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Rare Earth Benzene Tetraanion-Bridged Amidinate Complexes
IF 8.4 1区 化学
Chemical Science Pub Date : 2024-12-17 DOI: 10.1039/d4sc05982d
Peng-Bo Jin, Qian-Cheng Luo, Gemma Kate Gransbury, Richard E. P. Winpenny, David P Mills, Yan-Zhen Zheng
{"title":"Rare Earth Benzene Tetraanion-Bridged Amidinate Complexes","authors":"Peng-Bo Jin, Qian-Cheng Luo, Gemma Kate Gransbury, Richard E. P. Winpenny, David P Mills, Yan-Zhen Zheng","doi":"10.1039/d4sc05982d","DOIUrl":"https://doi.org/10.1039/d4sc05982d","url":null,"abstract":"The benzene tetraanion-bridged rare earth inverse arene amidinate complexes [{Ln(κ1:η6-Piso)}2(μ-η6:η6-C6H6)] (2-Ln, Ln = Gd, Tb, Dy, Y; Piso = {(NDipp)2CtBu}, Dipp = C6H3iPr2-2,6) were prepared by the reduction of parent Ln(III) bis-amidinate halide precursors [Ln(Piso)2X] (Ln = Tb, Dy; X = Cl, I) or [Ln(Piso)2I] (Ln = Gd, Y) with 3 eq. KC8 in benzene, or by the reaction of the homoleptic Ln(II) complexes [Ln(Piso)2] (Ln = Tb, Dy) with 2 eq. KC8 in benzene. The arene exchange reaction of 2-Tb with toluene gave crystals of [{Tb(κ1:η6-Piso)}2(μ-η6:η6-C7H8)] (3-Tb), while no reactions were observed when C6D6 solutions of 2-Y were separately treated with biphenyl, naphthalene or anthracene. The reactivity study shows that 2-Y can behave as a four-electron reductant to reduce 1,3,5,7-cyclooctatetraene (COT). Complexes 2-Ln were characterized by single crystal X-ray diffraction, elemental analysis, SQUID magnetometry, UV-vis-NIR, ATR-IR, NMR, density functional theory (DFT) and ab initio calculations. These data consistently show that 2-Ln formally contain Ln(III) centres with arene-capped inverse-sandwich Dipp–Ln(III)–(C6H6)4––Ln(III)–Dipp configurations, and DFT calculations on a model of 2-Y revealed strong Y–(C6H6)4– δ-bonding interactions between the filled π-orbitals of the benzene tetraanion and vacant 4d orbitals of the Y(III) ions. A strong intermolecular coupling interaction between the two Tb(III) centres in 2-Tb (Jtot = −6.84 cm–1) was evidenced by a step in a magnetization vs. field plot of 2-Tb at ca. 3.4 T at 2 K, which we attribute to an anti-ferromagnetic transition of the magnetic moment; we also determined an exchange coupling constant Jex = –0.25(1) cm–1 for 2-Gd.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"24 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841681","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
pH-Responsive Nanotubes from Asymmetric Cyclic Peptide-Polymer Conjugates 来自不对称环肽-聚合物共轭物的 pH 响应纳米管
IF 8.4 1区 化学
Chemical Science Pub Date : 2024-12-17 DOI: 10.1039/d4sc06288d
Zihe Cheng, Sébastien Perrier, Qiao Song, Stephen Hall
{"title":"pH-Responsive Nanotubes from Asymmetric Cyclic Peptide-Polymer Conjugates","authors":"Zihe Cheng, Sébastien Perrier, Qiao Song, Stephen Hall","doi":"10.1039/d4sc06288d","DOIUrl":"https://doi.org/10.1039/d4sc06288d","url":null,"abstract":"Self-assembling cyclic peptide nanotubes are fascinating supramolecular systems with promising potential for various applications, such as drug delivery, transmembrane ionic channels, and artificial light-harvesting systems. In this study, we present novel pH-responsive nanotubes based on asymmetric cyclic peptide-polymer conjugates. The pH response is introduced by a tertiary amine-based polymer, poly(dimethylamino ethyl methacrylate) (pDMAEMA) or poly(diethylamino ethyl methacrylate) (pDEAEMA) which is quaternised at low pH. The self-assembling behaviour of their corresponding conjugates is investigated using different scattering and spectroscopy techniques. Compared to conjugates with hydrophilic polymeric corona, the introduction of hydrophobic polymer chains on the periphery of the cyclic peptides can prevent water molecules from penetrating through to the peptide rings, allowing the construction of hydrogen bonding interactions between cyclic peptides to form longer nanotubes. The switching between assembly and non-assembly is triggered by the change in the surrounding environmental pH, which process is controlled by the coordination between hydrophobic interactions and electrostatic repulsions. Due to the different hydrophobicity of these two polymers, the self-assembly of their corresponding conjugates varies extensively. We first demonstrate this evolution in detail and describe the relationship between the self-assembly and the inherent properties of grafted polymers, such as polymer compositions, the protonation degree of the responsive polymers and the polymer molecular weight in solutions.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"47 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142831934","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
Hollow-SiO2@CuxZnyMgzAl-LDHs as catalyst precursors for CO2 hydrogenation to methanol 作为二氧化碳加氢制甲醇催化剂前驱体的中空二氧化硅@CuxZnyMgzAl-LDHs
IF 8.4 1区 化学
Chemical Science Pub Date : 2024-12-17 DOI: 10.1039/d4sc07292h
Tomasz Kondratowicz, Marta Gajewska, Jiangtong Li, Molly Meng-Jung Li, Zoë R. Turner, Chunping Chen, Dermot O'Hare
{"title":"Hollow-SiO2@CuxZnyMgzAl-LDHs as catalyst precursors for CO2 hydrogenation to methanol","authors":"Tomasz Kondratowicz, Marta Gajewska, Jiangtong Li, Molly Meng-Jung Li, Zoë R. Turner, Chunping Chen, Dermot O'Hare","doi":"10.1039/d4sc07292h","DOIUrl":"https://doi.org/10.1039/d4sc07292h","url":null,"abstract":"We report a new synthetic strategy for preparing well-organised, spherical and mesoporous, mixed-metal, hollow-core@layered double hydroxides. Hollow-SiO<small><sub>2</sub></small>@Cu<small><sub><em>x</em></sub></small>Zn<small><sub><em>y</em></sub></small>Mg<small><sub><em>z</em></sub></small>Al-LDHs (<em>x</em> + <em>y</em> + <em>z</em> = 2.32 ± 0.06) were prepared by exploiting a unique “memory effect” feature of LDH materials. The reconstruction with simultaneous incorporation of Cu<small><sup>2+</sup></small> and Zn<small><sup>2+</sup></small> into the LDH shell was achieved by exposing hollow-SiO<small><sub>2</sub></small>@Mg<small><sub>2</sub></small>Al-LDO to an aqueous solution containing Cu<small><sup>2+</sup></small> and Zn<small><sup>2+</sup></small> cations. The effect of a single reconstruction step with various concentrations of Cu<small><sup>2+</sup></small> and Zn<small><sup>2+</sup></small> solutions (20–80 mM), as well as the implementation of five successive cycles of calcination–reconstruction on the chemical composition, morphology, texture and structure of the resulting materials are described. Hollow-SiO<small><sub>2</sub></small>@Cu<small><sub><em>x</em></sub></small>Zn<small><sub><em>y</em></sub></small>Mg<small><sub><em>z</em></sub></small>Al-LDHs are precursors to active catalysts for CO<small><sub>2</sub></small> hydrogenation to methanol. The most active catalyst exhibits a space-time yield for methanol of 1.68 g<small><sub>MeOH</sub></small> g<small><sub>Cu</sub></small><small><sup>−1</sup></small> h<small><sup>−1</sup></small> at 270 °C (3 : 1 CO<small><sub>2</sub></small> : H<small><sub>2</sub></small>, 30 bar) which represents a 1.7-fold increase in space-time yield compared to commercial Cu/ZnO/Al<small><sub>2</sub></small>O<small><sub>3</sub></small> catalyst under the same conditions.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"42 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142831933","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
Folded-Twisted Mechanisms Control Dynamic Redox Properties, Photophysics and Electron Transfer of Anthanthrene-Quinodimethanes
IF 8.4 1区 化学
Chemical Science Pub Date : 2024-12-16 DOI: 10.1039/d4sc06442a
Abel Cardenas Valdivia, Frédéric Lirette, Jose Marin Marin-Beloqui, Abel Carreras, David Casanova, Joël Boismenu-Lavoie, Jean-Francois Morin, Juan Casado Cordón
{"title":"Folded-Twisted Mechanisms Control Dynamic Redox Properties, Photophysics and Electron Transfer of Anthanthrene-Quinodimethanes","authors":"Abel Cardenas Valdivia, Frédéric Lirette, Jose Marin Marin-Beloqui, Abel Carreras, David Casanova, Joël Boismenu-Lavoie, Jean-Francois Morin, Juan Casado Cordón","doi":"10.1039/d4sc06442a","DOIUrl":"https://doi.org/10.1039/d4sc06442a","url":null,"abstract":"The synthesis, electrochemical, spectroelectrochemical, photophysical and light induced electron transfer reactions in two new anthanthrene quinodimethanes have been studied and analyzed in the context of dynamic electrochemistry. Their properties are dependent on the interconversion between folded and twisted forms, which are separated by a relatively small energy range, thus allowing to explore their interconversion by variable temperature measurements. The photophysics of these molecules is mediated by a diradical excited state with a twisted structure that habilitates rapid intersystem crossing. Moreover, when codissolved with an electron acceptor compound such as PCBM, direct anthanthrene to PCBM electron transfer and back-electron transfer are also observed, resulting in the formation of charged states and, then, a raise in the population of the excited state triplet manifold upon charge recombination. Some of these properties have been interpreted with the help of quantum chemical calculations. The existence of an equilibrium between folded and twisted states upon electrochemical and photoexcitation stimuli represents a novelty in comparison with existing literature on compounds also showing dynamic electrochemical properties.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"409 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825660","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
Diacetylene-bridged covalent organic framework as crystalline graphdiyne analogue for photocatalytic hydrogen evolution
IF 8.4 1区 化学
Chemical Science Pub Date : 2024-12-16 DOI: 10.1039/d4sc06633b
Zhiqing Lin, Songyao Dai, Shan Yao, Qia-Chun Lin, Mengying Fu, Lai-Hon Chung, Bin Han, Jun He
{"title":"Diacetylene-bridged covalent organic framework as crystalline graphdiyne analogue for photocatalytic hydrogen evolution","authors":"Zhiqing Lin, Songyao Dai, Shan Yao, Qia-Chun Lin, Mengying Fu, Lai-Hon Chung, Bin Han, Jun He","doi":"10.1039/d4sc06633b","DOIUrl":"https://doi.org/10.1039/d4sc06633b","url":null,"abstract":"Graphdiyne (GDY) alone as photocatalyst is unsatisfactory because of low crystallinity, limited regulation of band gap, weak photogenerated charge separation, etc., and heterojunctioning with other materials is necessary to activate the photocatalytic activity of GDY. Through elaborate design, a diacetylene-rich linker (S2) was prepared and allowed to construct crystalline and structurally well-defined GDY-like covalent organic framework (COF, namely S2-TP COF) which merges the merits of both COF and GDY to boost photocatalytic hydrogen evolution reaction (HER). By theoretical prediction on the donor-acceptor (D-A) pair, other two monoacetylene-bridged COFs (S1-TP COF and S3-TP COF) were prepared for comparison. Exhibiting enhanced separation and suppressed recombination of photogenerated excitons, Pt-photodeposited S2-TP COF showed a higher HER rate (10.16 mmol g−1 h−1) than the other two non-GDY-like COFs (3.71 and 1.13 mmol g−1 h−1). The joint experimental-theoretical study suggests appropriate D-A structure for photogenerated charge separation and diacetylene motif as adsorption site to be key accounts for boosted HER. This work opens a new opportunity for the rational design of COF as GDY mimic for photocatalytic application.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"144 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825665","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
Two-photon brightness of NIR-emitting, atomically precise DNA-stabilized silver nanoclusters
IF 8.4 1区 化学
Chemical Science Pub Date : 2024-12-16 DOI: 10.1039/d4sc05853d
Joanna Olesiak-Banska, Agata Hajda, Rweetuparna Guha, Stacy M. Copp
{"title":"Two-photon brightness of NIR-emitting, atomically precise DNA-stabilized silver nanoclusters","authors":"Joanna Olesiak-Banska, Agata Hajda, Rweetuparna Guha, Stacy M. Copp","doi":"10.1039/d4sc05853d","DOIUrl":"https://doi.org/10.1039/d4sc05853d","url":null,"abstract":"Near-infrared (NIR) emitters with high two-photon absorption (2PA) cross-sections are of interest to enable in vivo imaging in the tissue transparency windows. This study explores the potential of DNA-stabilized silver nanoclusters (AgN-DNAs) as water-soluble two-photon absorbers. We investigate 2PA of four different atomically precise AgN-DNA species with far-red to NIR emission and varying nanocluster and ligand compositions. 2PA cross-sections, σ2, were determined by two-photon excited luminescence (TPEL) technique for a wide wavelength range from 810 to 1400 nm. The AgN-DNAs exhibited reversed strength of corresponding transitions in the two-photon regime, as compared to one-photon, which further demonstrates the complex photophysics of these emitters. Maximal 2PA cross-section value (813 GM) was observed for (DNA)3[Ag21]15+, which is stabilized by 3 DNA oligomers. (DNA)2[Ag16Cl2]8+ presented distinct 2PA behavior from the AgN-DNAs without chlorido ligands, with a high 2PA of 176 GM at 1050 nm. Our findings support the potential of AgN-DNAs as NIR-to-NIR two-photon probes that are both excited and emit in the NIR. Their high σ2 and fluorescence quantum yield values result in superior two-photon brightness on the order of ~102 GM, significantly higher than water-soluble organic fluorophores.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"41 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825666","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
pH-Responsive Supramolecular Switch of Rationally Designed Dipyrroethene-Based Chromophore 合理设计的双吡咯烷基色团的 pH 响应超分子开关
IF 8.4 1区 化学
Chemical Science Pub Date : 2024-12-16 DOI: 10.1039/d4sc07016j
Debasish Mandal, Abani Sarkar, Kanhu Charan Behera, Mangalampalli Ravikanth
{"title":"pH-Responsive Supramolecular Switch of Rationally Designed Dipyrroethene-Based Chromophore","authors":"Debasish Mandal, Abani Sarkar, Kanhu Charan Behera, Mangalampalli Ravikanth","doi":"10.1039/d4sc07016j","DOIUrl":"https://doi.org/10.1039/d4sc07016j","url":null,"abstract":"Herein, we present a strategy to access a novel class of pH-responsive, dual-state emissive (DSE), highly fluorescent pyrrole-based chromophores via diformylation of dipyrroethenes (DPE) followed by condensation with various anilines derivatives. The DPE-based chromophores exhibit a large Stokes’ shift and maintain good fluorescent quantum yields. Remarkably, these chromophores demonstrate reversible colourimetric changes and a fluorometric 'on-off-on' switch in response to pH variations. Various spectroscopic techniques, optical microscopy, X-ray crystallography, and computational studies revealed that the synthesized molecules adopt a two-dimensional conformation due to the presence of strong π···π stacking and hydrogen bonding interactions, allowing them to function as flexible molecular hosts. Under acidic conditions, selective protonation of imine bonds and subsequent complexation with counter anion enhance the host-guest interactions, resulting in a stable three-dimensional supramolecular structure. Notably, the reversibility of these molecules under basic conditions showcases the robustness and potential applications of these chromophores in various fields, ranging from the design of finely tuned pH-responsive degradable polymers to self-healing materials, sensing, and molecular devices.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"3 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825662","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
Kinetics and Dynamics of Atomic-Layer Dissolution on Low-Defect Ag
IF 8.4 1区 化学
Chemical Science Pub Date : 2024-12-16 DOI: 10.1039/d4sc05954a
Yufei Hang Wang, Roberto García Carrillo, Hang Ren
{"title":"Kinetics and Dynamics of Atomic-Layer Dissolution on Low-Defect Ag","authors":"Yufei Hang Wang, Roberto García Carrillo, Hang Ren","doi":"10.1039/d4sc05954a","DOIUrl":"https://doi.org/10.1039/d4sc05954a","url":null,"abstract":"Electrochemical metal dissolution reaction is a fundamental process in various critical technologies, including metal anode batteries and nanofabrication. However, experimentally revealing the kinetics and dynamics of active sites of metal dissolution reactions is challenging. Herein, we investigate metal dissolution on near-perfect single-crystal surfaces of Ag within regions of a few hundred nanometers isolated by scanning electrochemical cell microscopy (SECCM). Potential oscillation is observed under constant current conditions for dissolution. The one-to-one correspondence between the dissolution charge and the geometry of the dissolution from colocalized imaging allows ambiguous correlation, which suggests that each oscillation cycle corresponds to the dissolution of one atomic layer. The oscillation behavior is further explained in a kinetic model, which reveals that the oscillation comes from the dynamic evolution of the number of different active sites as the dissolution progresses on each atomic layer. In addition to the fundamental interest, the ability to observe layer-by-layer dissolution in electrochemical measurement suggests a potential pathway for developing electrochemical atomic layer etching for fabricating structures and devices with atomic precision.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"232 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825659","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
Probing the Synergistic Effects of Amino Compounds in Mitigating Oxidation in 2D Ti3C2Tx MXene nanosheets in Aqueous Environment
IF 8.4 1区 化学
Chemical Science Pub Date : 2024-12-16 DOI: 10.1039/d4sc05097e
Jai Kumar, Jiayi Tan, Razium Ali Soomro, Ning Sun, Bin Xu
{"title":"Probing the Synergistic Effects of Amino Compounds in Mitigating Oxidation in 2D Ti3C2Tx MXene nanosheets in Aqueous Environment","authors":"Jai Kumar, Jiayi Tan, Razium Ali Soomro, Ning Sun, Bin Xu","doi":"10.1039/d4sc05097e","DOIUrl":"https://doi.org/10.1039/d4sc05097e","url":null,"abstract":"The shelf life of 2D MXenes in functional devices and colloidal dispersions is compromised due to oxidation in the aqueous system. Herein, a systematic investigation is carried out to explore the potential of various amino compounds as antioxidants for Ti3C2Tx MXenes. A range of basic, acidic, and neutral amino acids were examined for their effectiveness, where certain antioxidants failed to protect MXenes from oxidation, while others accelerated their decomposition. Serine, threonine, and asparagine demonstrated excellent antioxidant activity, likely due to their evenly distributed molecular charges. These neutral amino acids outperformed glutamic acid, which possesses an electron-withdrawing -COOH group, and lysine, with an electron-donating -NH2 group. Serine functionalized MXene realized a stabilization time constant reaching 128 days, as determined by first-order reaction kinetics. Additionally, when employed as supercapacitor electrodes, aged MXene and serine-functionalized MXene exhibited specific capacitance values of 219.2 and 280.3 F g-1 at 5 A g-1 after 6 weeks, respectively. This work addresses a gap in the practical work on ionic stabilization of 2D MXenes and has significant implications for the long-term colloidal storage of MXenes using greener chemicals.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"17 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825661","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
Structure–reactivity relationships in CO2 hydrogenation to C2+ chemicals on Fe-based catalysts
IF 8.4 1区 化学
Chemical Science Pub Date : 2024-12-16 DOI: 10.1039/d4sc06376g
Jie Zhu, Shamil Shaikhutdinov, Beatriz Roldan Cuenya
{"title":"Structure–reactivity relationships in CO2 hydrogenation to C2+ chemicals on Fe-based catalysts","authors":"Jie Zhu, Shamil Shaikhutdinov, Beatriz Roldan Cuenya","doi":"10.1039/d4sc06376g","DOIUrl":"https://doi.org/10.1039/d4sc06376g","url":null,"abstract":"Catalytic conversion of carbon dioxide (CO<small><sub>2</sub></small>) to value-added products represents an important avenue towards achieving carbon neutrality. In this respect, iron (Fe)-based catalysts were recognized as the most promising for the production of C<small><sub>2+</sub></small> chemicals <em>via</em> the CO<small><sub>2</sub></small> hydrogenation reaction. However, the complex structural evolution of the Fe catalysts, especially during the reaction, presents significant challenges for establishing the structure–reactivity relationships. In this review, we provide critical analysis of recent <em>in situ</em> and <em>operando</em> studies on the transformation of Fe-based catalysts in the hydrogenation of CO<small><sub>2</sub></small> to hydrocarbons and alcohols. In particular, the effects of composition, promoters, support, and particle size on reactivity; the role of the catalyst's activation procedure; and the catalyst's evolution under reaction conditions will be addressed.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"106 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825664","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
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