Nature Catalysis最新文献_第2页

Recirculate to accumulate

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-03-26 DOI: 10.1038/s41929-025-01321-w

Benjamin Martindale

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Chemical capacitors for ammonia synthesis

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-03-26 DOI: 10.1038/s41929-025-01311-y

A. Daisley, J. S. J. Hargreaves

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Iminium catalysis meets Diels–Alderase

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-03-26 DOI: 10.1038/s41929-025-01312-x

Naoki Kato, Shingo Nagano

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Enzymological insights from ensembles

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-03-26 DOI: 10.1038/s41929-025-01318-5

Jan-Stefan Völler

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Proximity-independent acid–base synergy in a solid ZrOxHy catalyst for amine regeneration in post-combustion CO2 capture

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-03-19 DOI: 10.1038/s41929-025-01307-8

Cheng Zhou, Mostafa Torka Beydokhti, Fatima Rammal, Parveen Kumar, Maxime Lacroix, Walter Vermeiren, Michiel Dusselier, Yuhe Liao, Bert F. Sels

{"title":"Proximity-independent acid–base synergy in a solid ZrOxHy catalyst for amine regeneration in post-combustion CO2 capture","authors":"Cheng Zhou, Mostafa Torka Beydokhti, Fatima Rammal, Parveen Kumar, Maxime Lacroix, Walter Vermeiren, Michiel Dusselier, Yuhe Liao, Bert F. Sels","doi":"10.1038/s41929-025-01307-8","DOIUrl":"10.1038/s41929-025-01307-8","url":null,"abstract":"Post-combustion CO2 capture with amines offers an almost ready-to-use capture technology to assist in the transition towards net-zero carbon emission. However, the technology suffers from a high regeneration cost due to the high process temperatures involved. Utilization of catalysts in the regeneration process was reported to be an elegant solution to lower process temperatures while maintaining high reaction kinetics. Earlier studies were performed under batch conditions and therefore lack practical validation, and a deeper mechanistic understanding of the catalysis is also missing. This study introduces a practical-to-synthesize, highly efficient, stable and recyclable ZrOxHy solid catalyst, showing high catalytic CO2 desorption rates for most common aqueous amine solutions. Kinetic and ex situ/in situ spectroscopic data reveal a proximity-independent acid–base synergistic mechanism between two catalytic cycles. The approach was validated in a fixed-bed continuous reactor, demonstrating sensible contact time shortening (up to 85%), suggesting considerable potential savings in regeneration energy, reactor construction and amine solvent cost. CO2 capture with amines is an important technology for net zero, but is hampered by the high regeneration costs of the amines. Here, the authors develop an effective ZrOxHy solid catalyst for this process and demonstrate its applicability in a pilot test in a fixed-bed continuous reactor.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 3","pages":"270-281"},"PeriodicalIF":42.8,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-025-01307-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143654006","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}

引用次数: 0

Enantioselective C–H annulations enabled by either nickel- or cobalt-electrocatalysed C–H activation for catalyst-controlled chemodivergence

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-03-07 DOI: 10.1038/s41929-025-01306-9

Tristan von Münchow, Neeraj Kumar Pandit, Suman Dana, Philipp Boos, Sven Erik Peters, Josselin Boucat, Yi-Ru Liu, Alexej Scheremetjew, Lutz Ackermann

{"title":"Enantioselective C–H annulations enabled by either nickel- or cobalt-electrocatalysed C–H activation for catalyst-controlled chemodivergence","authors":"Tristan von Münchow, Neeraj Kumar Pandit, Suman Dana, Philipp Boos, Sven Erik Peters, Josselin Boucat, Yi-Ru Liu, Alexej Scheremetjew, Lutz Ackermann","doi":"10.1038/s41929-025-01306-9","DOIUrl":"10.1038/s41929-025-01306-9","url":null,"abstract":"Enantioselective electrocatalysis shows unique potential for the sustainable assembly of enantiomerically enriched molecules. This approach allows electro-oxidative C–H activation to be performed paired to the hydrogen evolution reaction. Recent progress has featured scarce transition metals with limited availability. Here we reveal that the earth-abundant 3d transition metals nickel and cobalt exhibit distinctive performance for enantioselective electrocatalysis with chemodivergent reactivity patterns. Enantioselective desymmetrizations of strained bicyclic alkenes were achieved through C–H annulations. A data-driven optimization of chiral N,O-bidentate salicyloxazoline-type ligands was crucial for enhancing enantioselectivity in nickel electrocatalysis. Notably, in the transition state of the enantio-determining step, secondary weak attractive π–π and CH–π interactions were identified, reflecting the informed adaptations in the ligand design. Detailed mechanistic investigations by experimental and computational studies revealed for the nickel electrocatalysis a C–N bond-forming reductive elimination from nickel(III) and for the cobalt electrocatalysis a C–C bond-forming nucleophilic addition from cobalt(III) as the product-determining steps. Controlling the selectivity of electrocatalysed C–H activation with earth-abundant base metals can increase its synthetic impact. Now chemodivergence of an electrocatalysed enantioselective C–H activation is achieved by using either ligand-bound Ni or Co in the catalytic system.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 3","pages":"257-269"},"PeriodicalIF":42.8,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-025-01306-9.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569952","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}

引用次数: 0

Electrified synthesis of n-propanol using a dilute alloy catalyst

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-02-28 DOI: 10.1038/s41929-025-01301-0

Yuanjun Chen, Xinyue Wang, Xiao-Yan Li, Rui Kai Miao, Juncai Dong, Zilin Zhao, Chuhao Liu, Jianan Erick Huang, Jinhong Wu, Senlin Chu, Weiyan Ni, Zunmin Guo, Yi Xu, Pengfei Ou, Bingjun Xu, Yang Hou, David Sinton, Edward H. Sargent

{"title":"Electrified synthesis of n-propanol using a dilute alloy catalyst","authors":"Yuanjun Chen, Xinyue Wang, Xiao-Yan Li, Rui Kai Miao, Juncai Dong, Zilin Zhao, Chuhao Liu, Jianan Erick Huang, Jinhong Wu, Senlin Chu, Weiyan Ni, Zunmin Guo, Yi Xu, Pengfei Ou, Bingjun Xu, Yang Hou, David Sinton, Edward H. Sargent","doi":"10.1038/s41929-025-01301-0","DOIUrl":"10.1038/s41929-025-01301-0","url":null,"abstract":"N-propanol is an important industrial solvent but the current industrial routes for its production rely on fossil fuels and generate high carbon dioxide emissions. Replacing fossil processes with electrochemical systems powered using renewable energy offers one route to reduce the carbon intensity of n-propanol manufacture. The electrosynthesis of n-propanol via carbon monoxide electroreduction relies on the coupling of C1 and C2 intermediates, and these are preferentially stabilized on different sites. Here we pursued the synthesis of catalysts in which a high-oxygen-affinity metal (such as Sn in the best catalysts herein) is present in dilute quantities within a Cu matrix. The Sn–Cu catalyst is then formed into a catalyst/carbon/ionomer heterojunction architecture that reverses electro-osmotic drag to concentrate the n-propanol produced. We achieve n-propanol electrosynthesis from carbon monoxide with a Faradaic efficiency of 47 ± 3% and a concentration of 30 wt% at an energy efficiency of 24%. We report stable n-propanol electrosynthesis for 120 h in a membrane-electrode assembly electrolyser. Electrosynthesis of n-propanol from CO has been limited by poor selectivity and low product concentration. Here a Sn–Cu catalyst/carbon/ionomer heterojunction is prepared where the adjacent atomic active sites favour the coupling of C1 and C2 intermediates to C3 product with 47% Faradaic efficiency and the reversal of electro-osmotic drag concentrates the product to 30 wt%.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 3","pages":"239-247"},"PeriodicalIF":42.8,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-025-01301-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518298","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}

引用次数: 0

The good samarium

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-02-26 DOI: 10.1038/s41929-025-01304-x

Benjamin Martindale