Catalysis Science & Technology最新文献

{"title":"Selective hydrogenation of nitroaromatics catalyzed by surface Pt-rich high-entropy alloy catalysts at room temperature†","authors":"Mingzhen Li ,&nbsp;Yongsheng Li ,&nbsp;Zekun Jing ,&nbsp;Deshun Huang ,&nbsp;Guozong Yue ,&nbsp;Yakun Guo ,&nbsp;Maobing Shuai","doi":"10.1039/d4cy01542h","DOIUrl":"10.1039/d4cy01542h","url":null,"abstract":"<div><div>The selective hydrogenation of nitroaromatics is a promising and environmentally friendly method for synthesizing the chemical intermediates of functionalized aromatic amines. However, achieving room-temperature hydrogenation remains a formidable challenge. In this study, we prepared a high-entropy alloy (HEA) catalyst with a similar core–shell structure, with a Pt-rich HEA as the shell and a CuNi-rich HEA as the core. This catalyst enables 100% conversion and selectivity for the hydrogenation of <em>p</em>-chloronitrobenzene under ambient temperature, in both solvent-involved and solvent-free systems. Additionally, it exhibits excellent stability, recyclability, and versatility. Furthermore, heat treatment-induced disruption of the Pt-rich surface structure leads to significant reduction in catalytic activity or even deactivation due to the migration of surface Pt atoms towards the interior of the alloy. These findings highlight the crucial role played by the Pt-rich surface structure in attaining outstanding performance in nitroaromatic hydrogenation. This work offers novel insights and strategies for designing efficient catalysts tailored specifically for selective nitroaromatic hydrogenation.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2369-2378"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740511","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}

{"title":"Monolithic wood-based carbon supported Pd nanoparticles with tunable exposure for boosting semi-hydrogenation of alkynols†","authors":"Cheng-Long Li ,&nbsp;Rui-Ping Zhang ,&nbsp;Lu Hou ,&nbsp;Ya-Dong Xie ,&nbsp;An-Hui Lu","doi":"10.1039/d4cy01543f","DOIUrl":"10.1039/d4cy01543f","url":null,"abstract":"<div><div>The selective hydrogenation of alkynols to enols catalyzed by carbon-supported Pd catalysts is a highly attractive reaction for the production of fine chemicals. However, the limited dispersion and stability of Pd species on the carbon support often hindered their catalytic activity. In this study, we developed a “carbon-layer anchored” method to synthesize Pd@NMC monolithic catalysts with tunable Pd exposure by the coating of nitrogen-containing polymer on the wood framework, followed by Pd loading, and carbonization procedures. The exposure of Pd nanoparticles can be controlled through a partial oxidation strategy. As a result, the semi-embedded Pd catalyst (Pd@NMC-250) exhibited superior activity and selectivity (91%) in the semi-hydrogenation of 2-methyl-3-butyn-2-ol (MBY). The reaction rate can reach 5110 mol mol_Pd⁻¹ h⁻¹, which is 4.5-fold higher than that of the commercial Lindlar catalyst under identical conditions (308 K, 5 bar H₂). Moreover, the monolithic catalyst presented good stability for enduring five cycles. The nitrogen species in the support and the carbon layer deposited on Pd nanoparticles during pyrolysis synergistically promote the Pd anchoring. After mild oxidation, the carbon layer is partially removed to form a semi-embedded Pd@C nanostructure, with the surface exposed and the bottom embedded on the carbon support, which enhances the stability. Furthermore, the monolithic wood-based carbon catalysts are easy to separate from the solution and thus have the potential for operating a variety of liquid-phase catalytic reactions beyond hydrogenation.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2238-2247"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740433","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}

{"title":"Unveiling the origin of high catalytic activity of WO3/MWCNT nanocomposites for the hydrogen evolution reaction†","authors":"Nitesh Dogra ,&nbsp;Sunil Singh Kushvaha ,&nbsp;Avijit Dewasi ,&nbsp;Sandeep Sharma","doi":"10.1039/d4cy01524j","DOIUrl":"10.1039/d4cy01524j","url":null,"abstract":"<div><div>The electrocatalytic performance of the hydrogen evolution reaction (HER) largely relies on lower Tafel slope and overpotential values. WO₃-based composites have emerged as one of the most promising electrocatalysts for the HER. Here, we report a facile two-step synthesis method for WO₃ and multi-walled carbon nanotube (MWCNT) composites with variable content of MWCNTs. The optimal integration of MWCNTs with oxygen vacancy-enriched WO₃ provides abundant active sites and better conductivity beneficial for the HER. The analysis reveals that the HER follows a Volmer and Heyrovsky reaction process. Composite formation and the presence of oxygen vacancies in WO₃ were confirmed through various characterization techniques. The optimized composite exhibited the lowest overpotential (<em>η</em>₁₀ = 0.2 V) and Tafel slope (70 mV dec⁻¹ and 85 mV dec⁻¹, before and after performing the stability test). This work provides a valuable insight into the understanding of the structure–HER activity relationship in WO₃/MWCNT composite-based electrocatalysts.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2327-2338"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740508","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}

{"title":"MOF-derived single-atom catalysts with dense zinc and nitrogen sites for efficient CO2 cycloaddition†","authors":"Zhijun Huang ,&nbsp;Jie Wu ,&nbsp;Fengwen Yan ,&nbsp;Guoqing Yuan","doi":"10.1039/d4cy01534g","DOIUrl":"10.1039/d4cy01534g","url":null,"abstract":"<div><div>ZIF-8 derived Zn single-atom catalysts (SACs) bearing both acidic Zn and basic N sites are active for the cycloaddition of CO₂ with epoxides. However, their low Zn and N contents limit their catalytic activities. Herein, Zn SACs with dense N and Zn sites (hZn SAC-N) are prepared from ZIF-8 using zinc powder and melamine as the extra Zn and N sources, respectively. The Zn loading and N/C ratio are 15.12 wt% and 0.289, much higher than those of the Zn SAC obtained from ZIF-8 alone (5.11 wt% and 0.233). The catalytic activity of hZn SAC-N improves 2.55 times due to the abundant Zn and N sites. A much better catalytic stability of hZn SAC-N than that of ZIF-8 is also confirmed due to the highly stable carbonaceous single-atom structure. Our finding provides a useful strategy for enriching the active sites of SACs for various applications.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2286-2294"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740437","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}

{"title":"Progress in catalytic strategies for mitigating NOx/N2O emissions: from mechanisms to applications","authors":"Minfan Qian ,&nbsp;Bin Guan ,&nbsp;Zhongqi Zhuang ,&nbsp;Junyan Chen ,&nbsp;Lei Zhu ,&nbsp;Zeren Ma ,&nbsp;Xuehan Hu ,&nbsp;Chenyu Zhu ,&nbsp;Sikai Zhao ,&nbsp;Kaiyou Shu ,&nbsp;Hongtao Dang ,&nbsp;Tiankui Zhu ,&nbsp;Zhen Huang","doi":"10.1039/d4cy01416b","DOIUrl":"10.1039/d4cy01416b","url":null,"abstract":"<div><div>In the context of global warming, the emission of the greenhouse gas nitrous oxide (N₂O) is an important factor limiting the application of ammonia fuels in marine and offshore power. The effective control of N₂O emissions by suppressing N₂O generation at the source and after-treatment of exhaust gases has a highly urgent practical significance. The primary source of N₂O in ammonia-fueled engines is the side reaction in aftertreatment process of nitrogen oxides (NO_<em>x</em>)—selective catalytic reduction (SCR). SCR is also an up-and-coming N₂O aftertreatment technology, so developing highly efficient N₂O-inhibiting NO_<em>x</em>-SCR catalysts and N₂O-SCR catalysts is the key to emission control. This article innovatively provides a detailed review of the principles and influencing factors of these two types of catalysts, respectively. Firstly, the generation mechanism of N₂O in the NO_<em>x</em>-SCR process with several common reducing agents is reviewed, and then the influencing factors of the catalyst performance are classified, the development and optimization of N₂O-SCR catalysts in recent years are reviewed, such as improving the structure of the catalyst. Then, the mechanism of N₂O-SCR with different reducing agents is reviewed, and the influencing factors and optimization methods of N₂O-SCR catalysts are classified and reviewed, such as adjusting the catalyst preparation conditions, changing the active component loading to increase the acidic center. Finally, some suggestions and outlooks for future research directions are presented. It is hoped that this paper can provide a theoretical basis for developing efficient catalysts adapted to industrial applications and contribute to the control of N₂O emissions.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2061-2103"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740465","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}

{"title":"Selective isomerization of β-pinene: a sustainable method for total utilization of turpentine as a biomass resource†","authors":"Robert E. Munday ,&nbsp;Ryan Z. Whitehead ,&nbsp;Elsa Iacono ,&nbsp;Philippa L. Jacob ,&nbsp;Steven M. Howdle ,&nbsp;Gary M. Walker ,&nbsp;Vincenzo Taresco ,&nbsp;Anabel E. Lanterna","doi":"10.1039/d4cy01247j","DOIUrl":"10.1039/d4cy01247j","url":null,"abstract":"<div><div>Abundant and naturally available terpenes, such as α-pinene, are gaining attention as polymer building blocks, providing a biogenic source to replace fossil carbon feedstocks. However, α-pinene extraction from the natural source, turpentine, requires energy demanding and wasteful distillation processes. Here, we used a facile and green photocatalytic approach to obtain highly pure α-pinene, allowing total utilization of turpentine as a biomass resource.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2132-2137"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d4cy01247j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740467","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}

{"title":"Cu-catalyzed [1,3]-asymmetric methoxy rearrangement of N-methoxyanilines: mechanistic insight†","authors":"Kazuki Masukawa ,&nbsp;Amu Kojima ,&nbsp;Takuma Sato ,&nbsp;Masahiro Terada ,&nbsp;Itaru Nakamura","doi":"10.1039/d5cy00106d","DOIUrl":"10.1039/d5cy00106d","url":null,"abstract":"<div><div>Cu-catalyzed reactions of <em>N</em>-methoxy-2,6-dimethylanilines in the presence of a cationic Cu catalyst ligated to a chiral NHC ligand, which has an (<em>ortho</em>-carbamoyl)phenyl group on the nitrogen atom of (<em>S</em>,<em>S</em>)-diphenylimidazolidinylidene, furnished chiral <em>ortho</em>-quinol imines with good enantioselectivity. In addition, a cascade reaction involving the [1,3]-methoxy rearrangement followed by the Diels–Alder reaction yielded the corresponding three-dimensional molecules in a diastereo- and enantioselective manner.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2138-2142"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d5cy00106d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740468","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}

{"title":"Enhanced coking-resistance of Ca- and Mg-incorporated Mo/V montmorillonite-supported catalysts during gas-phase glycerol conversion to allyl alcohol†","authors":"Da Jian Li ,&nbsp;Alfin Kurniawan ,&nbsp;Tania Roy ,&nbsp;Jin Wang ,&nbsp;Cheng Lan Liu ,&nbsp;Ze Zhen Wang ,&nbsp;Rong Zhen Mu ,&nbsp;Chun Hui Zhou","doi":"10.1039/d4cy01300j","DOIUrl":"10.1039/d4cy01300j","url":null,"abstract":"<div><div>The efficient production of allyl alcohol from glycerol is of great importance due to its significance as a valuable intermediate in chemical industries. During the catalytic conversion of glycerol to allyl alcohol by solid acid catalysts, carbon deposition (coking) is prone to occur on the catalyst surface, leading to slowing of the conversion process and fast deactivation of the catalyst. In this study, we obtained an efficient catalyst for the preparation of allyl alcohol from gas-phase glycerol by controlling the pore structure and surface acidity of the catalyst. The characterization results showed that hydrochloric acid and citric acid removed the silicon and aluminium elements from montmorillonite. Additionally, the acidity, pore volume, and surface area ratio of Na-MMT (<em>S</em>_BET = 34.5 m² g⁻¹, <em>V</em>_T = 0.19 cm³ g⁻¹) were all found to be improved in porous montmorillonite (HA₁MMT) catalyst (<em>S</em>_BET = 97.9 m² g⁻¹, <em>V</em>_T = 0.28 cm³ g⁻¹). After adding MoO_<em>x</em> and VO_<em>x</em>, the selectivity of the Mo/V-HA₁MMT catalyst for allyl alcohol was improved. XPS characterization results indicate that the synergistic effect of Mo and V can promote the transfer of electrons during the reaction process of glycerol conversion. Within 480 min of catalyzing the glycerol dehydration reaction, Mo_0.6V_0.4(5)-HA₁MMT was almost deactivated (conv. = 19.5%, sel._{allyl alcohol} = 31.2%) due to carbon deposition. When the catalyst was doped with calcium and magnesium components, a new active phase CaMo₄ was discovered on the catalyst, and the acidity of Ca_0.5Mg_0.5-Cat. (Cat. is Mo_0.6V_0.4(5)-HA₁MMT) decreased to 214.0 μmol g⁻¹. The coking-resistance performance of Ca_0.5Mg_0.5-Cat. was improved, and after 660 min of reaction, the catalyst was deactivated (conv. = 32.1%, sel._{allyl alcohol} = 30.1%) due to carbon deposition. During the 3rd catalyst regeneration test, Ca_0.5Mg_0.5-Cat. still maintained high activity (conv.= 63.3%, sel._{allyl alcohol} = 35.2%, sel._acrolein = 31.2%). These results indicate that suitable pore structure and acidity are crucial for designing a catalyst with coking-resistance properties.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2339-2352"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740509","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}

{"title":"Phenylcarbazole-stabilized palladium catalysts for efficient acetylene hydrochlorination†","authors":"Shahid Ali ,&nbsp;Lu Wang ,&nbsp;Haijun Yan ,&nbsp;Lei Dang ,&nbsp;Chao Yang ,&nbsp;Jide Wang ,&nbsp;Hui Sun ,&nbsp;Xiaofei Li ,&nbsp;Ronglan Wu ,&nbsp;Changhai Liang","doi":"10.1039/d4cy01414f","DOIUrl":"10.1039/d4cy01414f","url":null,"abstract":"<div><div>9-Phenylcarbazole (PCz) was employed to synthesize Pd-based/SAC catalysts using an ultrasonic-assisted impregnation method for acetylene hydrochlorination. The catalytic performance of the Pd–PCz/SAC catalysts was investigated, and the Pd–15PCz/SAC catalyst achieved 99.9% C₂H₂ conversion and over 99% vinyl chloride monomer (VCM) selectivity, with negligible catalyst deactivation over 380 h. Characterization demonstrated that the addition of PCz effectively stabilized the active Pd(<span>ii</span>) particles, inhibited carbon deposition, and prevented the loss of active Pd species. Density functional theory (DFT) simulations further verified the positive effect of PCz modification on the Pd-based/SAC catalyst by altering the energy profiles of reaction pathways and the adsorption energies of reactants and products, thus enhancing catalytic efficiency.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2272-2285"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740436","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}

{"title":"Tunable synthesis of alcohols and aldehydes by reductive hydroformylation of alkenes over heterogeneous Co catalysts†","authors":"Wenting Zhang ,&nbsp;Xinjiang Cui ,&nbsp;Shujuan Liu ,&nbsp;Ce Liu ,&nbsp;Hongli Wang ,&nbsp;Feng Shi","doi":"10.1039/d4cy01527d","DOIUrl":"10.1039/d4cy01527d","url":null,"abstract":"<div><div>Hydroformylation of alkenes constitutes a substantial industrial catalytic process. Tunable synthesis of alcohols and aldehydes by hydroformylation is challenging in heterogeneous catalysis. Here, we describe the encapsulation of single-atom Co catalysts in a porous phosphine polymer for the tunable synthesis of alcohols and aldehydes in olefin hydroformylation. With the polymer encapsulated single atom Co₂(CO)₈@PPh₃-1/10 as the catalyst, almost complete conversion of 1-octene and a selectivity to alcohols of 94% at 170 °C while aldehydes with 87% yield was obtained at 140 °C, and was eco-friendly with a 100% atomic efficiency reaction and in line with principles of ‘green chemistry’. Various catalyst characterization methods including XRD, TEM, HADDF-STEM and <em>in situ</em> FT-IR spectroscopy showed that Co species were homogeneously distributed in the pores of PPh₃ and the formation of HCo(CO)_<em>x</em> as the catalytically active species was successful. This work provides meaningful insights into the development of non-noble metal heterogeneous catalysts for the selective hydroformylation reaction.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 7","pages":"Pages 2295-2302"},"PeriodicalIF":4.4,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143740438","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}