Nature Catalysis最新文献_第9页

Understanding two voltammetric features of water reduction and water oxidation in mild pH solutions 了解在温和pH溶液中水还原和水氧化的两个伏安特性

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-05-14 DOI: 10.1038/s41929-025-01339-0

Xin Yuan, Michael T. Bender, Myohwa Ko, Kyoung-Shin Choi

{"title":"Understanding two voltammetric features of water reduction and water oxidation in mild pH solutions","authors":"Xin Yuan, Michael T. Bender, Myohwa Ko, Kyoung-Shin Choi","doi":"10.1038/s41929-025-01339-0","DOIUrl":"10.1038/s41929-025-01339-0","url":null,"abstract":"Electrification of many processes requires the use of aqueous solutions under mild pH conditions where the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) can become competing reactions. The HER and OER under mild pH conditions show peculiar voltammetric behaviours, specifically two reductive or oxidative features, that are not observed in strongly acidic and basic solutions. These behaviours cannot be fully explained by thermodynamic considerations only and are particularly complex owing to the involvement of multiple water species (H3O+, H2O and OH–) and the conversion between these species via water autodissociation and acid–base neutralization reactions. This Analysis provides a systematic and conceptual explanation of the effect of pH, potential, stirring and buffer on the thermodynamics and kinetics of the HER and OER, providing fundamental and yet essential insights into comprehending HER and OER behaviours under mild pH conditions, and their implications for other aqueous reactions more broadly. The electrochemical behaviour observed during water reduction and oxidation is considerably more complex under mild pH than under strongly acidic or alkaline conditions. This Analysis explains the origins of this behaviour and presents its implications for aqueous electrocatalysis.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 5","pages":"495-506"},"PeriodicalIF":44.6,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143945634","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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Asymmetric Hofmann–Löffler–Freytag-type reaction via a transient carbenium ion complex merging organocatalysis and photocatalysis 不对称Hofmann-Löffler-Freytag-type反应通过瞬态碳离子络合物合并有机催化和光催化

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-04-29 DOI: 10.1038/s41929-025-01329-2

Qihang Guo, Yihui Mao, Jiren Liu, Lujing Zhu, Xin Hong, Zhan Lu

{"title":"Asymmetric Hofmann–Löffler–Freytag-type reaction via a transient carbenium ion complex merging organocatalysis and photocatalysis","authors":"Qihang Guo, Yihui Mao, Jiren Liu, Lujing Zhu, Xin Hong, Zhan Lu","doi":"10.1038/s41929-025-01329-2","DOIUrl":"10.1038/s41929-025-01329-2","url":null,"abstract":"Carbenium ions have long been an important component in organic synthesis due to their indispensable role as intermediates. However, their inherent instability and remarkable reactivity pose notable challenges in achieving enantiocontrol. The use of ubiquitous C(sp3)–H bonds as precursors to achieve highly enantioselective transformations is a very important, yet less explored approach. Here we detail an asymmetric Hofmann–Löffler–Freytag-type reaction under visible-light irradiation, resulting in chiral Evans auxiliaries with excellent enantioselectivity. This protocol is distinguished by its high efficiency (turnover frequency, 154 h−1) and broad functional group tolerance. Mechanistic investigations reveal that the readily available bisoxazoline catalysts can expedite the reaction through a hydrogen-bonding effect and regulate enantioselectivity by transient coordination with carbenium ion intermediates. Enantiocontrolled transformation of carbenium ions is challenging due to their instability and high reactivity. Now, combining a chiral organocatalyst with a photocatalyst enables enantioselective intramolecular amidation of C(sp3)–H bonds to afford chiral oxazolidine products via a transient carbenium ion complex.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 5","pages":"448-456"},"PeriodicalIF":44.6,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143884773","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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Illuminating enantioselective alkyl−alkyl coupling 照亮对映选择性烷基-烷基偶联

IF 44.6 1区化学

Nature Catalysis Pub Date : 2025-04-25 DOI: 10.1038/s41929-025-01327-4

Weisai Zu, Xinlong Luo, Haohua Huo

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Reflecting on interphases 对界面的反思

IF 44.6 1区化学

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

Benjamin Martindale

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

IF 44.6 1区化学

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

Steven McIntosh

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Bridging catalysis 桥接催化

IF 44.6 1区化学

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

Francesco Zamberlan

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Oxygen matters 氧气的重要

IF 44.6 1区化学

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

Marcal Capdevila-Cortada

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

IF 44.6 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 44.6 1区化学

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

Jan-Stefan Völler

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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 44.6 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":"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). Supported single atoms are promising catalysts for alkane dehydrogenation, although tuning their reactivity via active site modulation remains a challenge. Here the authors introduce an Ir1–Cu1 dual-atom catalyst for n-butane dehydrogenation that outperforms the corresponding Ir1 single-atom system.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 5","pages":"436-447"},"PeriodicalIF":44.6,"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