Applied Catalysis A: General最新文献

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Heterogeneous bismuth catalyst for the selective hydrogenation of nitroarenes to arylamines using molecular hydrogen

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-02-05 DOI: 10.1016/j.apcata.2024.120080

Raju Kumar , Baint Singh , Achala Rana , Manvender Yadav , Jyotishman Kaishyop , Tuhin Surva Khan , Rajesh Kumar , Ganesh Naik , Anand Narani

Bismuth is renowned for its exceptional safety, highlighted by numerous examples demonstrating its low toxicity. Considering this, we present a novel, active, and reusable heterogeneous bismuth catalyst (Bi-NC/γ-Al₂O₃) for chemoselective hydrogenation of nitroarenes to aryl amines using molecular hydrogen. The Bi-NC/γ-Al₂O₃ catalyst was synthesized through a simple impregnation method followed by pyrolysis at 700°C, for 2 h under a nitrogen atmosphere. The physicochemical properties of fresh and spent Bi-NC/γ-Al₂O₃ catalysts were comprehensively characterized by powder X-ray diffraction (P-XRD), X-ray photoelectron spectroscopy (XPS), High-resolution transmission electron microscopy (HR-TEM), N₂ adsorption-desorption, H₂-temperature programmed reduction (H₂-TPR), NH₃-temperature programmed desorption (NH₃-TPD), and thermogravimetric analysis (TGA). The bismuth content in the Bi-NC/γ-Al₂O₃ catalyst was estimated by inductively coupled plasma optical emission spectroscopy (ICP-OES). The catalyst demonstrated exceptional performance and selectivity in reducing a wide variety of nitroarenes to their corresponding aryl amines, achieving good to excellent yields (36 examples). Furthermore, the Bi-NC/γ-Al₂O₃ catalyst was applied to the selective hydrogenation of nitro groups in three commercially available drugs. Additionally, five pharmaceutical intermediates, including linezolid, Norfloxacin, Carbamazepine, paracetamol, and tizanidine, were synthesized up to a ∼1 g scale with a quantitative yield, showcasing the catalyst activity and selectivity. Further, the reaction mechanism was elucidated by tracking the intermediates (through GC-FID & GC-MS) and employing Density Functional Theory (DFT). Notably, the Bi-NC/γ-Al₂O₃ catalyst is stable, recovered, and reused for four cycles without losing significant activity and selectivity.

{"title":"Heterogeneous bismuth catalyst for the selective hydrogenation of nitroarenes to arylamines using molecular hydrogen","authors":"Raju Kumar , Baint Singh , Achala Rana , Manvender Yadav , Jyotishman Kaishyop , Tuhin Surva Khan , Rajesh Kumar , Ganesh Naik , Anand Narani","doi":"10.1016/j.apcata.2024.120080","DOIUrl":"10.1016/j.apcata.2024.120080","url":null,"abstract":"<div><div>Bismuth is renowned for its exceptional safety, highlighted by numerous examples demonstrating its low toxicity. Considering this, we present a novel, active, and reusable heterogeneous bismuth catalyst (Bi-NC/γ-Al2O3) for chemoselective hydrogenation of nitroarenes to aryl amines using molecular hydrogen. The Bi-NC/γ-Al2O3 catalyst was synthesized through a simple impregnation method followed by pyrolysis at 700°C, for 2 h under a nitrogen atmosphere. The physicochemical properties of fresh and spent Bi-NC/γ-Al2O3 catalysts were comprehensively characterized by powder X-ray diffraction (P-XRD), X-ray photoelectron spectroscopy (XPS), High-resolution transmission electron microscopy (HR-TEM), N2 adsorption-desorption, H2-temperature programmed reduction (H2-TPR), NH3-temperature programmed desorption (NH3-TPD), and thermogravimetric analysis (TGA). The bismuth content in the Bi-NC/γ-Al2O3 catalyst was estimated by inductively coupled plasma optical emission spectroscopy (ICP-OES). The catalyst demonstrated exceptional performance and selectivity in reducing a wide variety of nitroarenes to their corresponding aryl amines, achieving good to excellent yields (36 examples). Furthermore, the Bi-NC/γ-Al2O3 catalyst was applied to the selective hydrogenation of nitro groups in three commercially available drugs. Additionally, five pharmaceutical intermediates, including linezolid, Norfloxacin, Carbamazepine, paracetamol, and tizanidine, were synthesized up to a ∼1 g scale with a quantitative yield, showcasing the catalyst activity and selectivity. Further, the reaction mechanism was elucidated by tracking the intermediates (through GC-FID & GC-MS) and employing Density Functional Theory (DFT). Notably, the Bi-NC/γ-Al2O3 catalyst is stable, recovered, and reused for four cycles without losing significant activity and selectivity.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"691 ","pages":"Article 120080"},"PeriodicalIF":4.7,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143135255","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

High-curvature single-atom catalysts for electrocatalysis: A review

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-02-05 DOI: 10.1016/j.apcata.2025.120160

Caili Chen, Zekai Zhang, Liangli Dai, Bolin Li, Zesheng Li

The catalytic performance of a high-curvature single-atom catalyst is highly dependent on its geometry and the type of metal atoms it carries. This review uses a combination of extensive literature research and theoretical analysis to comprehensively analyze several key aspects of high-curvature single-atom catalysts, including dimension, energy, reaction mechanism, radius of curvature, reaction selectivity, size, different metal atoms, and different types of reactions. In this paper, the unique advantages of high-curvature single-atom catalysts are successfully summarized and refined. On the one hand, it has been found that the surface of this catalyst is highly curved, which promotes the adsorption and reaction of atoms. On the other hand, this paper states that choosing the right radius of curvature is essential to optimize the catalytic process. The comprehensive literature analysis in recent years may provide important reference and enlightenment for researchers, promote the further development of the field of catalysis, and develop more advanced high-curvature single-atom catalytic materials.

{"title":"High-curvature single-atom catalysts for electrocatalysis: A review","authors":"Caili Chen, Zekai Zhang, Liangli Dai, Bolin Li, Zesheng Li","doi":"10.1016/j.apcata.2025.120160","DOIUrl":"10.1016/j.apcata.2025.120160","url":null,"abstract":"<div><div>The catalytic performance of a high-curvature single-atom catalyst is highly dependent on its geometry and the type of metal atoms it carries. This review uses a combination of extensive literature research and theoretical analysis to comprehensively analyze several key aspects of high-curvature single-atom catalysts, including dimension, energy, reaction mechanism, radius of curvature, reaction selectivity, size, different metal atoms, and different types of reactions. In this paper, the unique advantages of high-curvature single-atom catalysts are successfully summarized and refined. On the one hand, it has been found that the surface of this catalyst is highly curved, which promotes the adsorption and reaction of atoms. On the other hand, this paper states that choosing the right radius of curvature is essential to optimize the catalytic process. The comprehensive literature analysis in recent years may provide important reference and enlightenment for researchers, promote the further development of the field of catalysis, and develop more advanced high-curvature single-atom catalytic materials.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"694 ","pages":"Article 120160"},"PeriodicalIF":4.7,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143378048","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Modification strategies of TiO2-based nanocatalysts for CO2 reduction through photocatalysis: A mini review

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-02-05 DOI: 10.1016/j.apcata.2024.120054

Ya-Nan Jing, Xing-Liang Yin, Lei-lei Li

Anthropogenic emission of CO₂ severely hinders sustainable development of human society. Photocatalysis has emerged as a promising and environmentally friendly approach for converting CO₂ into one or two carbon compounds, and is anticipated to contribute positively to achieving the dual carbon goal. In recent years, TiO₂-based catalysts have demonstrated their effectiveness in the photocatalytic CO₂ reduction. This article provides a review of the principles and applications of TiO₂-based catalysts for CO₂ photocatalytic reduction, focusing on four common modification strategies: morphology control, co-catalyst loading, surface defect introduction, and heterostructure design. On this basis, this article summarizes the challenges faced in further increasing the efficiency of TiO₂-based photocatalytic CO₂ reduction, and looks forward to possible future development directions.

引用次数: 0

TiO2-anchored three-dimensional integration of layer covalent organic framework for photocatalytic H2 production

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-02-05 DOI: 10.1016/j.apcata.2024.120068

Ai-Juan Li, Tao Zhang, Sheng-Li Huang

Photocatalytic H₂ production presents great significance for sustainable development of energy and economy. Covalent organic frameworks (COFs) have received huge attention in photocatalytic applications. Herein, crystalline OH-COFs were synthesized through the transformation of imine bond to quinoline ring via Povarov reaction. TiO₂-COF exhibited excellent photocatalytic performance for H₂ production in H₂O/alcohol system. This strategy provides available method for the design and synthesis of highly efficient photocatalysts based on COF-inorganic semiconductor hybridization.

引用次数: 0

Efficient conversion of fluorinated greenhouse gases using aluminum-doped hydroxyapatite

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-02-05 DOI: 10.1016/j.apcata.2024.120089

Yiwei Sun , Xiaoli Wei , Sihui Wu , Fangcao Liu , Bing Liu , Wenfeng Han

In this study, a series of hydroxyl apatite catalysts (HA-xAl) with varying aluminum doping levels were synthesized using a hydrothermal method. The influence of aluminum doping on the activity and catalytic stability of HFC-152a dehydrofluorination was systematically investigated. Reaction rates were normalized according to the aluminum doping amount. The results revealed that the HA-5Al catalyst exhibited a high specific reaction rate of 16,500 mmol·h⁻¹ ·mol⁻¹ Al, indicating a significant enhancement in catalytic efficiency due to aluminum incorporation into the hydroxyapatite. Furthermore, the HA-20Al catalyst demonstrated a conversion exceeding 63 % after 100 h of reaction. This remarkable stability is attributed to the formation of a metastable active species, F-Al-O, which likely results from the limited interaction with the hydroxyapatite structure. Additionally, the optimal acidity and highly dispersed active sites of catalysts contribute to reduced carbon deposition and further enhance its stability.

引用次数: 0

Hydrotalcite-catalyzed methylation of isosorbide via dimethyl carbonate: Influence of the catalyst on the reaction mechanism

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-02-05 DOI: 10.1016/j.apcata.2024.120088

María José Ginés-Molina , José Santamaría-González , Pedro Maireles-Torres , Juan A. Cecilia , Rafael Luque , Manuel López-Granados , Giacomo Trapasso , Fabio Aricò , Juan Soto , Ramón Moreno-Tost

This work presents the results of the methylation of isosorbide to produce dimethyl isosorbide using dimethyl carbonate as methylating agent and reaction medium and a MgAl mixed oxide derived from the calcination of a commercial hydrotalcite as basic catalyst. This reaction was carried out using three types of reactors: a continuous liquid flow reactor and two batch reactors, the first one working at autogenous pressure and the other one at atmospheric pressure. The best results were achieved for the atmospheric pressure reactor, with the dimethyl isosorbide yield being 100 % at 110 ºC, after 8 h. Under these experimental conditions, the catalyst showed a loss of selectivity towards dimethyl isosorbide with consecutive catalytic cycles, reaching approximately 50 % dimethyl isosorbide yield after 5 catalytic cycles, but maintaining the isosorbide conversion at 100 %. The reaction mechanism most probably relies on the cooperation between the catalyst and the dimethyl carbonate. With the help of computational studies, it has been demonstrated that the adsorption of dimethyl carbonate on the catalyst takes place through the carbonyl group and that it adsorbs on either Mg^2 + or Al³⁺ ions. Finally, the assignation of the FTIR bands corresponding to the adsorbed dimethyl carbonate species revealed that it undergoes a surface reaction, leading to the formation of both methoxide and monomethyl carbonate adsorbed species. The presence of such species was identified as responsible for the changing pattern selectivity of the reaction during the reutilization of the catalyst.

{"title":"Hydrotalcite-catalyzed methylation of isosorbide via dimethyl carbonate: Influence of the catalyst on the reaction mechanism","authors":"María José Ginés-Molina , José Santamaría-González , Pedro Maireles-Torres , Juan A. Cecilia , Rafael Luque , Manuel López-Granados , Giacomo Trapasso , Fabio Aricò , Juan Soto , Ramón Moreno-Tost","doi":"10.1016/j.apcata.2024.120088","DOIUrl":"10.1016/j.apcata.2024.120088","url":null,"abstract":"<div><div>This work presents the results of the methylation of isosorbide to produce dimethyl isosorbide using dimethyl carbonate as methylating agent and reaction medium and a MgAl mixed oxide derived from the calcination of a commercial hydrotalcite as basic catalyst. This reaction was carried out using three types of reactors: a continuous liquid flow reactor and two batch reactors, the first one working at autogenous pressure and the other one at atmospheric pressure. The best results were achieved for the atmospheric pressure reactor, with the dimethyl isosorbide yield being 100 % at 110 ºC, after 8 h. Under these experimental conditions, the catalyst showed a loss of selectivity towards dimethyl isosorbide with consecutive catalytic cycles, reaching approximately 50 % dimethyl isosorbide yield after 5 catalytic cycles, but maintaining the isosorbide conversion at 100 %. The reaction mechanism most probably relies on the cooperation between the catalyst and the dimethyl carbonate. With the help of computational studies, it has been demonstrated that the adsorption of dimethyl carbonate on the catalyst takes place through the carbonyl group and that it adsorbs on either Mg2 + or Al3+ ions. Finally, the assignation of the FTIR bands corresponding to the adsorbed dimethyl carbonate species revealed that it undergoes a surface reaction, leading to the formation of both methoxide and monomethyl carbonate adsorbed species. The presence of such species was identified as responsible for the changing pattern selectivity of the reaction during the reutilization of the catalyst.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"691 ","pages":"Article 120088"},"PeriodicalIF":4.7,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143135082","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Effects of hydrogen spillover on CO2 hydrogenation over Pt-Co-Al based catalysts

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-02-05 DOI: 10.1016/j.apcata.2024.120051

Yiming He , Bowen Xu , Shuilian Liu , Weijie Fu , Jian Chen , Jie Ren , Ruiyan Sun , Zhenchen Tang , Chalachew Mebrahtu , Huanhao Chen , Feng Zeng

CO₂ hydrogenation presents a crucial pathway for carbon circularity. The activation, adsorption, and hydrogen spillover are key processes in CO₂ hydrogenation. This study investigates the effects of hydrogen spillover induced by Pt on CO₂ hydrogenation over Pt-promoted Co-Al catalysts. A series of Pt-promoted Co-Al catalysts were synthesized via co-precipitation and employed for CO₂ hydrogenation. The optimized Pt-promoted Co-Al catalyst efficiently converts CO₂, leading to the formation of methane (46.6 mmol g_cat⁻¹ h⁻¹), methanol (509.4 μmol g_cat⁻¹ h⁻¹), and higher alcohols (220.6 μmol g_cat⁻¹ h⁻¹). The Pt-promoted Co-Al catalysts facilitate hydrogen spillover, optimizing the catalysts’ reducibility and exposing more active sites. Moreover, the hydrogen adsorption is weakened due to the Pt induced hydrogen spillover, which facilitates the formation of *HCOO, *CH₃, and *CO intermediates. This in turn facilitate the coupling between *HCOO/*CO and *CH₃, enhancing the formation of higher alcohols.

{"title":"Effects of hydrogen spillover on CO2 hydrogenation over Pt-Co-Al based catalysts","authors":"Yiming He , Bowen Xu , Shuilian Liu , Weijie Fu , Jian Chen , Jie Ren , Ruiyan Sun , Zhenchen Tang , Chalachew Mebrahtu , Huanhao Chen , Feng Zeng","doi":"10.1016/j.apcata.2024.120051","DOIUrl":"10.1016/j.apcata.2024.120051","url":null,"abstract":"<div><div>CO2 hydrogenation presents a crucial pathway for carbon circularity. The activation, adsorption, and hydrogen spillover are key processes in CO2 hydrogenation. This study investigates the effects of hydrogen spillover induced by Pt on CO2 hydrogenation over Pt-promoted Co-Al catalysts. A series of Pt-promoted Co-Al catalysts were synthesized via co-precipitation and employed for CO2 hydrogenation. The optimized Pt-promoted Co-Al catalyst efficiently converts CO2, leading to the formation of methane (46.6 mmol gcat−1 h−1), methanol (509.4 μmol gcat−1 h−1), and higher alcohols (220.6 μmol gcat−1 h−1). The Pt-promoted Co-Al catalysts facilitate hydrogen spillover, optimizing the catalysts’ reducibility and exposing more active sites. Moreover, the hydrogen adsorption is weakened due to the Pt induced hydrogen spillover, which facilitates the formation of *HCOO, *CH3, and *CO intermediates. This in turn facilitate the coupling between *HCOO/*CO and *CH3, enhancing the formation of higher alcohols.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"691 ","pages":"Article 120051"},"PeriodicalIF":4.7,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143135089","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Accurate location of Ni and W active sites in hierarchical zeolite catalyst for the conversion of cellulose to alcohols

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-02-05 DOI: 10.1016/j.apcata.2024.120052

Wanying Liang , Guangyue Xu , Yao Fu

The process of converting cellulose into short-chain alcohols is a critical component of biomass valorization. In this study, we utilized an anion-cation co-directed hydrothermal method and wet impregnation to synthesize a hierarchical MFI zeolite with isolated Ni and W sites. We employed linear correlation analysis to evaluate the influence of pore size, site accessibility, and acidity on product selectivity. Balancing hydrogenation and acidic sites on the catalyst enhanced retro-aldol condensation and hydrogenation during cellulose conversion. Surface acidic sites accelerated glucose retro-aldol condensation, while micropore acidic sites aided in ethylene glycol hydrogenolysis. The close proximity of Ni and W facilitated high selectivity and yield of ethanol through bimetallic synergy. This research presented a novel strategy for preparing hierarchical zeolites with isolated metal sites and provides clarity on the cooperative roles of active sites in Ni-W bimetallic catalysts for cellulose conversion.

引用次数: 0

Lanthanum-group elements promoted PtGa catalysts for propane dehydrogenation: Exploring key performance descriptors

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-02-05 DOI: 10.1016/j.apcata.2024.120055

Haokun Wang, Xuelei Pan, Yanjie Wang, Bryan Kit Yue Ng, Shik Chi Edman Tsang

Propylene, a crucial component in the chemical industry, holds a prominent position as the second-largest material within petrochemicals, serving as a foundational element for major synthetic materials and essential industrial chemicals such as acetone and isopropanol. Conventional propylene production methods confront environmental challenges, promoting the investigation of alternative pathways, such as direct propane dehydrogenation. While commercial PtSn or PtGa-based catalysts have demonstrated success in propane dehydrogenation, further enhancements are imperative to mitigate operational costs. Therefore, this study utilizes four lanthanum-group elements (La, Ce, Pr, and Nd) with varying loadings (1 wt%, 3 wt%, and 5 wt%) to modify PtGa/Al₂O₃ catalyst, resulting in improved conversion, selectivity, and stability. Furthermore, this research establishes a clear structure-activity relationship based on some key performance descriptors, underscoring the effectiveness influence of reducibility, total acid concentration, and total coke content in conversion, selectivity, and stability. The impact of strong metal-support interactions on conversion and stability should also be considered, highlighting the complexities in accessing catalytic performances. The exploration of diverse performance descriptors revealed in this study contributes to the rational design of catalysts for propane dehydrogenation, addressing ongoing efforts to refine and tailor catalysts for efficient propane dehydrogenation. This study also offers valuable insights for optimizing catalytic performance across various industrial reactions, further advancing the field of catalysis and promoting sustainable and efficient chemical processes.

{"title":"Lanthanum-group elements promoted PtGa catalysts for propane dehydrogenation: Exploring key performance descriptors","authors":"Haokun Wang, Xuelei Pan, Yanjie Wang, Bryan Kit Yue Ng, Shik Chi Edman Tsang","doi":"10.1016/j.apcata.2024.120055","DOIUrl":"10.1016/j.apcata.2024.120055","url":null,"abstract":"<div><div>Propylene, a crucial component in the chemical industry, holds a prominent position as the second-largest material within petrochemicals, serving as a foundational element for major synthetic materials and essential industrial chemicals such as acetone and isopropanol. Conventional propylene production methods confront environmental challenges, promoting the investigation of alternative pathways, such as direct propane dehydrogenation. While commercial PtSn or PtGa-based catalysts have demonstrated success in propane dehydrogenation, further enhancements are imperative to mitigate operational costs. Therefore, this study utilizes four lanthanum-group elements (La, Ce, Pr, and Nd) with varying loadings (1 wt%, 3 wt%, and 5 wt%) to modify PtGa/Al2O3 catalyst, resulting in improved conversion, selectivity, and stability. Furthermore, this research establishes a clear structure-activity relationship based on some key performance descriptors, underscoring the effectiveness influence of reducibility, total acid concentration, and total coke content in conversion, selectivity, and stability. The impact of strong metal-support interactions on conversion and stability should also be considered, highlighting the complexities in accessing catalytic performances. The exploration of diverse performance descriptors revealed in this study contributes to the rational design of catalysts for propane dehydrogenation, addressing ongoing efforts to refine and tailor catalysts for efficient propane dehydrogenation. This study also offers valuable insights for optimizing catalytic performance across various industrial reactions, further advancing the field of catalysis and promoting sustainable and efficient chemical processes.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"691 ","pages":"Article 120055"},"PeriodicalIF":4.7,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143135091","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Revealing the positive and negative effects of strong metal support interactions on CO oxidation for Pt-supported different crystals (β- and γ-) MnO2 catalysts: Pt oxides and carbonate species

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-02-05 DOI: 10.1016/j.apcata.2024.120075

Jiacheng Xu , Jing Zhang , Lihua Xu , Shi Wang , Shuiliang Yao

Strong metal support interaction (SMSI) between precious metals and metal oxide support is an effective strategy to improve catalyst activity. However, the interfacial effects of SMSI on the catalyst surface are not clear. In this paper, Pt/MnO₂ catalysts with different MnO₂ crystal structures (β- and γ-) are used as research objects, and operando TPR-DRIFTS-MS is used as characterization technique. Pt/β-MnO₂ exhibited the highest CO oxidation activity (200 °C) and CO₂ selectivity (100 °C) due to its excellent redox properties. Among them, β-MnO₂ surface Pt mainly exists in the form of elemental Pt, while γ-MnO₂ surface Pt mainly exists in the form of PtO₂. Different forms of Pt have positive and negative effects on different MnO₂ crystals. DFT results show that Pt/β-MnO₂ has strong adsorption capacity for CO. Operando DRIFTS results indicate that Pt/β-MnO₂ surface PtO first reacts with CO to produce PtO_v (O_v represent oxygen vacancy) at low temperature. As the temperature rises, MnO and Pt-O-Mn also participate in CO reaction, forming MnO_v, Pt-O_v-Mn and gas-phase CO₂. It is worth noting that the formation of Pt-O_v-Mn plays an important role in the activation of O₂. The surface carbonate of the catalyst inhibited the activation of Pt-O_v-Mn. More PtO sites are conducive to the production of monodentate carbonate and the easier decomposition at low temperature, which is the decisive step of CO oxidation. These findings provide strong support for understanding the effect of SMSI effect on the intrinsic configuration of catalysts.

{"title":"Revealing the positive and negative effects of strong metal support interactions on CO oxidation for Pt-supported different crystals (β- and γ-) MnO2 catalysts: Pt oxides and carbonate species","authors":"Jiacheng Xu , Jing Zhang , Lihua Xu , Shi Wang , Shuiliang Yao","doi":"10.1016/j.apcata.2024.120075","DOIUrl":"10.1016/j.apcata.2024.120075","url":null,"abstract":"<div><div>Strong metal support interaction (SMSI) between precious metals and metal oxide support is an effective strategy to improve catalyst activity. However, the interfacial effects of SMSI on the catalyst surface are not clear. In this paper, Pt/MnO2 catalysts with different MnO2 crystal structures (β- and γ-) are used as research objects, and operando TPR-DRIFTS-MS is used as characterization technique. Pt/β-MnO2 exhibited the highest CO oxidation activity (200 °C) and CO2 selectivity (100 °C) due to its excellent redox properties. Among them, β-MnO2 surface Pt mainly exists in the form of elemental Pt, while γ-MnO2 surface Pt mainly exists in the form of PtO2. Different forms of Pt have positive and negative effects on different MnO2 crystals. DFT results show that Pt/β-MnO2 has strong adsorption capacity for CO. Operando DRIFTS results indicate that Pt/β-MnO2 surface Pt<img>O first reacts with CO to produce Pt<img>Ov (Ov represent oxygen vacancy) at low temperature. As the temperature rises, Mn<img>O and Pt-O-Mn also participate in CO reaction, forming Mn<img>Ov, Pt-Ov-Mn and gas-phase CO2. It is worth noting that the formation of Pt-Ov-Mn plays an important role in the activation of O2. The surface carbonate of the catalyst inhibited the activation of Pt-Ov-Mn. More Pt<img>O sites are conducive to the production of monodentate carbonate and the easier decomposition at low temperature, which is the decisive step of CO oxidation. These findings provide strong support for understanding the effect of SMSI effect on the intrinsic configuration of catalysts.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"691 ","pages":"Article 120075"},"PeriodicalIF":4.7,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143135100","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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Applied Catalysis A: General

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