Nature Catalysis最新文献_第10页

Square-pyramidal subsurface oxygen [Ag4OAg] drives selective ethene epoxidation on silver 方阵亚表面氧 [Ag4OAg] 在银上驱动选择性乙烯环氧化作用

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-03-25 DOI: 10.1038/s41929-024-01135-2

Dongxiao Chen, Lin Chen, Qian-Cheng Zhao, Zheng-Xin Yang, Cheng Shang, Zhi-Pan Liu

{"title":"Square-pyramidal subsurface oxygen [Ag4OAg] drives selective ethene epoxidation on silver","authors":"Dongxiao Chen, Lin Chen, Qian-Cheng Zhao, Zheng-Xin Yang, Cheng Shang, Zhi-Pan Liu","doi":"10.1038/s41929-024-01135-2","DOIUrl":"10.1038/s41929-024-01135-2","url":null,"abstract":"Ag-catalysed ethene epoxidation is the only viable route for making ethene oxide (EO) in industry, but the active site remains elusive due to the lack of tools to probe this reaction under high temperature and high-pressure conditions. Here, aided by advanced machine-learning grand canonical global structure exploration and in situ experiments, we identify a unique surface oxide phase, namely O5 phase, grown on Ag(100) under industrial catalytic conditions. This phase features square-pyramidal subsurface O and strongly adsorbed ethene, which can selectively convert ethene to EO. The other Ag surface facets, although also reconstructing to surface oxide phases, only contain surface O and produce CO2. The complex in situ surface phases with distinct selectivity contribute to an overall medium (50%) selectivity of Ag catalyst to EO. Our further catalysis experiments with in situ infra-red spectroscopy confirm the theory-predicted infra-red-active C=C vibration of adsorbed ethene on O5 phase and the microkinetics simulation results. Ethylene oxide is a key platform chemical that is produced industrially from the epoxidation of ethylene on silver catalysts, but the precise mechanism remains elusive. Now, in a joint computational–experimental effort, a phase of the silver catalyst grown on (100) facets that contains square-pyramidal subsurface oxygens and is stabilized by strongly adsorbed ethylene is identified as the active phase, and the mechanism is revealed.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140291527","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

Nanometre-resolved observation of electrochemical microenvironment formation at the nanoparticle–ligand interface 纳米分辨观测纳米粒子配体界面的电化学微环境形成

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-03-25 DOI: 10.1038/s41929-024-01119-2

Yu Shan, Xiao Zhao, Maria Fonseca Guzman, Asmita Jana, Shouping Chen, Sunmoon Yu, Ka Chon Ng, Inwhan Roh, Hao Chen, Virginia Altoe, Stephanie N. Gilbert Corder, Hans A. Bechtel, Jin Qian, Miquel B. Salmeron, Peidong Yang

{"title":"Nanometre-resolved observation of electrochemical microenvironment formation at the nanoparticle–ligand interface","authors":"Yu Shan, Xiao Zhao, Maria Fonseca Guzman, Asmita Jana, Shouping Chen, Sunmoon Yu, Ka Chon Ng, Inwhan Roh, Hao Chen, Virginia Altoe, Stephanie N. Gilbert Corder, Hans A. Bechtel, Jin Qian, Miquel B. Salmeron, Peidong Yang","doi":"10.1038/s41929-024-01119-2","DOIUrl":"10.1038/s41929-024-01119-2","url":null,"abstract":"The dynamic response of surface ligands on nanoparticles (NPs) to external stimuli critically determines the functionality of NP–ligand systems. For example, in electrocatalysis the collective dissociation of ligands on NP surfaces can lead to the creation of an NP/ordered-ligand interlayer, a microenvironment that is highly active and selective for CO2-to-CO conversion. However, the lack of in situ characterization techniques with high spatial resolution hampers a comprehensive molecular-level understanding of the mechanism of interlayer formation. Here we utilize in situ infrared nanospectroscopy and surface-enhanced Raman spectroscopy, unveiling an electrochemical bias-induced consecutive bond cleavage mechanism of surface ligands leading to formation of the NP/ordered-ligand interlayer. This real-time molecular insight could influence the design of confined localized fields in multiple catalytic systems. Moreover, the demonstrated capability of capturing nanometre-resolved, dynamic molecular-scale events holds promise for the advancement of using controlled local molecular behaviour to achieve desired functionalities across multiple research domains in nanoscience. Nanoparticles are often stabilized by capping ligands but the specific role of such ligands during catalytic processes is often ignored. Now, in situ techniques including spatially resolved infrared nanospectroscopy reveal the ligand-assisted formation of a catalytic microenvironment on the surface of silver nanoparticles with nanoscale precision during CO2 electroreduction.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140209849","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

Lithium-mediated nitrogen reduction to ammonia via the catalytic solid–electrolyte interphase 锂介导的氮通过催化固体电解质间相还原成氨

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-03-11 DOI: 10.1038/s41929-024-01115-6

Wesley Chang, Anukta Jain, Fateme Rezaie, Karthish Manthiram

{"title":"Lithium-mediated nitrogen reduction to ammonia via the catalytic solid–electrolyte interphase","authors":"Wesley Chang, Anukta Jain, Fateme Rezaie, Karthish Manthiram","doi":"10.1038/s41929-024-01115-6","DOIUrl":"10.1038/s41929-024-01115-6","url":null,"abstract":"The lithium-mediated nitrogen reduction reaction (LiNRR) produces ammonia in ambient conditions. This electrochemical pathway is dependent on a catalytic solid–electrolyte interphase—a nanoscale passivation layer formed from reductive electrolyte decomposition on the surface of lithium metal. The catalytic solid–electrolyte interphase is a unique nanostructured environment that exists on reactive metal surfaces and intimately influences product selectivity. Here we explore recent progress made in the field of lithium-mediated nitrogen reduction to ammonia, especially in light of growing knowledge about the nature of the catalytic solid–electrolyte interphase. We systematically analyse the observed chemical species and reactions that occur within the solid–electrolyte interphase. We also summarize key developments in kinetic and transport models, as well as highlight the cathodic and complementary anodic reactions. Trends in ammonia selectivities and rates with varying electrolyte compositions, cell designs and operating conditions are extracted and used to articulate a path forward for continued development of lithium-mediated nitrogen reduction to ammonia. The electrochemical synthesis of ammonia via the lithium-mediated reduction of N2 holds great promise to replace the carbon- and energy-intensive Haber–Bosch process. This Review discusses this approach and examines the critical role of the catalytic solid–electrolyte interphase formed on the electrode.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140114712","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

Split cross-coupling via Rh-catalysed activation of unstrained aryl–aryl bonds 通过 Rh 催化活化未受约束的芳基芳烷基键进行拆分交叉耦合

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-03-11 DOI: 10.1038/s41929-024-01120-9

Congjun Yu, Zining Zhang, Guangbin Dong

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A strongly coupled Ru–CrOx cluster–cluster heterostructure for efficient alkaline hydrogen electrocatalysis 用于高效碱性氢气电催化的强耦合 Ru-CrOx 簇簇异质结构

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-03-11 DOI: 10.1038/s41929-024-01126-3

Bingxing Zhang, Jianmei Wang, Guimei Liu, Catherine M. Weiss, Danqing Liu, Yaping Chen, Lixue Xia, Peng Zhou, Mingxia Gao, Yongfeng Liu, Jian Chen, Yushan Yan, Minhua Shao, Hongge Pan, Wenping Sun

{"title":"A strongly coupled Ru–CrOx cluster–cluster heterostructure for efficient alkaline hydrogen electrocatalysis","authors":"Bingxing Zhang, Jianmei Wang, Guimei Liu, Catherine M. Weiss, Danqing Liu, Yaping Chen, Lixue Xia, Peng Zhou, Mingxia Gao, Yongfeng Liu, Jian Chen, Yushan Yan, Minhua Shao, Hongge Pan, Wenping Sun","doi":"10.1038/s41929-024-01126-3","DOIUrl":"10.1038/s41929-024-01126-3","url":null,"abstract":"Constructing well-defined heterostructure interfaces in catalysts is an efficient strategy to break the so-called scaling relationships and to accelerate the reactions involving multiple intermediates. Here a cluster–cluster heterostructure catalyst composed of crystalline ruthenium cluster and amorphous chromium oxide cluster is designed to realize high-performance alkaline hydrogen electrocatalysis. The strongly coupled cluster–cluster heterostructure interface induces a unique interfacial interpenetration effect, which simultaneously optimizes the adsorption of intermediates on each cluster. The resulting catalyst exhibits impressive catalytic activities for the hydrogen oxidation reaction (exchange current density of 2.8 A mg−1Ru) and the hydrogen evolution reaction (mass activity of 23.0 A mg−1Ru at the overpotential of 100 mV) in alkaline media. The hydroxide exchange membrane fuel cell delivers a mass activity of 22.4 A mg−1Ru at 0.65 V and outstanding durability with no voltage loss over 105 h operation at 500 mA cm−2. The present work demonstrates the superiority of cluster–cluster heterostructure interface towards the development of advanced catalysts. The synthesis of well-defined heterostructure interfaces can be leveraged to design advanced catalysts. Now a catalyst consisting of carbon-supported Janus particles with crystalline Ru and amorphous CrOx sides is shown to achieve high performance for both alkaline hydrogen oxidation and evolution reactions due to the synergy between both sides.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140114713","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

Just counting ten 数到十

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-02-27 DOI: 10.1038/s41929-024-01122-7

Chenyu Wang

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The quest for correlations 寻求相关性

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-02-27 DOI: 10.1038/s41929-024-01129-0

引用次数: 0

Retraction Note: A universal principle for a rational design of single-atom electrocatalysts 撤回说明：合理设计单原子电催化剂的通用原则

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-02-27 DOI: 10.1038/s41929-024-01125-4

Haoxiang Xu, Daojian Cheng, Dapeng Cao, Xiao Cheng Zeng

引用次数: 0

Revisiting the universal principle for the rational design of single-atom electrocatalysts 重新审视合理设计单原子电催化剂的通用原理

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-02-27 DOI: 10.1038/s41929-023-01106-z

Haoxiang Xu, Daojian Cheng, Dapeng Cao, Xiao Cheng Zeng

{"title":"Revisiting the universal principle for the rational design of single-atom electrocatalysts","authors":"Haoxiang Xu, Daojian Cheng, Dapeng Cao, Xiao Cheng Zeng","doi":"10.1038/s41929-023-01106-z","DOIUrl":"10.1038/s41929-023-01106-z","url":null,"abstract":"The notion of descriptors has been widely used for assessing structure–activity relationships for many types of heterogenous catalytic reaction, as well as in searching for highly active single-atom catalysts (SACs). Here, with the aid of a machine-learning model for identifying key intrinsic properties of SACs, we revisit our previous descriptor φ [ , 339–348 (2018) ] and present φ′ to correlate the activity of graphene-based SACs for the oxygen reduction reaction, oxygen evolution reaction and hydrogen evolution reaction. The descriptor φ′ not only captures the activity trend among experimentally reported SACs, but can also help with the search for SACs to replace precious-metal-based commercial catalysts (for example Pt/C and IrO2), including Fe-pyridine/pyrrole-4N for the oxygen reduction reaction and Co-pyridine/pyrrole-4N for the oxygen evolution reaction (discovered in previous experimental studies). More importantly, we show that the descriptor φ′ can be broadly applicable to correlate SACs embedded in small-, mid- and large-sized macrocyclic complexes, so long as the active metal centre has the same local coordination environment. In 2018 a descriptor was put forward to correlate the activity of various electrocatalytic reactions on carbon-based single-atom catalysts, but some data the work was based on were later found to be incorrect. This work revisits and amends the original 2018 study while presenting a modified version of the φ descriptor.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":null,"pages":null},"PeriodicalIF":37.8,"publicationDate":"2024-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139987503","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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Closed-loop optimization 闭环优化

IF 37.8 1区化学

Nature Catalysis Pub Date : 2024-02-27 DOI: 10.1038/s41929-024-01124-5

Marçal Capdevila-Cortada

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