Chem Catalysis最新文献

筛选
英文 中文
Boosting active hydrogen generation by anchored Ru sites in Co3O4 for nitrate-to-ammonia electrosynthesis 通过锚定 Co3O4 中的 Ru 位点提高硝酸-氨电合成中的活性制氢能力
IF 9.4
Chem Catalysis Pub Date : 2024-10-17 DOI: 10.1016/j.checat.2024.101152
Zhaole Lu, Rong Yang, Yingchao Yu, Yuting Wang, Bin Zhang, Lingjun Kong
{"title":"Boosting active hydrogen generation by anchored Ru sites in Co3O4 for nitrate-to-ammonia electrosynthesis","authors":"Zhaole Lu, Rong Yang, Yingchao Yu, Yuting Wang, Bin Zhang, Lingjun Kong","doi":"10.1016/j.checat.2024.101152","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101152","url":null,"abstract":"The electrochemical reduction of nitrate to ammonia can serve as an effective complement to the traditional Haber-Bosch process. Currently, rapid and continuous ammonia production is challenging because of the multistep hydrogenation process and the constant alkalinization of the electrolyte. Herein, Ru atoms are incorporated into the octahedral sites of Co<sub>3</sub>O<sub>4</sub> to achieve an ammonia yield rate of 24.6 mg h<sup>−1</sup> cm<sup>−2</sup>. Electrochemical <em>in situ</em> spectroscopic analyses and theoretical calculations reveal that Ru sites improve water molecule coverage and facilitate the production of active hydrogen atoms, leading to stable and orderly ammonia production. Furthermore, a peak power density of 32.28 mW cm<sup>−2</sup>, a high ammonia Faradaic efficiency of 98.2%, and excellent durability (91 h) are achieved in a Ru-Co<sub>3</sub>O<sub>4</sub>-based Zn-nitrate battery, indicating its practical applicability. This work may provide a method for efficient nitrate reduction to ammonia or other hydrogenation reactions via the synergistic modulation of active sites.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"3 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444429","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Quantum confinement for stable nickel catalyst in hydrogen oxidation 氢氧化中稳定镍催化剂的量子约束
IF 9.4
Chem Catalysis Pub Date : 2024-10-17 DOI: 10.1016/j.checat.2024.101150
Jihyeon Park, Drew Higgins
{"title":"Quantum confinement for stable nickel catalyst in hydrogen oxidation","authors":"Jihyeon Park, Drew Higgins","doi":"10.1016/j.checat.2024.101150","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101150","url":null,"abstract":"The quest for low-cost, Earth-abundant catalysts for hydrogen oxidation reactions (HORs) in anion-exchange membrane fuel cells (AEMFCs) has led to significant advancements in recent years, yet challenges pertaining to the stability of non-platinum-group metal catalysts operational conditions still remain. The study by Zhou et al. in <em>Nature Energy</em> presents an innovative approach to enhance the stability and performance of nickel (Ni) catalysts for the HOR by using quantum confinement effects to suppress Ni oxidation. This research not only addresses surface passivation of Ni-based catalysts but also unlocks new possibilities for designing advanced catalysts for energy conversion technologies.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"10 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444432","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Strong metal-support interaction between Ni and BaCO3 boosts CO2 hydrogenation 镍和 BaCO3 之间强烈的金属支撑相互作用促进了二氧化碳加氢反应
IF 9.4
Chem Catalysis Pub Date : 2024-10-17 DOI: 10.1016/j.checat.2024.101143
Hai Wang, Liang Wang
{"title":"Strong metal-support interaction between Ni and BaCO3 boosts CO2 hydrogenation","authors":"Hai Wang, Liang Wang","doi":"10.1016/j.checat.2024.101143","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101143","url":null,"abstract":"In the current issue of <em>Chem Catalysis</em>, Zhu and co-workers report the construction of a neotype strong metal-support interaction between Ni nanoparticle and BaCO<sub>3</sub> via H<sub>2</sub> reduction and CO<sub>2</sub> hydrogenation. The migration of BaCO<sub>3</sub> onto Ni nanoparticles leads to the formation of porous overlayers, which not only stabilized the Ni nanoparticles against sintering but also formed abundant Ni-BaCO<sub>3</sub> interfaces for CO<sub>2</sub> enrichment, thereby enhancing CO<sub>2</sub> hydrogenation to methane.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"68 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444430","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synergistic effects in organic mixtures for enhanced catalytic hydrogenation and hydrodeoxygenation 有机混合物中增强催化加氢和加氢脱氧的协同效应
IF 9.4
Chem Catalysis Pub Date : 2024-10-16 DOI: 10.1016/j.checat.2024.101135
Ankit Mathanker, Sahil Halarnkar, Bolton Tran, Nirala Singh, Bryan R. Goldsmith
{"title":"Synergistic effects in organic mixtures for enhanced catalytic hydrogenation and hydrodeoxygenation","authors":"Ankit Mathanker, Sahil Halarnkar, Bolton Tran, Nirala Singh, Bryan R. Goldsmith","doi":"10.1016/j.checat.2024.101135","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101135","url":null,"abstract":"The hydrogenation and hydrodeoxygenation (HDO) of organic mixtures are important processes in bio-oil conversion and plastics upcycling. Understanding how the presence of co-reactants in organic mixtures affects the kinetics is critical for designing reactors that can convert these mixtures into desired products. Here, we discuss cases in (electro)catalysis where the presence of a co-reactant <em>R</em><sub>2</sub> enhances the rate of hydrogenation or HDO of another reactant <em>R</em><sub>1</sub> beyond the rate if only <em>R</em><sub>1</sub> is present. We divide the discussion into simple and complex mutual influences. Simple mutual influences occur when the presence of <em>R</em><sub>2</sub> does not change the mechanism or values of rate constants of elementary steps for <em>R</em><sub>1</sub>. A complex mutual influence of <em>R</em><sub>2</sub> on <em>R</em><sub>1</sub> occurs if the presence of <em>R</em><sub>2</sub> changes the rate constants of elementary steps involving <em>R</em><sub>1</sub>. We discuss challenges and opportunities in discerning the different mutual influences and increasing their synergistic effects in organic mixtures.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"66 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142440410","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Chiral pyrrolidines via an enantioselective Hofmann-Löffler-Freytag reaction 通过对映选择性 Hofmann-Löffler-Freytag 反应制备手性吡咯烷酮
IF 9.4
Chem Catalysis Pub Date : 2024-10-16 DOI: 10.1016/j.checat.2024.101149
Pavitra Laohapaisan, Ipshita Roy, David A. Nagib
{"title":"Chiral pyrrolidines via an enantioselective Hofmann-Löffler-Freytag reaction","authors":"Pavitra Laohapaisan, Ipshita Roy, David A. Nagib","doi":"10.1016/j.checat.2024.101149","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101149","url":null,"abstract":"Radical C–H aminations enable rapid access to the most common heterocycles in medicines (e.g., pyrrolidines), yet stereocontrol of these powerful transformations remains a challenge. Here, we report the discovery of the first enantio- and regioselective C–H imination, which readily converts ketones to enantioenriched pyrrolidines. This enantioselective Hofmann-Löffler-Freytag reaction mechanism entails iminyl radical generation from an oxime by a chiral Cu catalyst that facilitates 1,5-H-atom transfer (HAT) to form a remote C-radical regioselectively. The selective capture of this alkyl radical as an organocopper(III) complex then mediates highly stereoselective reductive elimination to unprotected pyrrolines. The broad steric and electronic scope of this remote C–H amination has been probed systematically, along with key mechanistic aspects of enantiodetermination, radical intermediacy, and atypical Cu(III) ligands that enable this uniquely selective C–N coupling. Importantly, either (1) reductions or (2) nucleophilic additions to these enantioenriched pyrrolines provide the most rapid syntheses of chiral pyrrolidines to date.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"124 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142440409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sulfur-facilitated in situ deep reconstruction of transition metal molybdates toward superior electrocatalytic oxidation of alkaline seawater 硫促进过渡金属钼酸盐原位深度重构,实现碱性海水的卓越电催化氧化作用
IF 9.4
Chem Catalysis Pub Date : 2024-10-15 DOI: 10.1016/j.checat.2024.101144
Zhan Zhao, Shiyu Qin, Xiang Li, Jianpeng Sun, Zizhen Li, Xiangchao Meng
{"title":"Sulfur-facilitated in situ deep reconstruction of transition metal molybdates toward superior electrocatalytic oxidation of alkaline seawater","authors":"Zhan Zhao, Shiyu Qin, Xiang Li, Jianpeng Sun, Zizhen Li, Xiangchao Meng","doi":"10.1016/j.checat.2024.101144","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101144","url":null,"abstract":"Inducing the rapid and deep self-reconstruction of anodes has the potential to achieve the desired structure for effective oxygen evolution reactions (OERs) in seawater, but it is challenging. Herein, sulfur-assisted structural reconstruction of transition metal molybdates was fabricated. Benefiting from the electronic escape effect that occurs due to metal–O/–S bonding orbitals in the pre-catalyst, deep electrochemical reconstruction to highly active S-doped oxyhydroxides was achieved via rational S–metal hybridization and phase transition in the pre-catalyst. Meanwhile, combining the theoretical calculations and spectroscopic tests, it was found that introducing S atoms into oxyhydroxides activated lattice oxygen atoms, thereby boosting the intrinsic OER activity following the lattice oxygen mechanism pathway. As tested, the final S-doped oxyhydroxide catalysts exhibited excellent electrocatalytic activity with an ultralow overpotential of 166 mV at 10 mA cm<sup>−2</sup> in alkaline seawater oxidation. This work showcased a feasible strategy of sulfur-assisted structural reconstruction to fabricate highly efficient and chemically stable materials for seawater splitting.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"66 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142435996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electron paramagnetic resonance spectroscopy for the analysis of single-atom catalysts 电子顺磁共振光谱法用于分析单原子催化剂
IF 9.4
Chem Catalysis Pub Date : 2024-10-15 DOI: 10.1016/j.checat.2024.101136
Mikhail Agrachev, Vera Giulimondi, Ivan Surin, Sharon Mitchell, Gunnar Jeschke, Javier Pérez-Ramírez
{"title":"Electron paramagnetic resonance spectroscopy for the analysis of single-atom catalysts","authors":"Mikhail Agrachev, Vera Giulimondi, Ivan Surin, Sharon Mitchell, Gunnar Jeschke, Javier Pérez-Ramírez","doi":"10.1016/j.checat.2024.101136","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101136","url":null,"abstract":"Single-atom catalysts (SACs) are an important material class, lying at the forefront of precision design for heterogeneous catalysis research. Despite extensive investigations of their structure and reactivity using state-of-the-art analytical tools, new approaches are sought to improve the understanding of their properties and catalytic behavior. This review highlights the often-overlooked potential of electron paramagnetic resonance (EPR) spectroscopy, which is exceptionally suited to studying isolated paramagnetic species. EPR provides valuable complementary insights into SACs, including metal oxidation state, dispersion degree, local coordination environment, and catalytically relevant features of support materials. To enhance the technique’s accessibility, we provide a tutorial on EPR, summarize significant findings to date, place them within a broader methodological framework for SAC applications, and identify key directions for future research.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"230 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436305","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
An enzymatic cascade for high-yield and stereoselective synthesis of 4-fluoro-L-threonine 高产率和立体选择性合成 4-氟-L-苏氨酸的酶级联反应
IF 9.4
Chem Catalysis Pub Date : 2024-10-15 DOI: 10.1016/j.checat.2024.101148
Alberto De Maria, Manuel Nieto-Domínguez, Phillip T. Lowe, David O′Hagan, Pablo I. Nikel
{"title":"An enzymatic cascade for high-yield and stereoselective synthesis of 4-fluoro-L-threonine","authors":"Alberto De Maria, Manuel Nieto-Domínguez, Phillip T. Lowe, David O′Hagan, Pablo I. Nikel","doi":"10.1016/j.checat.2024.101148","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101148","url":null,"abstract":"The critical role of fluorine in bioactive molecule design requires selective fluorination methods for synthesizing novel building blocks, such as fluorinated amino acids. Here, we focused on L-threonine aldolases (LTAs), enzymes that mediate reversible aldol additions to the α carbon of glycine. Their C–C bond formation ability and substrate flexibility make these enzymes ideal catalysts for fluorine biocatalysis. We harnessed the promiscuous activity of the LTAs isolated from either <em>Escherichia coli</em> or <em>Pseudomonas putida</em> on 2-fluoroacetaldehyde in a two-step enzymatic cascade for efficient 4-fluoro-L-threonine synthesis. By implementing 2-fluoroethanol as the primary fluorodonor in these cascades, we demonstrated that the LTA enzyme isolated from <em>P</em>. <em>putida</em> mediates a high 4-fluoro-L-threonine yield (&gt;90%) while displaying stereoselectivity for the L-<em>syn</em> form.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"17 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142435995","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Utilizing operando catalyst regeneration to uncover insights in the methanol-to-hydrocarbons process 利用操作性催化剂再生技术揭示甲醇制烃类工艺的奥秘
IF 9.4
Chem Catalysis Pub Date : 2024-10-15 DOI: 10.1016/j.checat.2024.101134
Sophie H. van Vreeswijk, Luke A. Parker, Arnaud T. Sanderse, Ramon Oord, Florian Meirer, Bert M. Weckhuysen
{"title":"Utilizing operando catalyst regeneration to uncover insights in the methanol-to-hydrocarbons process","authors":"Sophie H. van Vreeswijk, Luke A. Parker, Arnaud T. Sanderse, Ramon Oord, Florian Meirer, Bert M. Weckhuysen","doi":"10.1016/j.checat.2024.101134","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101134","url":null,"abstract":"The methanol-to-hydrocarbons (MTH) catalyst deactivation is reversible, and deactivating coke molecules can be removed via regeneration experiments. Regeneration of small-pore zeolite SSZ-13 first leads to the elimination of polyaromatic deactivating compounds, leaving the active aromatic intermediates intact. Partial regeneration experiments can provide an alternative approach to study small-pore zeolites by mimicking co-feeding of aromatic intermediates. Catalyst properties and reaction intermediates were followed with <em>operando</em> UV-visible spectroscopy and X-ray diffraction. It was shown that all the coke is formed within the zeolite cages and that the lattice expansion is due to the formation of hydrocarbon molecules. Additionally, indications for separate reaction mechanisms to produce ethylene and propylene were established. With confocal fluorescence microscopy (CFM), it was determined that upon regeneration, the hydrocarbons were less conjugated and more homogeneously distributed. A full hydrocarbon pool mechanism was established for the MTH reaction over zeolite SSZ-13.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"23 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142435997","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Next-generation functional surfactant for mild C−H arylation under micellar conditions 用于胶束条件下温和 C-H 芳基化的新一代功能表面活性剂
IF 9.4
Chem Catalysis Pub Date : 2024-10-10 DOI: 10.1016/j.checat.2024.101146
Pascal Hauk, Sven Trienes, Fabrice Gallou, Lutz Ackermann, Joanna Wencel-Delord
{"title":"Next-generation functional surfactant for mild C−H arylation under micellar conditions","authors":"Pascal Hauk, Sven Trienes, Fabrice Gallou, Lutz Ackermann, Joanna Wencel-Delord","doi":"10.1016/j.checat.2024.101146","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101146","url":null,"abstract":"Micellar reaction conditions have emerged as a powerful and sustainable strategy in synthetic organic chemistry. Numerous transformations have been reported to work under micellar conditions; however, transformations such as C−H activation remain scarce, and the compartmentalization effects are not yet fully understood. Herein, we describe a rational surfactant design for challenging C−H activation. Incorporating a pyridone ligand into a commercially available PS-750-M surfactant allows for overcoming the compartmentalization issues, resulting in an efficient Ru-catalyzed direct arylation under mild reaction conditions and with excellent selectivity. Physicochemical characterization of this surfactant shed light on the inherent properties of the novel PyOH-750-M surfactant while recycling of the surfactant allows for product formation with a low E-factor of 5.5 without a drop in reactivity.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"108 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398321","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信