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Hydrogenation of perfluoroolefins catalyzed by palladium nanoparticles anchored on the layered carbon nitride† 层状氮化碳†上钯纳米颗粒催化全氟烯烃加氢反应
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2025-03-17 DOI: 10.1039/d5cy00105f
Peihong Zhang , Huiyao Yang , Liantao Jiang , Yaofeng Wang , Guliang Liu , Yanyan Diao , Chang Su , Hongyan Wang
{"title":"Hydrogenation of perfluoroolefins catalyzed by palladium nanoparticles anchored on the layered carbon nitride†","authors":"Peihong Zhang ,&nbsp;Huiyao Yang ,&nbsp;Liantao Jiang ,&nbsp;Yaofeng Wang ,&nbsp;Guliang Liu ,&nbsp;Yanyan Diao ,&nbsp;Chang Su ,&nbsp;Hongyan Wang","doi":"10.1039/d5cy00105f","DOIUrl":"10.1039/d5cy00105f","url":null,"abstract":"<div><div>Perfluoroolefins are extensively utilized in chip cooling applications under the “dual carbon” goals and due to the inherent requirements for green and sustainable development. Graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) serves as a crucial support material for loading precious metals. In this study, nitrogen atoms are doped into carbon as structural defects to enhance the interaction, resulting in highly dispersed palladium nanoparticles obtained through wet impregnation. The sub-nanometer scale dispersion of palladium is constructed in the “six-fold cavity” of g-C<sub>3</sub>N<sub>4</sub>, due to the presence of cyano groups in the structure. The strong Pd–N interaction ensures that Pd nanoparticles are highly dispersed on g-C<sub>3</sub>N<sub>4</sub>. The interfacial synergistic effect between the Pd NPs and g-C<sub>3</sub>N<sub>4</sub> facilitates effective adsorption and activation of H<sub>2</sub> on Pd/g-C<sub>3</sub>N<sub>4</sub>, thereby promoting hydrogenation reactions and improving catalytic performance. Palladium atoms are fully utilized at low loadings, resulting in enhanced catalytic activity and stability. Experimental results demonstrate that Pd-DCN exhibits optimal catalytic performance for the hydrogenation of perfluoroolefins at a palladium loading of 0.1 wt%.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 9","pages":"Pages 2919-2927"},"PeriodicalIF":4.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143911810","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
Hydrogenation of perfluoroolefins catalyzed by palladium nanoparticles anchored on the layered carbon nitride† 层状氮化碳†上钯纳米颗粒催化全氟烯烃加氢反应
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2025-03-17 DOI: 10.1039/D5CY00105F
Peihong Zhang, Huiyao Yang, Liantao Jiang, Yaofeng Wang, Guliang Liu, Yanyan Diao, Chang Su and Hongyan Wang
{"title":"Hydrogenation of perfluoroolefins catalyzed by palladium nanoparticles anchored on the layered carbon nitride†","authors":"Peihong Zhang, Huiyao Yang, Liantao Jiang, Yaofeng Wang, Guliang Liu, Yanyan Diao, Chang Su and Hongyan Wang","doi":"10.1039/D5CY00105F","DOIUrl":"https://doi.org/10.1039/D5CY00105F","url":null,"abstract":"<p >Perfluoroolefins are extensively utilized in chip cooling applications under the “dual carbon” goals and due to the inherent requirements for green and sustainable development. Graphitic carbon nitride (g-C<small><sub>3</sub></small>N<small><sub>4</sub></small>) serves as a crucial support material for loading precious metals. In this study, nitrogen atoms are doped into carbon as structural defects to enhance the interaction, resulting in highly dispersed palladium nanoparticles obtained through wet impregnation. The sub-nanometer scale dispersion of palladium is constructed in the “six-fold cavity” of g-C<small><sub>3</sub></small>N<small><sub>4</sub></small>, due to the presence of cyano groups in the structure. The strong Pd–N interaction ensures that Pd nanoparticles are highly dispersed on g-C<small><sub>3</sub></small>N<small><sub>4</sub></small>. The interfacial synergistic effect between the Pd NPs and g-C<small><sub>3</sub></small>N<small><sub>4</sub></small> facilitates effective adsorption and activation of H<small><sub>2</sub></small> on Pd/g-C<small><sub>3</sub></small>N<small><sub>4</sub></small>, thereby promoting hydrogenation reactions and improving catalytic performance. Palladium atoms are fully utilized at low loadings, resulting in enhanced catalytic activity and stability. Experimental results demonstrate that Pd-DCN exhibits optimal catalytic performance for the hydrogenation of perfluoroolefins at a palladium loading of 0.1 wt%.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 9","pages":" 2919-2927"},"PeriodicalIF":4.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143913702","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
Modulating *CO coverage via the pyrrolic-N content on carbon for enhanced electrocatalytic CO2 reduction to CO† 通过碳上的吡咯- n含量调节*CO覆盖,以增强电催化CO2还原为CO†
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2025-03-17 DOI: 10.1039/d5cy00100e
Fang Zhao , Yingzheng Zhang , Caiyue Wang , Jiatao Zhang , Di Zhao
{"title":"Modulating *CO coverage via the pyrrolic-N content on carbon for enhanced electrocatalytic CO2 reduction to CO†","authors":"Fang Zhao ,&nbsp;Yingzheng Zhang ,&nbsp;Caiyue Wang ,&nbsp;Jiatao Zhang ,&nbsp;Di Zhao","doi":"10.1039/d5cy00100e","DOIUrl":"10.1039/d5cy00100e","url":null,"abstract":"<div><div>The electrocatalytic CO<sub>2</sub> reduction reaction (eCO<sub>2</sub>RR) is a new energy technology that shows a feasible way to achieve carbon neutrality and to produce valuable fuels and feedstocks with effective electrocatalysts. Nitrogen-doped carbon (NC) materials have become the most promising carbon-based electrocatalysts to produce CO and potential metal carriers to produce multi-carbon products due to their low cost, high activity, and ability to enhance metal–carrier interactions. However, aiming at high selectivity of CO, it is important to optimize the competing coverage of *CO and *H on the NC working electrocatalyst surface. Here, for the first time, we controllably adjusted the pyrrolic-N content on NC <em>via</em> a simple strategy of pyrrolic-N-abundant phthalocyanine-assisted pyrolysis of a common MOF precursor (ZIF-8), which then modulated the *CO and *H coverage for enhanced electrocatalytic CO<sub>2</sub> reduction to CO with an FE<sub>CO</sub> value of above 92% at −0.6 V <em>vs.</em> RHE. Mechanistic studies showed that the high content of pyrrolic-N of Pr-a-NC induced the surface coverage of *CO to be much higher than that of the control samples. Meanwhile, under the conditions of high *CO coverage, adsorbed *CO intermediates combined with the active *H generated the high-coverage intermediate *COH, which is one of the most common intermediates to generate multi-carbon products. So, this work not only provides an effective strategy for the future rational design of carbon electrocatalysts to generate CO, but also opens an avenue to engineer carbon–nitrogen coordination substrate-loaded metal electrocatalysts for the production of multi-carbon products from the eCO<sub>2</sub>RR.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 9","pages":"Pages 2898-2907"},"PeriodicalIF":4.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143911879","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
Boosting visible light photocatalytic oxidation of CO using Au nanocatalysts through synergistic preparation of an Fe-doped TiO2 support and cold plasma treatment† 通过协同制备fe掺杂TiO2载体和冷等离子体处理,促进Au纳米催化剂可见光催化氧化CO
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2025-03-17 DOI: 10.1039/d4cy01550a
Tong Xu , Bangyou Jia , Kaiwei Yan , Chenlong Wang , Bin Zhu , Xiaosong Li
{"title":"Boosting visible light photocatalytic oxidation of CO using Au nanocatalysts through synergistic preparation of an Fe-doped TiO2 support and cold plasma treatment†","authors":"Tong Xu ,&nbsp;Bangyou Jia ,&nbsp;Kaiwei Yan ,&nbsp;Chenlong Wang ,&nbsp;Bin Zhu ,&nbsp;Xiaosong Li","doi":"10.1039/d4cy01550a","DOIUrl":"10.1039/d4cy01550a","url":null,"abstract":"<div><div>TiO<sub>2</sub>-supported Au nanocatalysts are highly attractive for visible light photocatalysis owing to their efficient surface plasmon resonance (SPR) and superior intrinsic catalytic activity. The prevailing strategies to prepare high-performance plasmonic Au/TiO<sub>2</sub> include constructing highly active Au–TiO<sub>2</sub> interfaces by modulating the electronic and geometric properties of Au nanoparticles or the TiO<sub>2</sub> support. Herein, we report a synergism of an Fe-doped TiO<sub>2</sub> (Fe@TiO<sub>2</sub>) support and cold plasma treatment for the preparation of an Au/Fe@TiO<sub>2</sub>–P catalyst, enabling this Au nanocatalyst to outperform samples fabricated <em>via</em> classical methods for the visible light photocatalytic oxidation of CO. The key to this collaborative preparation is treating the Au species on Fe@TiO<sub>2</sub> derived from hydrothermal synthesis with cold plasma, which constructs large numbers of Au–Fe@TiO<sub>2</sub> interfaces by generating unique interactions between Au nanoparticles and the support. The Au/Fe@TiO<sub>2</sub>–P catalyst features high dispersion of Au and abundant surface oxygen species, thus accelerating the visible light photocatalytic oxidation of CO along the hot-electron transfer reaction pathway. This investigation demonstrates a promising approach to design and construct high-performance supported Au nanocatalysts for visible light photocatalysis.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 9","pages":"Pages 2844-2851"},"PeriodicalIF":4.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143911881","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
Regulating Ni2P electronic structure and morphology with cobalt: a one-step route to enhanced electrocatalytic urea oxidation and water splitting† 用钴调节Ni2P电子结构和形态:一步法增强电催化尿素氧化和水分解†
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2025-03-17 DOI: 10.1039/d5cy00008d
Peng Zhang , Fozia Sultana , Tongtong Li , Xiaojun Qin , Meijie Shi , Tong Wei , Kaicheng Qian , Mingwu Tan , Zhixue Li , Jianming Bai , Renhong Li
{"title":"Regulating Ni2P electronic structure and morphology with cobalt: a one-step route to enhanced electrocatalytic urea oxidation and water splitting†","authors":"Peng Zhang ,&nbsp;Fozia Sultana ,&nbsp;Tongtong Li ,&nbsp;Xiaojun Qin ,&nbsp;Meijie Shi ,&nbsp;Tong Wei ,&nbsp;Kaicheng Qian ,&nbsp;Mingwu Tan ,&nbsp;Zhixue Li ,&nbsp;Jianming Bai ,&nbsp;Renhong Li","doi":"10.1039/d5cy00008d","DOIUrl":"10.1039/d5cy00008d","url":null,"abstract":"<div><div>The effectiveness of electrochemical hydrogen production is predominantly impeded by the slow kinetics associated with the anodic oxygen evolution reaction (OER). Nevertheless, the method of urea-assisted energy-efficient alkaline hydrogen production has surfaced as a viable alternative strategy. In this study, a highly efficient Ni<sub>2</sub>P/NiCoP/NF electrocatalyst, featuring a unique combination of nanosheet and nanoneedle structures, is fabricated by fine-tuning the synthesis process. When employed as a catalyst, Ni<sub>2</sub>P/NiCoP/NF demonstrated exceptional catalytic efficiency, achieving a current density of 100 mA cm<sup>−2</sup> at a notably low potential of 1.31 V (<em>vs.</em> RHE) in the urea oxidation reaction (UOR). Notably, this potential was 210 mV lower than that required for the OER. Moreover, the system demonstrated excellent stability, maintaining a stable performance for over 36 hours. Theoretical calculations suggested that cobalt incorporation could facilitate the relocation of the d band center of Ni<sub>2</sub>P/NiCoP/NF towards the Fermi level, thereby enhancing electron transport efficiency. This adjustment enhanced the electron transport and increased urea adsorption, thereby accelerating the urea oxidation reaction (UOR). Scanning electron microscopy (SEM) analysis revealed a highly uniform and well-distributed nanostructure, whereas electrochemical measurements indicated significant enhancement in performance. Both of these outcomes directly resulted from the precise control of the synthesis parameters. This study showcases the successful integration of hybrid structure formation and morphology control strategies to design cost-effective catalysts for electrochemical conversion processes, thereby offering a sustainable and environmentally friendly approach towards energy-efficient hydrogen production.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 9","pages":"Pages 2733-2744"},"PeriodicalIF":4.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143911885","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
Selective hydrogenolysis of furfuryl alcohol towards 1,5-pentanediol over a Co/CeO2 catalyst† Co/CeO2催化剂上糠醇选择性氢解制备1,5-戊二醇的研究
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2025-03-17 DOI: 10.1039/d5cy00077g
Chen Cao , Fei Liu , Lin Li , Xiaoli Pan , Weixiang Guan , Aiqin Wang , Tao Zhang
{"title":"Selective hydrogenolysis of furfuryl alcohol towards 1,5-pentanediol over a Co/CeO2 catalyst†","authors":"Chen Cao ,&nbsp;Fei Liu ,&nbsp;Lin Li ,&nbsp;Xiaoli Pan ,&nbsp;Weixiang Guan ,&nbsp;Aiqin Wang ,&nbsp;Tao Zhang","doi":"10.1039/d5cy00077g","DOIUrl":"10.1039/d5cy00077g","url":null,"abstract":"<div><div>The selective hydrogenolysis of C–O bonds in furfuryl alcohol (FFA) into high-value pentanediols is of great significance to the production of bio-based polyesters and polyurethanes. Herein, a supported 5Co/CeO<sub>2</sub> catalyst was designed to facilitate the selective conversion of FFA to 1,5-pentanediol (1,5-PeD). Complete conversion of FFA was achieved within 1 h at 170 °C and 4 MPa H<sub>2</sub>, with a 54% selectivity to 1,5-PeD. The production rate reached 13 mol<sub>1,5-PeD</sub> mol<sub>Co</sub><sup>−1</sup> h<sup>−1</sup>, the highest value reported so far. The kinetic studies revealed that the reaction rate had a first order dependence on both hydrogen pressure and FFA concentration, with an apparent activation energy of 76 kJ mol<sup>−1</sup>. Characterization using H<sub>2</sub>-TPR, H<sub>2</sub>-TPD, and XPS revealed that compared with 5Co/MgO and 5Co/ZrO<sub>2</sub>, the 5Co/CeO<sub>2</sub> catalyst had the highest Co<sup>0</sup>/Co<sup>2+</sup> ratio (0.69) and abundant oxygen vacancies. Moreover, the oxygen vacancy concentration increased with the reduction temperature of 5Co/CeO<sub>2</sub>, and linearly correlated with the reaction rate. Raman, FFA-DRIFTS, and substrate control experiments showed that FFA was adsorbed on oxygen vacancies with both the furan oxygen and hydroxyl oxygen atoms. This unique adsorption mode facilitated the ring opening reactions. Co<sup>0</sup> was responsible for hydrogen activation while the oxygen vacancies from both the interfacial Co<sup>2+</sup> and CeO<sub>2</sub> were responsible for FFA adsorption. The good synergy between the Co<sup>0</sup> and the adjacent oxygen vacancies allows the efficient conversion of FFA to 1,5-PeD. This study provides a useful guideline for the design of non-precious metal catalysts for upgrading other biomass-derived molecules <em>via</em> selective hydrogenolysis of C–O bonds.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 9","pages":"Pages 2928-2937"},"PeriodicalIF":4.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143911890","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
Cross-linked Mg–porphyrin polymer as an efficient heterogeneous photocatalyst for the cycloaddition of aziridines with CO2 under ambient conditions† 交联镁卟啉聚合物作为一种高效的非均相光催化剂,在环境条件下与CO2环加成偶氮吡啶
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2025-03-17 DOI: 10.1039/d5cy00089k
Sushanta Kumar Meher , Sunil Roul , Krishnan Venkatasubbaiah
{"title":"Cross-linked Mg–porphyrin polymer as an efficient heterogeneous photocatalyst for the cycloaddition of aziridines with CO2 under ambient conditions†","authors":"Sushanta Kumar Meher ,&nbsp;Sunil Roul ,&nbsp;Krishnan Venkatasubbaiah","doi":"10.1039/d5cy00089k","DOIUrl":"10.1039/d5cy00089k","url":null,"abstract":"<div><div>The conversion of CO<sub>2</sub> to value-added chemical products is one of the hottest scientific topics that is receiving considerable interest. Oxazolidinone, a product derived from CO<sub>2</sub>, has received widespread attention due to its potential applications in the preparation of natural products. Here, we report a new heterogeneous polymer-supported magnesium–porphyrin as a photocatalyst for the conversion of CO<sub>2</sub> and aziridines to oxazolidinones under ambient conditions (room temperature and 1 atmosphere CO<sub>2</sub> pressure). We further studied the scope of oxazolidinone synthesis using various aziridines, and the catalyst was successfully reused several times.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 9","pages":"Pages 2706-2712"},"PeriodicalIF":4.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143911800","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
Activity enhancement of Ru/TiO2 catalysts for catalytic hydrogenation of amides to amines through controlling strong metal–support interactions† 通过控制强金属-载体相互作用增强Ru/TiO2催化剂酰胺加氢制胺活性
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2025-03-17 DOI: 10.1039/d5cy00073d
Shilong Zhao , Huaijun Ma , Wei Qu , Zhijian Tian
{"title":"Activity enhancement of Ru/TiO2 catalysts for catalytic hydrogenation of amides to amines through controlling strong metal–support interactions†","authors":"Shilong Zhao ,&nbsp;Huaijun Ma ,&nbsp;Wei Qu ,&nbsp;Zhijian Tian","doi":"10.1039/d5cy00073d","DOIUrl":"10.1039/d5cy00073d","url":null,"abstract":"<div><div>Efficient and selective catalytic hydrogenation of amides to amines is highly significant but extremely challenging. Here, a series of Ru/TiO<sub>2</sub> catalysts were prepared with the impregnation method at different calcination and reduction temperatures. Multiple characterization tools were used to characterize the physicochemical properties of the catalysts. The hydrogenation of butyramide to butylamine as a model reaction was used to evaluate the catalytic performance. The catalytic activity of the Ru catalyst supported on rutile TiO<sub>2</sub> was superior to that on anatase TiO<sub>2</sub>. As the calcination temperature increased from 200 °C to 600 °C, the catalytic performance of Ru/rutile catalysts monotonously decreased. With the reduction temperature increasing from 200 °C to 600 °C, Ru/rutile catalysts displayed a volcano-like trend of catalytic activity. The Ru/rutile catalyst calcined at 200 °C and reduced at 500 °C exhibited the highest catalytic performance, with 93% butyramide conversion and 65% selectivity to butylamine at 150 °C with 5 MPa H<sub>2</sub>. The evaluation and characterization results suggested that the lattice match between RuO<sub>2</sub> and rutile TiO<sub>2</sub> prevented Ru particle aggregation under high-temperature calcination, and smaller Ru particles were in favor of the amide hydrogenation reaction. The coverage of the TiO<sub><em>x</em></sub> overlayer on Ru nanoparticles and the Ru–TiO<sub><em>x</em></sub> boundary perimeter were effectively modulated by the strong metal–support interaction under different catalyst reduction temperatures, resulting in the optimization of the amide hydrogenation reactivity over Ru/rutile catalysts. This study facilitates the understanding of the influence of strong metal–support interaction on the catalytic hydrogenation of amide.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 9","pages":"Pages 2852-2866"},"PeriodicalIF":4.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143911680","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
Deactivation mechanisms and mitigation strategies for nickel-based acetylene semi-hydrogenation catalysts† 镍基乙炔半加氢催化剂失活机理及缓减策略
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2025-03-17 DOI: 10.1039/d5cy00098j
Yi Miao , Shuzhe Zheng , Jiaqi Qi , Mingyi Xiao , Mingwu Tan , Zhongting Hu , Xiaonian Li , Jinshu Tian , Yihan Zhu
{"title":"Deactivation mechanisms and mitigation strategies for nickel-based acetylene semi-hydrogenation catalysts†","authors":"Yi Miao ,&nbsp;Shuzhe Zheng ,&nbsp;Jiaqi Qi ,&nbsp;Mingyi Xiao ,&nbsp;Mingwu Tan ,&nbsp;Zhongting Hu ,&nbsp;Xiaonian Li ,&nbsp;Jinshu Tian ,&nbsp;Yihan Zhu","doi":"10.1039/d5cy00098j","DOIUrl":"10.1039/d5cy00098j","url":null,"abstract":"<div><div>Acetylene semi-hydrogenation is a crucial reaction in the ethylene purification industry, and nickel-based catalysts are widely studied due to their low cost and excellent hydrogenation activity. However, the catalytic stability of these catalysts remains a significant challenge, with unclear deactivation mechanisms and a lack of effective strategies. In this paper, we used techniques such as hydrogen-programmed temperature reduction coupled with on-line mass spectrometry (H<sub>2</sub>-TPR-MS), <em>in situ</em> Fourier transform infrared spectroscopy (<em>in situ</em> FT-IR) under reaction conditions, and Diffuse Reflectance Infrared Fourier Transform Spectroscopy with CO as a probe molecule (CO-DRIFTS) to uncover a non-classical deactivation mechanism for supported nickel-based catalysts. Specifically, we discovered that the active Ni component interacts with hydroxyl groups on the support surface under reaction conditions, leading to the formation of inactive NiO<sub><em>x</em></sub> species. This interaction alters the electronic structure of the active Ni sites, affecting the adsorption and activation of acetylene, and ultimately results in gradual catalyst deactivation. Based on these findings, we proposed a strategy to modify the support surface and weaken this interaction, which enabled the design of highly stable nickel-based catalysts.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"15 9","pages":"Pages 2838-2843"},"PeriodicalIF":4.4,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143911798","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
Fluorite phase La–M–O (M = Zr and Ce) composite oxides for oxidative dehydrogenation of ethane at low or high temperatures: redox sites vs. lattice oxygen† 低温或高温下乙烷氧化脱氢用萤石相La-M-O (M = Zr和Ce)复合氧化物:氧化还原位点与晶格氧†
IF 4.4 3区 化学
Catalysis Science & Technology Pub Date : 2025-03-17 DOI: 10.1039/d4cy01484g
Jieqi Zhou , Liang Guo , Junwei Xu , Rumeng Ouyang , Xiaomei Yu , Xiuzhong Fang , Jiating Shen , Xiang Wang
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