-01396-5","DOIUrl":"10.1038/s41929-025-01396-5","url":null,"abstract":"Non-covalent interactions between the electrocatalyst surface and its electrolyte play a vital role in shaping the microenvironments of electrochemical interfaces. Yet, direct spectroscopic investigation of these interactions and their catalytic effects has remained elusive in electrocatalysis research. Here, using in situ Raman spectroscopy, we resolve a universal change of interfacial water structure at electrified Cu surfaces during alkaline CO reduction reaction. An intricate non-covalent interaction between interfacial water and surface hydroxyl (OHad) was recognized through a proposed OHad···M+(H2O)n complex, with M+ representing electrolyte cations. On exposure to catalytic potentials, these non-covalent complexes evolve into local OH−···M+(H2O)n species residing within the electrical double layer and favour CO reduction reaction into acetate over other C2 products. These results demonstrate the crucial roles of non-covalent interactions in determining the activity of surface reactions, whose existence and rational design may offer opportunities for future fine control of electrocatalysis processes. Understanding the interplay between the catalyst surface and its microenvironment is important for the development of electrocatalysis. Here, in situ Raman spectroscopy is used to resolve the interactions between copper, surface-adsorbed hydroxyl, electrolyte cations and interfacial water during electrocatalytic CO reduction.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 8","pages":"843-852"},"PeriodicalIF":44.6,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145123703","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}

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Electrosynthesis of ethylene glycol from ethylene coupled with CO2 capture 乙烯电合成乙二醇与CO2捕集

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-08-18 DOI: 10.1038/s41929-025-01392-9

Rong Xia, Yiqing Chen, Yuxin Chang, Heejong Shin, Huajie Ze, Hengzhou Liu, Pengfei Ou, Roham Dorakhan, Sungjin Park, Panos Papangelakis, Zunmin Guo, Eduardo G. Machado, Marcio V. Reboucas, Mohsen Nikkhoo, Ricardo G. A. Duarte, Daojin Zhou, Yuan Liu, Weiyan Ni, Cong Tian, Yuanjun Chen, Christine Yu, Omar K. Farha, Ke Xie, Edward H. Sargent

{"title":"Electrosynthesis of ethylene glycol from ethylene coupled with CO2 capture","authors":"Rong Xia, Yiqing Chen, Yuxin Chang, Heejong Shin, Huajie Ze, Hengzhou Liu, Pengfei Ou, Roham Dorakhan, Sungjin Park, Panos Papangelakis, Zunmin Guo, Eduardo G. Machado, Marcio V. Reboucas, Mohsen Nikkhoo, Ricardo G. A. Duarte, Daojin Zhou, Yuan Liu, Weiyan Ni, Cong Tian, Yuanjun Chen, Christine Yu, Omar K. Farha, Ke Xie, Edward H. Sargent","doi":"10.1038/s41929-025-01392-9","DOIUrl":"10.1038/s41929-025-01392-9","url":null,"abstract":"Current ethylene glycol (EG) production generates 46 million metric tons of CO2 equiv. emission annually. While electrified synthesis could decarbonize this process, existing ethylene oxidation systems suffer from high energy consumption resulting from excessive voltages. Here we identify, with the aid of in situ photoluminescence spectroscopy, an increased pH at the membrane–anode interface within a membrane–electrode assembly electrolyser and find that it arises due to hydroxide counter-migration across the membrane. To address this challenge, we integrate cathodic electrochemical carbon capture to reduce hydroxide flux and develop RuSnOx catalysts that favour *Cl over *OH adsorption, facilitating chloride-mediated ethylene oxidation. The system achieves 94% Faradaic efficiency for ethylene-to-EG conversion and 91% CO2 capture efficiency from a 10% CO2 stream, sequestering 0.60 tonnes CO2 per tonne of EG produced from ethylene. This approach results in an estimated carbon intensity of 0.133 tonnes CO2 equiv. per tonne EG, compared with the global average of 1.2 tonnes CO2 equiv. per tonne EG. Current industrial methods of ethylene glycol production generate substantial CO2 emissions. Here electrocatalytic ethylene-to-ethylene glycol conversion is coupled to electrochemical CO2 capture, decreasing carbon intensity by an order of magnitude.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 8","pages":"833-842"},"PeriodicalIF":44.6,"publicationDate":"2025-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145123640","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

Tailoring the active sites in Cu-SSZ-13 as a catalyst for the selective catalytic reduction of NH3 to minimize HCHO and HCN emissions 定制Cu-SSZ-13中的活性位点，作为选择性催化还原NH3的催化剂，以减少HCHO和HCN的排放

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-08-18 DOI: 10.1038/s41929-025-01389-4

Simon Barth, Deniz Zengel, Tiago J. Goncalves, Philipp N. Plessow, Felix Studt, Jan-Dierk Grunwaldt, Maria Casapu

{"title":"Tailoring the active sites in Cu-SSZ-13 as a catalyst for the selective catalytic reduction of NH3 to minimize HCHO and HCN emissions","authors":"Simon Barth, Deniz Zengel, Tiago J. Goncalves, Philipp N. Plessow, Felix Studt, Jan-Dierk Grunwaldt, Maria Casapu","doi":"10.1038/s41929-025-01389-4","DOIUrl":"10.1038/s41929-025-01389-4","url":null,"abstract":"Synthetic fuels are promising candidates for achieving carbon neutrality and lowering soot formation. However, their combustion leads to notable amounts of formaldehyde and other oxygenates. These emissions further affect the selective catalytic reduction (SCR) of NOx and cause secondary HCN emissions due to their reaction with NH3. This study focuses on elucidating the structural features of Cu-SSZ-13—a widely applied NH3-SCR catalyst—that lead to high formaldehyde conversion while minimizing HCN emissions. Complementary in situ/operando characterization techniques supported by density functional theory calculations are systematically applied for a series of Cu-SSZ-13 catalysts with different Cu loadings and Si/Al ratios. The obtained results demonstrate that the decrease in SCR activity due to the presence of HCHO correlates with the formation of mobile Cu–CN species, whereas low HCN emissions at >350 °C are associated with the presence of ZCuOH species in the catalyst structure. Alternative fuels such as biomethane are attractive, although their combustion generates pollutants such as formaldehyde that impair conventional abatement technologies. This study elucidates the impact of HCHO during the selective catalytic reduction of NOx over Cu-SSZ-13 catalysts, revealing important structural and mechanistic aspects.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 8","pages":"804-821"},"PeriodicalIF":44.6,"publicationDate":"2025-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-025-01389-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145123704","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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An NAD⁺ analogue enables assembly of structurally diverse artificial photoenzymes for enantiodivergent [2 + 2] cycloadditions NAD +模拟物可以组装结构多样的人工光酶，用于对映异构[2 + 2]环加成

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-08-12 DOI: 10.1038/s41929-025-01390-x

Ping Du, Jinsi Li, Tai-Ping Zhou, Jun Wang, Wenhao Hu, Haoyu Li, Binju Wang, Hui-Jie Pan

{"title":"An NAD⁺ analogue enables assembly of structurally diverse artificial photoenzymes for enantiodivergent [2 + 2] cycloadditions","authors":"Ping Du, Jinsi Li, Tai-Ping Zhou, Jun Wang, Wenhao Hu, Haoyu Li, Binju Wang, Hui-Jie Pan","doi":"10.1038/s41929-025-01390-x","DOIUrl":"10.1038/s41929-025-01390-x","url":null,"abstract":"Although artificial enzymes have significantly expanded the scope of enzyme-catalysed transformations, their construction typically relies on the irreversible incorporation of non-natural active sites. Inspired by natural cofactors, here we show a reversible binding strategy for artificial enzyme design using benzophenone adenine dinucleotide (BpAD), a photoactive NAD⁺ analogue that can integrate seamlessly into a broad range of NAD⁺-dependent protein scaffolds. The resulting artificial photoenzymes catalyse both inter- and intramolecular [2 + 2] cycloaddition reactions with excellent enantioselectivity, broad substrate compatibility and notable enantiodivergence. Computational studies confirm the precise binding mode of BpAD and reveal a key exo-attack pathway in the stepwise C–C bond formation mechanism. Notably, BpAD-catalysed reactions are highly orthogonal to those mediated by NAD⁺, allowing simultaneous use without interference. This work introduces a versatile and generalizable approach to artificial enzyme development, leveraging the inherent diversity of NAD⁺-dependent proteins for tailored catalytic applications. Expanding the methods for constructing artificial enzymes is of high interest. Now a photoactive cofactor is designed that mimics NAD+, allowing its insertion into a range of NAD+-binding protein scaffolds to catalyse inter- and intramolecular [2 + 2] cycloaddition reactions.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 8","pages":"822-832"},"PeriodicalIF":44.6,"publicationDate":"2025-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144819690","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}

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Metalloradical-driven enzymatic CO2 reduction by a dynamic Ni–Fe cluster 金属自由基驱动的动态Ni-Fe簇酶促CO2还原

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-08-01 DOI: 10.1038/s41929-025-01388-5

Yudhajeet Basak, Christian Lorent, Jae-Hun Jeoung, Ingo Zebger, Holger Dobbek

{"title":"Metalloradical-driven enzymatic CO2 reduction by a dynamic Ni–Fe cluster","authors":"Yudhajeet Basak, Christian Lorent, Jae-Hun Jeoung, Ingo Zebger, Holger Dobbek","doi":"10.1038/s41929-025-01388-5","DOIUrl":"10.1038/s41929-025-01388-5","url":null,"abstract":"Carbon monoxide dehydrogenases (CODHs) selectively catalyse the reversible reduction of CO2 to CO and water. The catalytic centre of CODHs contains a unique [NiFe4(OH)(µ3-S)4] cluster whose role in activating and converting CO2 is poorly understood. Here we reveal the structures of all catalytically relevant oxidation states with and without substrates and products bound. We show that the Ni–Fe cluster combines a rigid Fe–S core with a dynamic Ni(I/II)–Fe(II) dyad. The redox-active element is the Ni ion, cycling between square-planar Ni(II) and T-shaped Ni(I) states with metalloradical character, the latter serving as the nucleophile for CO2 activation. The Fe(II) ion switches between two positions, the one preceding CO2 activation is close to Ni(I) with a potential Ni(I)–Fe(II) interaction and the other binds the substrates CO2 and water. We demonstrate how the Ni–Fe cluster creates an efficient CO2 reduction catalyst and provides a blueprint for the design of novel catalysts based on abundant transition metals. The mechanism by which the [NiFe4S4] cluster of carbon monoxide dehydrogenases (CODHs) catalyses CO2 reduction is poorly understood. Now the structures of all catalytically relevant states of a CODH are solved, revealing the dynamics of the cluster during turnover and the role of Ni in CO2 activation.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 8","pages":"794-803"},"PeriodicalIF":44.6,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-025-01388-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144756649","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Behind the curtain 幕后

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-24 DOI: 10.1038/s41929-025-01394-7

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Tethered oxygen turns methane into methanol 束缚氧将甲烷转化为甲醇

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-07-24 DOI: 10.1038/s41929-025-01381-y

Aditya Prajapati

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A copper enzyme for Lewis acid biocatalysis 用于路易斯酸生物催化的铜酶

IF 44.6 1区化学