Nature Catalysis最新文献

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

IF 37.8 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":"https://doi.org/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.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"34 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","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":"","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 37.8 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":"https://doi.org/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.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"18 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","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":"","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 37.8 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":"https://doi.org/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.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"68 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","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":"","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

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Pulsed electrolysis through neutron lenses

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-02-26 DOI: 10.1038/s41929-025-01305-w

Marçal Capdevila-Cortada

引用次数: 0

Neither H2 nor O2 in hydrogenative oxidations with water

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-02-26 DOI: 10.1038/s41929-024-01287-1

Jianliang Xiao

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Under pressure

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-02-26 DOI: 10.1038/s41929-025-01303-y

Davide Esposito

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Metal vacancies in semiconductor oxides enhance hole mobility for efficient photoelectrochemical water splitting

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-02-25 DOI: 10.1038/s41929-025-01300-1

Jun Wang, Kang Liu, Wanru Liao, Yicui Kang, Hanrui Xiao, Yingkang Chen, Qiyou Wang, Tao Luo, Jiawei Chen, Hongmei Li, Ting-Shan Chan, Shanyong Chen, Evangelina Pensa, Liyuan Chai, Fangyang Liu, Liangxing Jiang, Changxu Liu, Junwei Fu, Emiliano Cortés, Min Liu

{"title":"Metal vacancies in semiconductor oxides enhance hole mobility for efficient photoelectrochemical water splitting","authors":"Jun Wang, Kang Liu, Wanru Liao, Yicui Kang, Hanrui Xiao, Yingkang Chen, Qiyou Wang, Tao Luo, Jiawei Chen, Hongmei Li, Ting-Shan Chan, Shanyong Chen, Evangelina Pensa, Liyuan Chai, Fangyang Liu, Liangxing Jiang, Changxu Liu, Junwei Fu, Emiliano Cortés, Min Liu","doi":"10.1038/s41929-025-01300-1","DOIUrl":"https://doi.org/10.1038/s41929-025-01300-1","url":null,"abstract":"Achieving efficient carrier separation in transition-metal-oxide semiconductors is crucial for their applications in optoelectronic and catalytic devices. However, the substantial disparity in mobility between holes and electrons heavily limits device performance. Here we develop a general strategy for enhancing hole mobility via reducing their effective mass through metal vacancy (VM) management. The introduction of VM yields remarkable improvements in hole mobility: 430% for WO3, 350% for TiO2 and 270% for Bi2O3. To illustrate the importance of this finding, we applied the VM concept to photoelectrochemical water splitting, where efficient carrier separation is highly coveted. In particular, VM-WO3 achieves a 4.4-fold enhancement in photo-to-current efficiency, yielding a performance of 4.8 mA cm−2 for both small- and large-scale photoelectrodes with exceptional stability for over 120 h.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"27 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486093","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

Electron and proton storage on separate Ru and BaO domains mediated by conductive low-work-function carbon to accelerate ammonia synthesis 以导电低功耗碳为媒介，在独立的 Ru 和 BaO 域上存储电子和质子，加速氨的合成

IF 37.8 1区化学

Nature Catalysis Pub Date : 2025-02-24 DOI: 10.1038/s41929-025-01302-z

Yaejun Baik, Seunghyuck Chi, Kyeongjin Lee, DongHwan Oh, Kyungho Lee, Minkee Choi

{"title":"Electron and proton storage on separate Ru and BaO domains mediated by conductive low-work-function carbon to accelerate ammonia synthesis","authors":"Yaejun Baik, Seunghyuck Chi, Kyeongjin Lee, DongHwan Oh, Kyungho Lee, Minkee Choi","doi":"10.1038/s41929-025-01302-z","DOIUrl":"https://doi.org/10.1038/s41929-025-01302-z","url":null,"abstract":"Ammonia (NH3) has gained attention as a carbon-free fuel and hydrogen carrier, making its energy-efficient production increasingly important. Here we demonstrate that Ru and BaO, connected by conductive carbon, can separately store e− and H+, like a chemical capacitor under NH3 synthesis conditions. H atoms generated on the Ru surface by H2 activation polarize into H+/e− pairs. Subsequently, H+ migrates over the carbon surfaces to neutralize basic BaO, while e− accumulates in conductive Ru/carbon. As the work function of carbon decreases, Ru gradually becomes enriched with e−, facilitating N2 activation via π-backdonation and alleviating H2 poisoning. Thus, an optimized catalyst synthesized using N-doped MWNT with the lowest work function, exhibited 7.4 times higher activity than a reference Ba–Ru/MgO catalyst. The results show that charge distribution within catalysts can be markedly altered under reaction conditions, and its rational control can enable the design of active NH3 synthesis catalysts.<figure></figure>","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"24 1","pages":""},"PeriodicalIF":37.8,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477557","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

Enantioconvergent nucleophilic substitution via synergistic phase-transfer catalysis

IF 42.8 1区化学

Nature Catalysis Pub Date : 2025-02-13 DOI: 10.1038/s41929-024-01288-0

Claire Dooley, Francesco Ibba, Bence B. Botlik, Chiara Palladino, Christopher A. Goult, Yuan Gao, Andrew Lister, Robert S. Paton, Guy C. Lloyd-Jones, Véronique Gouverneur

{"title":"Enantioconvergent nucleophilic substitution via synergistic phase-transfer catalysis","authors":"Claire Dooley, Francesco Ibba, Bence B. Botlik, Chiara Palladino, Christopher A. Goult, Yuan Gao, Andrew Lister, Robert S. Paton, Guy C. Lloyd-Jones, Véronique Gouverneur","doi":"10.1038/s41929-024-01288-0","DOIUrl":"10.1038/s41929-024-01288-0","url":null,"abstract":"Catalytic enantioconvergent nucleophilic substitution reactions of alkyl halides are highly valuable transformations, but they are notoriously difficult to implement. Specifically, nucleophilic fluorination is a renowned challenge, especially when inexpensive alkali metal fluorides are used as fluorinating reagents due to their low solubility, high hygroscopicity and Brønsted basicity. Here we report a solution by developing the concept of synergistic hydrogen bonding phase-transfer catalysis. Key to our strategy is the combination of a chiral bis-urea hydrogen bond donor (HBD) and an onium salt—two phase-transfer catalysts essential for the solubilization of potassium fluoride—as a well-characterized ternary HBD–onium fluoride complex. Mechanistic investigations indicate that this chiral ternary complex is capable of enantiodiscrimination of racemic benzylic bromides and α-bromoketones, and upon fluoride delivery affords fluorinated products in high yields and enantioselectivities. This work provides a foundation for enantioconvergent fluorination chemistry enabled through the combination of a HBD catalyst with a co-catalyst specifically curated to meet the requirement of the electrophile. The catalytic enantioconvergent nucleophilic fluorination of alkyl halides using inexpensive alkali metal fluorides is a persistent challenge. Now this has been achieved by synergistic hydrogen bonding phase-transfer catalysis combining a chiral bis-urea hydrogen bond donor and an onium salt.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 2","pages":"107-115"},"PeriodicalIF":42.8,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-024-01288-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401416","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