Nature Catalysis最新文献_第8页

Localized thermal levering events drive spontaneous kinetic oscillations during CO oxidation on Rh/Al2O3 局部热杠杆事件驱动 Rh/Al2O3 上 CO 氧化过程中的自发动力学振荡

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-02 DOI: 10.1038/s41929-024-01181-w

Donato Decarolis, Monik Panchal, Matthew Quesne, Khaled Mohammed, Shaojun Xu, Mark Isaacs, Adam H. Clark, Luke L. Keenan, Takuo Wakisaka, Kohei Kusada, Hiroshi Kitagawa, C. Richard A. Catlow, Emma K. Gibson, Alexandre Goguet, Peter P. Wells

{"title":"Localized thermal levering events drive spontaneous kinetic oscillations during CO oxidation on Rh/Al2O3","authors":"Donato Decarolis, Monik Panchal, Matthew Quesne, Khaled Mohammed, Shaojun Xu, Mark Isaacs, Adam H. Clark, Luke L. Keenan, Takuo Wakisaka, Kohei Kusada, Hiroshi Kitagawa, C. Richard A. Catlow, Emma K. Gibson, Alexandre Goguet, Peter P. Wells","doi":"10.1038/s41929-024-01181-w","DOIUrl":"10.1038/s41929-024-01181-w","url":null,"abstract":"Unravelling kinetic oscillations, which arise spontaneously during catalysis, has been a challenge for decades but is important not only to understand these complex phenomena but also to achieve increased activity. Here we show, through temporally and spatially resolved operando analysis, that CO oxidation over Rh/Al2O3 involves a series of thermal levering events—CO oxidation, Boudouard reaction and carbon combustion—that drive oscillatory CO2 formation. This catalytic sequence relies on harnessing localized temperature episodes at the nanoparticle level as an efficient means to drive reactions in situations in which the macroscopic conditions are unfavourable for catalysis. This insight provides a new basis for coupling thermal events at the nanoscale for efficient harvesting of energy and enhanced catalyst technologies. Understanding oscillation phenomena in catalysis is a long-standing challenge. Here the authors report a temporally and spatially resolved operando analysis of CO oxidation over Rh/Al2O3, revealing the interplay of Boudouard reaction and carbon combustion in generating the oscillations.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 7","pages":"829-837"},"PeriodicalIF":42.8,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41929-024-01181-w.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141495889","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

Embedded oxide clusters stabilize sub-2 nm Pt nanoparticles for highly durable fuel cells 嵌入式氧化物团簇稳定了 2 纳米以下的铂纳米颗粒，从而实现了高度耐用的燃料电池

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-01 DOI: 10.1038/s41929-024-01180-x

Bosi Peng, Zeyan Liu, Luca Sementa, Qingying Jia, Qiang Sun, Carlo U. Segre, Ershuai Liu, Mingjie Xu, Yu-Han (Joseph) Tsai, Xingxu Yan, Zipeng Zhao, Jin Huang, Xiaoqing Pan, Xiangfeng Duan, Alessandro Fortunelli, Yu Huang

{"title":"Embedded oxide clusters stabilize sub-2 nm Pt nanoparticles for highly durable fuel cells","authors":"Bosi Peng, Zeyan Liu, Luca Sementa, Qingying Jia, Qiang Sun, Carlo U. Segre, Ershuai Liu, Mingjie Xu, Yu-Han (Joseph) Tsai, Xingxu Yan, Zipeng Zhao, Jin Huang, Xiaoqing Pan, Xiangfeng Duan, Alessandro Fortunelli, Yu Huang","doi":"10.1038/s41929-024-01180-x","DOIUrl":"10.1038/s41929-024-01180-x","url":null,"abstract":"Platinum (Pt) nanocatalysts are essential for facilitating the cathodic oxygen reduction reaction in proton exchange membrane fuel cells but suffer from a trade-off between activity and durability. Here we present the design of a fine nanocatalyst comprising Pt nanoparticles with sparsely embedded cobalt oxide clusters (CoOx@Pt). This design exploits the strong Pt/oxide interaction, which grants the catalyst its high structural and chemical durability without sacrificing activity. The CoOx@Pt nanocatalyst delivers a high initial mass activity of 1.10 A mgPt−1, a rated power density of 1.04 W cm−2 and a Pt utilization of 10.4 W mgPt−1 in a membrane electrode assembly. It exhibits a notably high durability that features a mass activity retention of 88.2%, a voltage loss of 13.3 mV at 0.8 A cm−2 and a small rated power loss of 7.5% after accelerated stress testing. This durability could offer a long projected lifetime of 15,000 hours and may greatly reduce the lifetime-adjusted cost. Pt-based catalysts are state-of-the-art cathodes in fuel cells, but they experience a trade-off between activity and durability. Now a Pt nanocatalyst with embedded cobalt oxide clusters is shown to promote stability during proton exchange membrane fuel cell operation without sacrificing activity, achieving 88.2% mass activity retention after 30,000 accelerated stress test cycles.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 7","pages":"818-828"},"PeriodicalIF":42.8,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141489488","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

Mimicking hydrogen-atom-transfer-like reactivity in copper-catalysed olefin hydrofunctionalization 在铜催化的烯烃氢功能化过程中模拟氢原子转移反应

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-07-01 DOI: 10.1038/s41929-024-01182-9

Jun-Jie Wang, He Huang, Han-Li Sun, Fan Yang, Jun Wen, Rong Zhu

{"title":"Mimicking hydrogen-atom-transfer-like reactivity in copper-catalysed olefin hydrofunctionalization","authors":"Jun-Jie Wang, He Huang, Han-Li Sun, Fan Yang, Jun Wen, Rong Zhu","doi":"10.1038/s41929-024-01182-9","DOIUrl":"10.1038/s41929-024-01182-9","url":null,"abstract":"The renaissance of catalytic metal hydride hydrogen atom transfer (MHAT) offers advanced tools for radical chemistry on simple olefins. While 3d transition metals like cobalt, iron and manganese have been extensively studied in catalytic MHAT, the potential of copper remains unexplored. This is due to the polar reactivity exhibited by classical nucleophilic Cu(I)–H. Here we report copper-catalysed MHAT-like oxidative hydrofunctionalization reactions. In contrast to conventional Cu(I)–H chemistry, the putative Cu-MHAT process produces alkyl radicals with high chemoselectivity and regioselectivity, which are subsequently captured by Cu(II) species to undergo coupling reactions with a broad scope of oxygen-, nitrogen-, halogen- and carbon-based nucleophiles. Preliminary results suggest viable extension to asymmetric catalysis and radical polymerization. This work offers a complementary oxidative MHAT platform. Cobalt, iron or manganese catalysts are the metals of choice in alkene functionalization reactions via catalytic metal hydride hydrogen atom transfer (MHAT). Now a complementary MHAT-like system based on copper is proposed to operate in a regioselective Markovnikov addition reaction of nucleophiles to olefins.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 7","pages":"838-846"},"PeriodicalIF":42.8,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141489507","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 radical strategy towards ortho-amination reactions 实现正配位反应的激进策略

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-06-26 DOI: 10.1038/s41929-024-01178-5

Quoc Hoang Pham, Rene M. Koenigs

引用次数: 0

Parallel experiments in electrochemical CO2 reduction enabled by standardized analytics 利用标准化分析技术进行二氧化碳电化学还原平行实验

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-06-26 DOI: 10.1038/s41929-024-01172-x

Alessandro Senocrate, Francesco Bernasconi, Peter Kraus, Nukorn Plainpan, Jens Trafkowski, Fabian Tolle, Thomas Weber, Ulrich Sauter, Corsin Battaglia

{"title":"Parallel experiments in electrochemical CO2 reduction enabled by standardized analytics","authors":"Alessandro Senocrate, Francesco Bernasconi, Peter Kraus, Nukorn Plainpan, Jens Trafkowski, Fabian Tolle, Thomas Weber, Ulrich Sauter, Corsin Battaglia","doi":"10.1038/s41929-024-01172-x","DOIUrl":"10.1038/s41929-024-01172-x","url":null,"abstract":"Electrochemical CO2 reduction (eCO2R) is a promising strategy to transform detrimental CO2 emissions into sustainable fuels and chemicals. Key requirements for advancing this field are the development of analytical systems and of methods that are able to accurately and reproducibly assess the performance of catalysts, electrodes and electrolysers. Here we present a comprehensive analytical system for eCO2R based on commercial hardware, which captures data for >20 gas and liquid products with <5 min time resolution by chromatography, tracks gas flow rates, monitors electrolyser temperatures and flow pressures, and records electrolyser resistances and electrode surface areas. To complement the hardware, we develop an open-source software that automatically parses, aligns in time and post-processes the heterogeneous data, yielding quantities such as Faradaic efficiencies and corrected voltages. We showcase the system’s capabilities by performing measurements and data analysis on eight parallel electrolyser cells simultaneously. Electrocatalytic CO2 reduction powered by renewable electricity is a promising technology for sustainable fuel and chemical production but accurate and reproducible analytical methods are required to advance the basic and applied science. Here a comprehensive analytical system is designed to capture numerous operating parameters in real time with automated and standardized data analysis.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 6","pages":"742-752"},"PeriodicalIF":42.8,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141461986","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 evolving atoms 氧原子进化

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-06-26 DOI: 10.1038/s41929-024-01186-5

Benjamin Martindale

引用次数: 0

The unbearable lightness of hyperbolic language 夸张语言无法承受之轻

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-06-26 DOI: 10.1038/s41929-024-01191-8

引用次数: 0

Monitoring catalytic nanosites in action 监测催化纳米材料的作用

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-06-26 DOI: 10.1038/s41929-024-01171-y

Katrin F. Domke

引用次数: 0

Absolute band-edge energies are over-emphasized in the design of photoelectrochemical materials 在设计光电化学材料时过分强调绝对带边能量

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-06-26 DOI: 10.1038/s41929-024-01161-0

Aaron J. Kaufman, Adam C. Nielander, Gerald J. Meyer, Stephen Maldonado, Shane Ardo, Shannon W. Boettcher

{"title":"Absolute band-edge energies are over-emphasized in the design of photoelectrochemical materials","authors":"Aaron J. Kaufman, Adam C. Nielander, Gerald J. Meyer, Stephen Maldonado, Shane Ardo, Shannon W. Boettcher","doi":"10.1038/s41929-024-01161-0","DOIUrl":"10.1038/s41929-024-01161-0","url":null,"abstract":"The absolute band-edge potentials of semiconductors and their positions relative to solution redox potentials are often invoked as design principles for photoelectrochemical devices and particulate photocatalysts. Here we show that these criteria are not necessary and limit the exploration of materials that may advance the fields of photoelectrochemistry, photochemistry and photocatalysis. We discuss how band-edge energies are not singular parameters and instead shift with pH, electrolyte type and surface chemistry. The free energies of electrons and holes, rather than those of solution redox couples, dictate overall reaction spontaneity and thus reactivity. Favourable charge-transfer kinetics can occur even when the relevant electrolyte redox potential(s) appear outside the bandgap, enabled by the inversion or accumulation of electronic charge at the semiconductor surface. This discussion informs design principles for photocatalytic systems engineering for both one-electron and multi-electron redox reactions (for example, H2 evolution, H2O oxidation and CO2 reduction). The absolute position of band edges is widely considered an indispensable design principle for selection of appropriate semiconductors for a given photo(electro)catalytic reaction. In this Perspective, the authors re-examine this idea from a viewpoint of semiconductor physics and make the case that alignment of band edges with chemical redox potentials is of limited importance.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"7 6","pages":"615-623"},"PeriodicalIF":42.8,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141461891","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

Gilding σ-type cyclopropenium cations 镀金σ型环丙烯阳离子

IF 42.8 1区化学

Nature Catalysis Pub Date : 2024-06-26 DOI: 10.1038/s41929-024-01183-8

Jan-Stefan Völler

引用次数: 0