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Catalysis for the Energy Transition 能源转换的催化作用
IF 3.9 3区 化学
ChemCatChem Pub Date : 2025-08-05 DOI: 10.1002/cctc.202500588
Dr. John R. Lockemeyer, Dr. Tracy L. Lohr, Dr. Michael A. Reynolds, Dr. Alexander van der Made
{"title":"Catalysis for the Energy Transition","authors":"Dr. John R. Lockemeyer,&nbsp;Dr. Tracy L. Lohr,&nbsp;Dr. Michael A. Reynolds,&nbsp;Dr. Alexander van der Made","doi":"10.1002/cctc.202500588","DOIUrl":"10.1002/cctc.202500588","url":null,"abstract":"<p>Society is at a critical juncture regarding the future of energy security. Traditional fossil resources have been execrated while many sustainable alternatives in the energy transition are commercially or economically unfit-for-purpose. While the amalgamation of energy molecules beyond 2050 remains uncertain, catalysis will play a role in how these molecules are produced. The aim of this perspective is to provide a view of where catalysis can impact technologies necessary for the current energy transition from fossil-based sources to renewable ones, with the primary goal being to reduce net carbon dioxide emissions. This discussion focuses on the importance and means to obtain energy carrier molecules, and the challenges associated with producing them by sustainable means. Production of the target molecules will rely upon development of catalysts designed specifically for each application area involved in the energy transition space, with some technology areas requiring more R&amp;D than others. Discussion around specific opportunities and challenges for envisioned catalysts and processes will be presented. Addressing the demand for energy in forms that can be stored and transported(i. e. the concept of molecular energy carriers) is highlighted with special attention given to specific examples. We will demonstrate that regardless of the chosen route to mitigate the CO<sub>2</sub> footprint of current fossil hydrocarbons, catalysts and catalysis will play an essential role.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 16","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144905449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Correction to “First Row Transition Metals in Olefin Metathesis: The Role of Iron and Manganese” 对“第一排过渡金属在烯烃分解中的作用:铁和锰”的修正
IF 3.9 3区 化学
ChemCatChem Pub Date : 2025-08-05 DOI: 10.1002/cctc.202501166
{"title":"Correction to “First Row Transition Metals in Olefin Metathesis: The Role of Iron and Manganese”","authors":"","doi":"10.1002/cctc.202501166","DOIUrl":"10.1002/cctc.202501166","url":null,"abstract":"&lt;p&gt;A. Brotons Rufes, J. P. Martínez, N. Joly, S. Gaillard, J.-L. Renaud, S. Posada Pérez, A. Poater, &lt;i&gt;ChemCatChem&lt;/i&gt; &lt;b&gt;2025&lt;/b&gt;, &lt;i&gt;17&lt;/i&gt;, e00570.&lt;/p&gt;&lt;p&gt;https://doi.org/10.1002/cctc.202500570&lt;/p&gt;&lt;p&gt;After publication, it was brought to our attention that the discussion of the article by Lincoln and Iluc, cited as Ref. [92] in our work, was lacking. The supplemented discussion follows:&lt;/p&gt;&lt;p&gt;The article by Lincoln and Iluc&lt;sup&gt;[92]&lt;/sup&gt; reports the metathesis of olefins catalyzed by iron carbene complexes. Here, the authors demonstrate that a pincer-ligated iron complex can form a metallacyclobutane intermediate upon reaction with norbornadiene and its derivatives, validating a key intermediate previously elusive for first-row metal-catalyzed olefin metathesis.&lt;/p&gt;&lt;p&gt;This study highlights the unique ability of a PC(sp&lt;sup&gt;2&lt;/sup&gt;)P iron complex to activate a strained olefin through a [2 + 2] addition to form a well-characterized metallacyclobutane intermediate, which subsequently converts to a ring-opened iron alkylidene. Importantly, the formation and breakdown of this intermediate obeys the classical Chauvin olefin metathesis mechanism, a process previously predominantly associated with late transition metal species.&lt;/p&gt;&lt;p&gt;The authors provide extensive structural, spectral, and magnetic data to characterize the intermediate, adding credibility to their proposal. The crystallographically defined structures of the metallacyclobutane and its ring-opened counterpart illuminate key bond formations and cleavages that underpin the metathesis process. Furthermore, the observation of a reversible formation of the ring-opened intermediate upon addition of phosphine underscores a delicate thermodynamics that controls this transformation, reflecting the fundamental role of phosphine dissociation in accessing reactive species.&lt;/p&gt;&lt;p&gt;This work underscores the potential of base metal catalysis in olefin metathesis, a transformation previously thought to be predominantly the domain of 4d and 5d metal species. Importantly, the authors show how careful choice of ancillary pincer and phosphine components can stabilize reactive intermediate species, allowing the observation of key snapshots along the metathesis pathway.&lt;/p&gt;&lt;p&gt;This study not only expands our understanding of the mechanisms by which first-row metal compounds activate olefins but also paves the way for future exploration of base metal-catalyzed olefin metathesis. The ability to employ iron, a non-precious, abundant, and environmentally friendly metal, to catalyze a transformation previously thought to be the purview of heavy metal species holds promise for developing more sustainable and cost-effective catalytic strategies.&lt;/p&gt;&lt;p&gt;Overall, this manuscript provides a sophisticated and insightful view into the mechanisms of iron-catalyzed olefin metathesis and highlights the potential for designing base metal catalyzers to perform challenging bond-forming reactions with high selectivity and under mi","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 16","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202501166","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144905450","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Homogeneous Base-Metal-Catalyzed Transfer Hydrogenation of Unsaturated N-Containing Organic Compounds 均相碱金属催化不饱和含n有机化合物的转移加氢反应
IF 3.9 3区 化学
ChemCatChem Pub Date : 2025-08-05 DOI: 10.1002/cctc.202500702
Ainur Slamova, Dr. Kristina A. Gudun, Dr. Andrey Y. Khalimon
{"title":"Homogeneous Base-Metal-Catalyzed Transfer Hydrogenation of Unsaturated N-Containing Organic Compounds","authors":"Ainur Slamova,&nbsp;Dr. Kristina A. Gudun,&nbsp;Dr. Andrey Y. Khalimon","doi":"10.1002/cctc.202500702","DOIUrl":"10.1002/cctc.202500702","url":null,"abstract":"<p>Owing to the synthetic availability of imines, N-heteroarenes, nitriles, carboxamides, and nitroarenes, their catalytic hydrogenation is considered an attractive and atom-economical route to a diversity of amines, which find widespread applications specialty chemical industries. Although catalytic hydrogenation of unsaturated N-containing organic compounds with compressed H<sub>2</sub> gas is well-established, such transformations require expensive high-pressure equipment and have associated H<sub>2</sub> handling risks. In contrast, transfer hydrogenation protocols utilize nongaseous hydrogen sources, offering significant advantages in the operational cost and safety of transformations. Whereas many economical nonprecious metal catalysts have been described for efficient transfer hydrogenation of aldehydes and ketones, similar systems for selective transfer hydrogenation of unsaturated nitrogen-containing organic compounds have been developed relatively recently. This review aims to highlight current advances and challenges of base-metal-catalyzed (i.e., Mn, Fe, Co, Ni, and Cu) transfer hydrogenation of imines, N-heteroarenes, nitriles, nitro compounds, as well as carboxamides and related molecules to the corresponding amines. Mechanistic aspects of catalytic reactions, the substrate scope, and selectivity of the transformations are also discussed.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 17","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144998859","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Ambient CO2 Hydrogenation to Formate Over NiPd Catalyst NiPd催化剂上环境CO2加氢生成甲酸酯
IF 3.9 3区 化学
ChemCatChem Pub Date : 2025-08-04 DOI: 10.1002/cctc.202500771
Jayashree Parthiban, Bhanu Priya, Rohit Kumar Rai, Satoshi Suganuma, Kiyotaka Nakajima, Sanjay Kumar Singh
{"title":"Ambient CO2 Hydrogenation to Formate Over NiPd Catalyst","authors":"Jayashree Parthiban,&nbsp;Bhanu Priya,&nbsp;Rohit Kumar Rai,&nbsp;Satoshi Suganuma,&nbsp;Kiyotaka Nakajima,&nbsp;Sanjay Kumar Singh","doi":"10.1002/cctc.202500771","DOIUrl":"10.1002/cctc.202500771","url":null,"abstract":"<p>The urgent need for sustainable CO<sub>2</sub> management has driven the development of efficient catalytic systems capable of converting CO<sub>2</sub> into value-added chemicals under mild conditions. Herein, we report a Ni<sub>9</sub>Pd<sub>1</sub> catalyst with a low Pd content (Ni/Pd = 9:1) for the selective CO<sub>2</sub> hydrogenation to formate at low temperatures. Remarkably, this catalyst exhibits exceptional versatility, efficiently hydrogenating both aqueous (bi)carbonate and CO<sub>2</sub> captured from air (as carbonate) to formate. Moreover, this catalyst shows appreciable robustness by achieving cumulative formate yields of 770.5 mmol g<sub>Pd</sub><sup>−1</sup> (TON of 82, STY of 32.18 mmol<sub>formate</sub> g<sub>Pd</sub><sup>−1 </sup>h<sup>−1</sup> at 28 °C) and 1371.9 mmol g<sub>Pd</sub><sup>−1</sup> (TON of 146, STY of 57.16 mmol<sub>formate</sub> g<sub>Pd</sub><sup>−1 </sup>h<sup>−1</sup> at 80 °C) over multiple cycles. The synergistic Ni-to-Pd interaction in this catalyst leads to the efficient CO<sub>2</sub> activation and H<sub>2</sub> dissociation, enabling operation under mild conditions. This study demonstrates an integrated and sustainable approach where CO<sub>2</sub> captured from air can be hydrogenated to formate at low temperature.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 17","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-08-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144998622","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Sustainable Production of 1-Propanol via the Selective Hydrogenolysis of Glycerol Over a Tailored Iridium–Rhenium Oxide Catalyst Supported on HUSY Zeolite 在HUSY分子筛负载的定制氧化铱铼催化剂上通过甘油选择性氢解可持续生产1-丙醇
IF 3.9 3区 化学
ChemCatChem Pub Date : 2025-07-31 DOI: 10.1002/cctc.202500885
Supphathee Chaowamalee, Atikhun Chotirattanachote, Wongsakorn Khammee, Chanoknun Kalvibool, Chawalit Ngamcharussrivichai
{"title":"Sustainable Production of 1-Propanol via the Selective Hydrogenolysis of Glycerol Over a Tailored Iridium–Rhenium Oxide Catalyst Supported on HUSY Zeolite","authors":"Supphathee Chaowamalee,&nbsp;Atikhun Chotirattanachote,&nbsp;Wongsakorn Khammee,&nbsp;Chanoknun Kalvibool,&nbsp;Chawalit Ngamcharussrivichai","doi":"10.1002/cctc.202500885","DOIUrl":"10.1002/cctc.202500885","url":null,"abstract":"<p>1-Propanol (1-PO) is a widely used industrial solvent and an important chemical intermediate. In this study, the hydrogenolysis of glycerol to 1-PO was investigated over conventional proton-form ultrastable (HUSY) zeolite, monometallic Ir-loaded HUSY (Ir-HUSY), and Ir–ReO<sub>x</sub> metal–metal oxide supported on HUSY (IrRe-HUSY). The IrRe-HUSY catalysts, which were prepared via a sequential two-step incipient wetness impregnation method, exhibited favorable physicochemical properties, including improved acid properties and uniform metal dispersion. Therefore, the bimetallic IrRe-HUSY catalysts demonstrated a considerably higher catalytic performance, achieving a glycerol conversion of 78.9% and 1-PO yield of 39.2%, than HUSY zeolite and Ir-HUSY, which demonstrated only 32.9% glycerol conversion and 11.1% 1-PO yield. This improvement in the catalytic properties of the IrRe-HUSY catalysts was attributed to the synergistic effects among the three catalyst components: (1) ReO<sub>x</sub> clusters facilitated glycerol adsorption and activation; (2) Ir nanoparticles promoted C─O bond cleavage and hydrogenation; and (3) the acidic HUSY support enhanced dehydration steps. Additionally, the effects of operating conditions, such as catalyst loading, reaction time, and temperature, on 1-PO production were systematically investigated. The surface structure of IrRe-HUSY and the mechanistic pathway for glycerol hydrogenolysis over the IrRe-HUSY catalyst were elucidated.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 17","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144999150","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Tunable Morphologies of Fe-Embedded Cr-MOF Derived Catalyst for Efficient CO2 Hydrogenation 含铁Cr-MOF衍生的高效CO2加氢催化剂的可调形貌
IF 3.9 3区 化学
ChemCatChem Pub Date : 2025-07-27 DOI: 10.1002/cctc.202500784
Swarit Dwivedi, Vignesh Pakkiam, Rajan Lakshman, Sanje Mahasivam, Malgorzata Kowalik, Alan L. Chaffee, Adri C.T. van Duin, Akshat Tanksale, Nikhil V. Medhekar
{"title":"Tunable Morphologies of Fe-Embedded Cr-MOF Derived Catalyst for Efficient CO2 Hydrogenation","authors":"Swarit Dwivedi,&nbsp;Vignesh Pakkiam,&nbsp;Rajan Lakshman,&nbsp;Sanje Mahasivam,&nbsp;Malgorzata Kowalik,&nbsp;Alan L. Chaffee,&nbsp;Adri C.T. van Duin,&nbsp;Akshat Tanksale,&nbsp;Nikhil V. Medhekar","doi":"10.1002/cctc.202500784","DOIUrl":"10.1002/cctc.202500784","url":null,"abstract":"<p>We report a stable MOF-derived bimetallic FeCrC<i><sub>x</sub></i> catalyst for heterogeneous catalytic reactions. Using ReaxFF molecular dynamics, we uncover the atomistic pathways that drive the thermal conversion of MIL-101(Cr) and its Fe-loaded analogue. The presence of iron in the framework lowers its stability, resulting in higher mass loss and fragmentation of the aromatic linkers during thermal transformation. Our simulations predict the formation of highly dispersed Fe─Cr core-shell nanoparticles with a Cr core when transformed at high temperatures. However, our simulations show that Fe nanoparticles are embedded in a chromium-carbon matrix at lower temperatures. This MIL-101(Cr)-derived FeCrC<i><sub>x</sub></i> (Fe and Cr embedded in a residual carbon-rich environment) catalyst was then experimentally prepared and demonstrated activity in the aqueous phase for CO<sub>2</sub> hydrogenation to methanol. Significantly, the MOF-derived FeCrC<i><sub>x</sub></i> catalyst transformed at 500 °C showed approximately five times better yield than the catalyst treated at 400 °C, which we attribute to the Fe─Cr core-shell particles in the former. We are confident that our integrated computational-experimental strategy will accelerate the discovery of MOF-derived bimetallic catalysts and unlock their potential in a broad spectrum of applications.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 18","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/cctc.202500784","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145102361","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Sustainable Strategies for Fixation of CO2 into Valuable Chemicals Catalyzed by Functionalized Porous Materials 功能化多孔材料催化二氧化碳转化为有价化学品的可持续策略
IF 3.9 3区 化学
ChemCatChem Pub Date : 2025-07-27 DOI: 10.1002/cctc.202500807
Dr. Debarati Chakraborty, Dr. Arindam Modak, Prof. Asim Bhaumik
{"title":"Sustainable Strategies for Fixation of CO2 into Valuable Chemicals Catalyzed by Functionalized Porous Materials","authors":"Dr. Debarati Chakraborty,&nbsp;Dr. Arindam Modak,&nbsp;Prof. Asim Bhaumik","doi":"10.1002/cctc.202500807","DOIUrl":"10.1002/cctc.202500807","url":null,"abstract":"<p>Bulk scale utilization of CO<sub>2</sub> as C1 feedstock is very demanding not only from the environmental perspective, but it is very challenging for addressing the global energy crisis, carbon recycling, and sustainability. Functionalized porous materials having CO<sub>2</sub> adsorption sites and large internal surface areas are the ideal candidates for catalyzing the fixation of CO<sub>2</sub> into fuels and commodity chemicals. In this review we have highlighted the advancements made in designing different class of microporous and mesoporous materials (zeolites, mesoporous materials, MOFs, COFs, POPs, metal phosphonates, etc.) over the years for the synthesis of cyclic carbonates, polycarbonates, carbamates, <i>N</i>-formylated amines, polyhydroxyurethanes, ureas, imidazoles, and related heterocyclic compounds through CO<sub>2</sub> fixation reactions. Further, direct CO<sub>2</sub> reduction to methanol, dimethyl ether (DME), formic acid, ethanol, etc. are particularly important in the context of renewable energy. We have discussed the catalytic role of different class of porous nanomaterials for understanding the promotional role of the reactive sites in catalyzing these CO<sub>2</sub> conversion reactions. Mechanistic aspects of these chemical transformations are illustrated with a major emphasis on the key factors affecting the CO<sub>2</sub> and substrate activation processes. Finally, the challenges faced by the researchers in achieving the desired targets in these CO<sub>2</sub> conversion reactions are highlighted, which could contribute significantly in carbon recycling in the future.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 17","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144999117","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Advances and Perspectives of Mild Thermal Treatment Strategy in Covalent/Metal-Organic Frameworks Derived Porous Catalysts 共价/金属-有机骨架衍生多孔催化剂温和热处理策略的研究进展与展望
IF 3.9 3区 化学
ChemCatChem Pub Date : 2025-07-27 DOI: 10.1002/cctc.202401981
Jinyan Wang, Huimin Sun, Yu Wu, Hailong Hu, Fang Duan, Mingliang Du, Shuanglong Lu
{"title":"Advances and Perspectives of Mild Thermal Treatment Strategy in Covalent/Metal-Organic Frameworks Derived Porous Catalysts","authors":"Jinyan Wang,&nbsp;Huimin Sun,&nbsp;Yu Wu,&nbsp;Hailong Hu,&nbsp;Fang Duan,&nbsp;Mingliang Du,&nbsp;Shuanglong Lu","doi":"10.1002/cctc.202401981","DOIUrl":"10.1002/cctc.202401981","url":null,"abstract":"<p>Mild thermal treatment (MTT) strategy is an emerging method for designing covalent/metal-organic frameworks (COFs/MOFs) derived porous catalysts, which can not only maintain their unique porous and periodic structures but also endow them with new properties. This review systematically examines the recent advancements in deriving materials from COFs/MOFs via MTT strategy. The discussion encompasses various types of derivatives, including framework-carbon composites, framework-metal nanoparticle hybrids, and mesoporous structures. These materials demonstrate notable advantages in catalysis, such as enhanced electrical conductivity, improved structural stability, and the incorporation of abundant active sites, which collectively contribute to their superior catalytic performance. Furthermore, we critically analyze the structural and functional enhancements enabled by these derivatives, emphasizing their contributions to advancing catalytic applications. In addition, we propose future research directions, including elucidating the mechanisms underlying material transformations during thermal treatment, diversifying catalyst design strategies, and establishing precise structure–performance relationships. These insights aim to provide a comprehensive understanding of the interplay between catalyst structures and their functionalities, thereby guiding the rational design of next-generation catalytic materials.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 15","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145135738","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 and Reactivity of AgCu/SiO2 Bimetallic Catalysts for Alkene Epoxidation 烯烃环氧化AgCu/SiO2双金属催化剂的结构和反应性
IF 3.9 3区 化学
ChemCatChem Pub Date : 2025-07-27 DOI: 10.1002/cctc.202500921
Yogita Soni, Seth March, Steven L. Suib, E. Charles H. Sykes, Prashant Deshlahra
{"title":"Structure and Reactivity of AgCu/SiO2 Bimetallic Catalysts for Alkene Epoxidation","authors":"Yogita Soni,&nbsp;Seth March,&nbsp;Steven L. Suib,&nbsp;E. Charles H. Sykes,&nbsp;Prashant Deshlahra","doi":"10.1002/cctc.202500921","DOIUrl":"10.1002/cctc.202500921","url":null,"abstract":"<p>AgCu bimetallic materials have attracted significant interest as catalysts for selective oxidation reactions. Near-surface alloys of Ag on Cu have been shown to activate O<sub>2</sub> efficiently at exposed reverse-segregated isolated Cu atoms within the surface Ag layers. This study focuses on the synthesis of nanoparticle analogs of these alloys and measurement of their performance for ethylene and propylene epoxidation. Supported Cu/SiO<sub>2</sub> catalysts were prepared by strong electrostatic adsorption and partial galvanic replacement of Cu atoms with Ag cations in aqueous media, which led to bimetallic nanoparticles of 3–10 nm average size and 0.25–1.6 Ag:Cu atomic ratios. Galvanic exchange stoichiometry, elemental maps and UV–vis spectroscopy reveal coexistence of Ag and Cu in the nanoparticles. Diffuse reflectance infrared spectra of bound CO indicate the formation of nanoparticles with a Cu core and Ag shell when catalysts with high Ag:Cu ratios are reduced to metallic form. The bimetallic catalysts show improvement over monometallic Ag and Cu and their physical mixtures, exhibiting higher rates, higher initial selectivity than Ag, and resistance to secondary reactions that decrease the selectivity of Cu catalysts at higher alkene conversion. These results demonstrate a simple synthesis method of more selective bimetallic AgCu nanoparticles with core-shell like structures, which may be of use in a variety of selective oxidation reactions.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 18","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145102360","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
H2O2 Suppression During Oxygen Reduction Using Mixed Metal Oxides 混合金属氧化物对氧还原过程中H2O2的抑制作用
IF 3.9 3区 化学
ChemCatChem Pub Date : 2025-07-27 DOI: 10.1002/cctc.202500886
Sekhar Kumar Biswal, Chinmoy Ranjan
{"title":"H2O2 Suppression During Oxygen Reduction Using Mixed Metal Oxides","authors":"Sekhar Kumar Biswal,&nbsp;Chinmoy Ranjan","doi":"10.1002/cctc.202500886","DOIUrl":"10.1002/cctc.202500886","url":null,"abstract":"<p>The development of efficient and selective oxygen reduction reaction (ORR) catalysts is central to advancing electrochemical energy technologies. While platinum remains the benchmark, its high cost, peroxide selectivity, and durability issues demand alternatives. Transition metal oxides (TMOs) are promising in alkaline media, yet their ORR activity is hampered by weak oxygen binding and high activation barriers. This concept article introduces a coordination mismatch strategy to enhance ORR performance in mixed-metal oxides, specifically Cu[M]O<sub>x</sub> (M═Co, Ni, Fe, Mn). By combining metals with differing oxygen coordination preferences, Cu<sup>2+</sup> (four-fold) and M<sup>n+</sup> (typically six-fold), local lattice strain and undercoordinated sites are introduced, enhancing O<sub>2</sub> adsorption and O─O bond cleavage. Cu-rich compositions, especially Cu<sub>0.8</sub>Co<sub>0.2</sub>O<sub>x</sub>/Au, demonstrate high ORR activity, low H<sub>2</sub>O<sub>2</sub> yield, and excellent stability. In situ Raman spectroscopy confirms stable M─O─Cu frameworks and redox-active Cu centers. The approach is validated across multiple dopants and supported by DFT studies showing stabilized OOH* intermediates and favorable energetics. These findings demonstrate that coordination engineering is a powerful strategy for designing efficient, selective, and robust nonprecious metal catalysts for electrochemical energy conversion.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 15","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145135737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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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