Catalysis Science & Technology最新文献_第10页

Sulfated niobia and zirconia catalysts for the synthesis of ethyl levulinate 硫酸氧化铌和氧化锆催化剂合成乙酰丙酸乙酯

IF 4 3区化学

Catalysis Science & Technology Pub Date : 2026-05-19 Epub Date: 2026-04-09 DOI: 10.1039/d5cy01343g

Jaime E. Bayona Solano , Ana Julia Avila , Daniel A. Sánchez , Gabriela M. Tonetto

{"title":"Sulfated niobia and zirconia catalysts for the synthesis of ethyl levulinate","authors":"Jaime E. Bayona Solano , Ana Julia Avila , Daniel A. Sánchez , Gabriela M. Tonetto","doi":"10.1039/d5cy01343g","DOIUrl":"10.1039/d5cy01343g","url":null,"abstract":"<div><div>The esterification of levulinic acid into ethyl levulinate is a key reaction for biomass valorization, and the development of highly active and stable solid acid catalysts is essential to improve process efficiency. In this context, this work evaluates how sulfation strategies affect the acidic properties and catalytic behavior of niobium pentoxide- and zirconium dioxide-based catalysts in levulinic acid esterification with ethanol. Catalysts were synthesized by wet impregnation followed by filtration or evaporation, using sulfuric acid or ammonium sulfate as sulfur sources, and characterized by X-ray diffraction, N<sub>2</sub> physisorption, laser diffraction, potentiometric titration with <em>n</em>-butylamine, and FT-IR with pyridine adsorption. Sulfation modified not only the density and strength of acid sites, but also their Brønsted/Lewis nature, promoting the formation of strong and very strong acid sites, particularly in zirconia-based catalysts. Catalytic tests showed that sulfated zirconia prepared by wet impregnation–evaporation with ammonium sulfate achieved the highest performance, reaching up to 98% conversion at 140 °C. A multiparametric analysis revealed statistically significant correlations between levulinic acid conversion and BET surface area, the number of strong and very strong acid sites, and the relative Brønsted/Lewis acid site concentration, demonstrating that catalytic activity is governed by the generation of strong Brønsted acid sites and their stability under reaction conditions.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"16 9","pages":"Pages 3218-3228"},"PeriodicalIF":4.0,"publicationDate":"2026-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147967907","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

Soft selective light absorber for efficient photothermal chemical processes in complex reactor geometries 用于复杂反应器中高效光热化学过程的软选择性光吸收剂

IF 4 3区化学

Catalysis Science & Technology Pub Date : 2026-05-19 Epub Date: 2026-04-13 DOI: 10.1039/d6cy00129g

Fuzhen Hu , Wei Wang , Dachao Yuan , Kai Du , Jiacong Guo , Lin Ma , Yuan Tang , Yaguang Li , Jinhua Ye

{"title":"Soft selective light absorber for efficient photothermal chemical processes in complex reactor geometries","authors":"Fuzhen Hu , Wei Wang , Dachao Yuan , Kai Du , Jiacong Guo , Lin Ma , Yuan Tang , Yaguang Li , Jinhua Ye","doi":"10.1039/d6cy00129g","DOIUrl":"10.1039/d6cy00129g","url":null,"abstract":"<div><div>Photothermal chemical processes are expected to solve the dilemma of fossil energy consumption, but the sunlight-irradiated temperatures of reactors are ∼200 °C, which is insufficient to drive chemical processes. Herein, we have designed a large-scale soft, selective light absorber by spray-coating a two-dimensional MXene layer on Al foil. By optimising the MXene layer thickness, the material achieves 88% solar absorption while limiting infrared radiation to one-fifth. Meanwhile, the excellent flexibility enables the soft, selective light absorber to encapsulate various chemical process reactors (disc, conical, spiral tube), allowing them to reach sunlight-irradiated temperatures of ∼400 °C, more than double those of reactors coated with carbon black powder. Consequently, the three reactors are applied for photothermal gas-state reverse water-gas shift reaction, solid-state CO<sub>2</sub> desorption, and liquid-state methanol reforming reactions, which showed a CO generation rate of >1200 mol g<sup>−1</sup> h<sup>−1</sup>, a CO<sub>2</sub> desorption rate of >3 mL min<sup>−1</sup>, and a H<sub>2</sub> generation rate of >300 mmol g<sup>−1</sup> h<sup>−1</sup>, respectively, at least 10 times higher than for the reactors coated with carbon black. This work reports retrofitting soft, selective light absorbers to chemical process reactors for the first time, producing efficient photothermal reactors and providing a solid foundation for the future development of the sunlight-driven chemical industry.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"16 9","pages":"Pages 3404-3411"},"PeriodicalIF":4.0,"publicationDate":"2026-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147967844","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

Bimetallic CuRu/Al2O3 catalyst for highly selective hydrogenation of furfural to furfuryl alcohol 高选择性糠醛加氢制糠醇的双金属cuu /Al2O3催化剂

IF 4 3区化学

Catalysis Science & Technology Pub Date : 2026-05-19 Epub Date: 2026-03-25 DOI: 10.1039/d5cy01514f

Meichen Pan , Zhenduo Huang , Yuhao Yang , Yongzhen Gao , Meng Zhang , Zhongyi Liu

{"title":"Bimetallic CuRu/Al2O3 catalyst for highly selective hydrogenation of furfural to furfuryl alcohol","authors":"Meichen Pan , Zhenduo Huang , Yuhao Yang , Yongzhen Gao , Meng Zhang , Zhongyi Liu","doi":"10.1039/d5cy01514f","DOIUrl":"10.1039/d5cy01514f","url":null,"abstract":"<div><div>The selective hydrogenation of furfural (FAL) to furfuryl alcohol (FA) derived from biomass sources is crucial for alleviating the energy crisis. Cu-based catalysts with low cost and high selectivity are widely employed in this reaction. To enhance the activity of Cu-based catalysts under mild conditions, this study synthesized the bimetallic CuRu/Al<sub>2</sub>O<sub>3</sub> catalysts with varying Ru contents <em>via</em> the deposition–reduction method. The physicochemical properties characterized by XRD, TEM, H<sub>2</sub>-TPR, H<sub>2</sub>-TPD, XPS, and FT-IR techniques revealed that Ru doping promoted the dispersion of Cu species and improved the H<sub>2</sub> adsorption ability. Additionally, strong Cu–Ru interactions, which derived from electron transfer from Cu to Ru, enhanced the metal reducibility. As a result, the bimetallic 5Cu1Ru/Al<sub>2</sub>O<sub>3</sub> catalyst exhibited the outstanding performance of 99.9% FAL conversion and 99.9% FA selectivity within 4 h at 90 °C under 1 MPa H<sub>2</sub> pressure, with an exceptionally low apparent activation energy of 118.4 kJ mol<sup>−1</sup>. TG analysis indicated that increasing Ru content lowered the temperature of FA desorption, thereby easily re-exposing the active sites for the reaction cycle. The current investigation provides a reference for designing the efficient bimetallic catalysts to achieve high FAL conversion under mild conditions.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"16 9","pages":"Pages 3288-3301"},"PeriodicalIF":4.0,"publicationDate":"2026-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147967940","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

Regioselective direct synthesis of mono- and bis-substituted benzimidazoles via base-switchable aerobic N-heterocyclic carbene organocatalysis 碱基可切换好氧n杂环碳的区域选择性直接合成单取代和双取代苯并咪唑

IF 4 3区化学

Catalysis Science & Technology Pub Date : 2026-05-19 Epub Date: 2026-04-02 DOI: 10.1039/d6cy00036c

Janmejaya Sen , Richa Sharma , Amol T. Mahajan , Abdul Rahaman T. A. , Samir T. Sahu , Alexander S. Novikov , Sandeep Chaudhary

{"title":"Regioselective direct synthesis of mono- and bis-substituted benzimidazoles via base-switchable aerobic N-heterocyclic carbene organocatalysis","authors":"Janmejaya Sen , Richa Sharma , Amol T. Mahajan , Abdul Rahaman T. A. , Samir T. Sahu , Alexander S. Novikov , Sandeep Chaudhary","doi":"10.1039/d6cy00036c","DOIUrl":"10.1039/d6cy00036c","url":null,"abstract":"<div><div>Herein, we disclosed a metal-free, highly efficient, and sustainable N-heterocyclic carbene-based organocatalyst utilized for the regioselective synthesis of mono- () and bis-substituted benzimidazole () derivatives under the optimized reaction conditions. The new catalytic protocol demonstrated high efficiency across a broad spectrum of substituted <em>o</em>-phenylenediamines () and substituted benzyl alcohols (), and showed excellent tolerance towards various functional groups. The operationally developed protocol is quite simple, utilizes NHC as an organocatalyst, and furnishes the desired mono- () and bis-substituted benzimidazole () derivatives in up to 77% and 87% yields, respectively. While using NHC as an organocatalyst (catalyst C), bis-substituted benzimidazoles were obtained in the presence of a strong base (KO<sup><em>t</em></sup>Bu), whereas mono-substituted benzimidazole was afforded using a weaker base (Cs<sub>2</sub>CO<sub>3</sub>). To gain deeper insight into the underlying mechanistic pathway, an array of control experiments has been performed. The mechanistic pathway involves <em>in situ</em> formation of aldehyde from the dehydrogenation of alcohol with the aid of NHC. Then, the resulting aldehyde condenses with diamine to generate imine, which, on further assistance with NHC, forms <em>aza</em>-Breslow intermediate, is converted into imidoyl azolium in aerobic conditions that subsequently undergoes cyclization to furnish benzimidazole. The mechanistic studies involved the detection of BHT-trapped ketyl adduct. Furthermore, EPR experiments suggested the possible involvement of free-radical species. Further, the synthetic utility of this protocol was demonstrated by gram-scale synthesis, intermolecular cyclization to 2-phenylquinazoline, and the synthesis of fungicide fuberidazole.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"16 9","pages":"Pages 3366-3377"},"PeriodicalIF":4.0,"publicationDate":"2026-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147967841","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

Light driven catalytic CO2 reduction: lessons learnt when low is actually no activity 光驱动的催化二氧化碳还原：当低实际上是没有活动的经验教训

IF 4 3区化学

Catalysis Science & Technology Pub Date : 2026-05-19 Epub Date: 2026-04-08 DOI: 10.1039/d5cy01378j

Varinder Singh , Kieran DeMonte , Olivier Schott , Folaranmi S. Akogun , Garry S. Hanan , Sally Brooker

引用次数: 0

Green electrochemical upcycling of PET waste via bimetallic catalyst-driven ethylene glycol selective oxidation to formate 双金属催化剂驱动乙二醇选择性氧化生成甲酸酯的PET废弃物绿色电化学升级回收

IF 4 3区化学

Catalysis Science & Technology Pub Date : 2026-05-19 Epub Date: 2026-03-23 DOI: 10.1039/d6cy00210b

Xiaolu Wu , Zhishan Liang , Wensheng Zhang , Youlin Huang , Guanhui Xu , Wei Wang , Dongxue Han

{"title":"Green electrochemical upcycling of PET waste via bimetallic catalyst-driven ethylene glycol selective oxidation to formate","authors":"Xiaolu Wu , Zhishan Liang , Wensheng Zhang , Youlin Huang , Guanhui Xu , Wei Wang , Dongxue Han","doi":"10.1039/d6cy00210b","DOIUrl":"10.1039/d6cy00210b","url":null,"abstract":"<div><div>The rapid accumulation of plastic waste has created an urgent need for efficient and sustainable upcycling strategies. Herein, we report a Zn and Cu co-doped spinel oxide electrocatalyst (CuO/ZnCuCo<sub>2</sub>O<sub>4</sub>) for the selective electrochemical conversion of polyethylene terephthalate (PET) into formate under mild conditions. Dual-metal incorporation modulates the electronic structure of Co<sub>3</sub>O<sub>4</sub> and optimizes the adsorption–desorption behavior of key intermediates during the ethylene glycol oxidation reaction (EGOR). As a result, the catalyst achieves a current density of 10 mA cm<sup>−2</sup> at 1.37 V <em>vs.</em> RHE, a high formate faradaic efficiency of 95.54%, and a formate production rate of 0.78 mmol cm<sup>−2</sup> h<sup>−1</sup>, together with excellent operational stability. When applied to hydrolysates derived from real waste PET, the system still delivers a formate yield of 85.6%, demonstrating strong tolerance to impurities and practical applicability. Density functional theory calculations reveal that the synergistic interaction among Zn, Cu, and Co regulates the electronic structure, facilitates EG adsorption, and lowers the energy barrier of key oxidation steps. This work provides a structure-engineering strategy for high-performance spinel electrocatalysts and advances the electrochemical upcycling of plastic waste.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"16 9","pages":"Pages 3343-3354"},"PeriodicalIF":4.0,"publicationDate":"2026-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147967898","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

Efficient hydrogen production by γ-g-C3N4/Ag–CdS heterojunction photocatalyst via S-scheme mechanism γ-g-C3N4/ Ag-CdS异质结光催化剂S-scheme制氢机理

IF 4 3区化学

Catalysis Science & Technology Pub Date : 2026-05-19 Epub Date: 2026-04-07 DOI: 10.1039/d6cy00035e

K. S. Chandrakantha , H. R. Deepu , Mahesh Itagi , Madhura N. Talwar , Smitha Ankanahalli Shankaregowda , K. Mantelingu , P. Madhusudan , S. Srikantaswamy , K. S. Rangappa

{"title":"Efficient hydrogen production by γ-g-C3N4/Ag–CdS heterojunction photocatalyst via S-scheme mechanism","authors":"K. S. Chandrakantha , H. R. Deepu , Mahesh Itagi , Madhura N. Talwar , Smitha Ankanahalli Shankaregowda , K. Mantelingu , P. Madhusudan , S. Srikantaswamy , K. S. Rangappa","doi":"10.1039/d6cy00035e","DOIUrl":"10.1039/d6cy00035e","url":null,"abstract":"<div><div>Photocatalytic water splitting is a promising approach for sustainable hydrogen generation. This study aims to develop a simple and efficient photocatalyst and to investigate the influence of gamma irradiation on photocatalytic water splitting performance. A gamma irradiated graphitic carbon nitride/silver–cadmium sulfide (γ-g-C<sub>3</sub>N<sub>4</sub>/Ag–CdS) heterostructure composite was synthesized <em>via</em> microwave-assisted hydrothermal method, followed by melamine polymerization and the resultant catalyst was subsequently exposed to gamma radiation. The γ-g-C<sub>3</sub>N<sub>4</sub>/Ag–CdS catalyst exhibited enhanced photocatalytic hydrogen production, demonstrating the effectiveness of gamma irradiation and the incorporation of Ag nanoparticles, which enabled an S-scheme electron transfer pathway, thereby improving stability and catalytic performance while reducing reliance on high-cost noble metals such as platinum. Enhanced efficiency was achieved through suppressed charge carrier recombination, improved interfacial charge transfer, and increased visible-light absorption. Gamma irradiation promoted charge separation without additional chemical reagents, and microwave-assisted synthesis reduced reaction time and energy consumption. The hydrogen evolution rate of the gamma irradiated composite reached 5600 μmol g<sup>−1</sup> h<sup>−1</sup>, compared to 4100 μmol g<sup>−1</sup> h<sup>−1</sup> for the unirradiated sample. The γ-g-C<sub>3</sub>N<sub>4</sub>/Ag–CdS photocatalyst delivers a ∼36% increase in hydrogen evolution rate compared to the untreated composite. This work provides valuable insights for the development of stable and high-performance photocatalysts for sustainable hydrogen generation.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"16 9","pages":"Pages 3355-3365"},"PeriodicalIF":4.0,"publicationDate":"2026-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147967899","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

Tailoring amorphous alumina catalysts with enriched five-coordinated aluminum via pH control 通过pH控制富五配位铝定制无定形氧化铝催化剂

IF 4 3区化学

Catalysis Science & Technology Pub Date : 2026-05-19 Epub Date: 2026-03-18 DOI: 10.1039/d5cy01418b

Takumi Watanabe , Haruto Kamiya , Yunzi Xin , Yuping Xu , Takashi Shirai

{"title":"Tailoring amorphous alumina catalysts with enriched five-coordinated aluminum via pH control","authors":"Takumi Watanabe , Haruto Kamiya , Yunzi Xin , Yuping Xu , Takashi Shirai","doi":"10.1039/d5cy01418b","DOIUrl":"10.1039/d5cy01418b","url":null,"abstract":"<div><div>Amorphous alumina is known to contain a high fraction of five-coordinated aluminum species (Al(<span>v</span>)), which are recognized as active sites and serve as anchoring sites for noble metals. In this study, we aimed to synthesize highly active amorphous alumina enriched in Al(<span>v</span>) by controlling the pH during the gelation of aluminum hydroxide using buffers with different concentrations (0.1, 1, 10, and 100 mM). After dehydration, the resulting alumina was characterized and evaluated for VOC decomposition. While the Al(<span>v</span>) fraction increased with buffer concentration (42–53% at 650 °C), no direct correlation was observed between activity and the parameter Al(<span>v</span>) ratio in terms of specific surface area. Instead, deconvolution of the <sup>27</sup>Al NMR spectra revealed that Al(<span>v</span>) consists of sharp (trigonal bipyramidal) and broad (square pyramidal) components, the latter exhibiting a strong correlation with VOC decomposition when specific surface area was taken into consideration (<em>R</em><sup>2</sup> = 0.77). Experimental results and insights from previous research suggest that high pH suppresses hydroxide precipitation, yielding small amorphous particles prone to aggregation, whereas low pH promotes nitrate incorporation into the lattice, leading to structural disorder and site blocking on pyramidal Al(<span>v</span>). Among the tested conditions, the 1 mM buffer produced amorphous alumina with an optimal balance of surface area and Al(<span>v</span>) broad content, achieving for the first time 100% VOC decomposition using pure amorphous alumina. These findings highlight pH control as a promising strategy for tailoring active Al(<span>v</span>) sites in alumina catalysts.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"16 9","pages":"Pages 3150-3159"},"PeriodicalIF":4.0,"publicationDate":"2026-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147967903","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

From multifunctional catalysts to smart substrates: adsorption control for efficient light-driven one-pot benzimidazole synthesis over Pd/NH2–Ni–Fe-MOF 从多功能催化剂到智能底物：Pd/ NH2-Ni-Fe-MOF上高效光驱动一锅苯并咪唑合成的吸附控制

IF 4 3区化学

Catalysis Science & Technology Pub Date : 2026-05-19 Epub Date: 2026-04-13 DOI: 10.1039/d6cy00076b

Hurunqing Liu , Lin Ye , Yun Yuan , Quanyuan Wang , Dengrong Sun , Zhaohui Li

{"title":"From multifunctional catalysts to smart substrates: adsorption control for efficient light-driven one-pot benzimidazole synthesis over Pd/NH2–Ni–Fe-MOF","authors":"Hurunqing Liu , Lin Ye , Yun Yuan , Quanyuan Wang , Dengrong Sun , Zhaohui Li","doi":"10.1039/d6cy00076b","DOIUrl":"10.1039/d6cy00076b","url":null,"abstract":"<div><div>Light-driven one-pot tandem/cascade reactions have attracted increasing interest due to their green process and atomic efficiency. In addition to active sites, the adsorption behavior of reaction substrates also plays a critical role on the catalytic process, but is always overlooked. Herein, we report that modulating the reaction substrates to regulate the adsorption behavior of intermediates can effectively facilitate one-pot multi-step reactions. <em>O</em>-Nitroaniline is strategically selected to replace the commonly used <em>o</em>-phenylenediamine for reaction with benzyl alcohol to synthesize benzimidazole in a one-pot process under visible-light irradiation. The use of <em>o</em>-nitroaniline effectively promotes the adsorption of the benzyl alcohol-derived aldehyde intermediate on the catalyst but weakens the adsorption of <em>o</em>-nitroaniline-derived <em>o</em>-phenylenediamine. Thus, the condensation between these two intermediates can proceed smoothly, alleviating the fatal polymerization side reaction of <em>o</em>-phenylenediamine, affording high efficiency in light-driven benzimidazole production. Departing from the conventional catalyst design, this work underscores an effective way to modulate the reaction substrates for accelerated one-pot synthesis, signifying an important contribution to the design of one-pot synthesis systems.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"16 9","pages":"Pages 3336-3342"},"PeriodicalIF":4.0,"publicationDate":"2026-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147967897","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

Linking hydrothermal deactivation of Cu-CHA catalysts for NH3-SCR to dealumination and reduced [Cu2(NH3)4O2]2+ formation Cu-CHA催化剂水热失活与NH3- scr脱铝及减少[Cu2(NH3)4O2]2+生成的联系

IF 4.2 3区化学

Catalysis Science & Technology Pub Date : 2026-04-27 Epub Date: 2026-03-06 DOI: 10.1039/d5cy01491c

Shivangi Singh , Ton V. W. Janssens , Henrik Grönbeck

{"title":"Linking hydrothermal deactivation of Cu-CHA catalysts for NH3-SCR to dealumination and reduced [Cu2(NH3)4O2]2+ formation","authors":"Shivangi Singh , Ton V. W. Janssens , Henrik Grönbeck","doi":"10.1039/d5cy01491c","DOIUrl":"10.1039/d5cy01491c","url":null,"abstract":"<div><div>NH<sub>3</sub>-Selective Catalytic Reduction (NH<sub>3</sub>-SCR) is a critical technology for controlling NO<sub><em>x</em></sub> emissions from diesel and H<sub>2</sub> engines. Cu-exchanged chabazite (Cu-CHA) materials are preferred catalysts for the NH<sub>3</sub>-SCR reaction thanks to high activity, selectivity and stability under normal operating conditions. However, exposure of Cu-CHA to water at high temperatures (≥650 °C) leads to loss of Brønsted acid sites due to dealumination. Here, we have measured the activity and selectivity of hydrothermally aged Cu-CHA. The hydrothermal deactivation is linked to changes in the amount of Brønsted acid sites as measured by NH<sub>3</sub>-Temperature-Programmed Desorption (TPD) and the ability to form the key intermediate [Cu<sub>2</sub>(NH<sub>3</sub>)<sub>4</sub>O<sub>2</sub>]<sup>2+</sup>, as probed by NO-Temperature-Programmed Reaction (TP Reaction). The activity decreases rapidly during the first 10 hours of aging, which correlates with a rapid loss of Brønsted acid sites. The activity after 10 hours is reduced at a slower rate, which coincides with a loss in ability to form [Cu<sub>2</sub>(NH<sub>3</sub>)<sub>4</sub>O<sub>2</sub>]<sup>2+</sup>. The measurements are corroborated by density functional theory based microkinetic modeling. The simulations show that the part of the reaction cycle that occurs over Brønsted acid sites in fresh catalysts can occur at a slower rate over silanol nests in the aged catalyst. Roughly half of the activity loss after 100 hours of aging can be attributed to the decrease of Brønsted acid sites, whereas the remaining loss can be related to reduced formation of the [Cu<sub>2</sub>(NH<sub>3</sub>)<sub>4</sub>O<sub>2</sub>]<sup>2+</sup> complex.</div></div>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":"16 8","pages":"Pages 2889-2898"},"PeriodicalIF":4.2,"publicationDate":"2026-04-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147751103","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