Molecular Catalysis最新文献_第8页

Insight into SO2 poisoning mechanism of MnOx-CeO2/Ti-bearing blast furnace slag catalyst for low temperature NH3-SCR reaction 低温 NH3-SCR 反应中 MnOx-CeO2/Ti 轴高炉矿渣催化剂的 SO2 中毒机理探析

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-10-18 DOI: 10.1016/j.mcat.2024.114609

Ming Kong , Heping Liao , Linjiang Song , Shengchao Zhang , Yunchuan Wang , Wei Feng , Zhifang Liu , Xianling Deng , Lu Yao , Handan Zhang

{"title":"Insight into SO2 poisoning mechanism of MnOx-CeO2/Ti-bearing blast furnace slag catalyst for low temperature NH3-SCR reaction","authors":"Ming Kong , Heping Liao , Linjiang Song , Shengchao Zhang , Yunchuan Wang , Wei Feng , Zhifang Liu , Xianling Deng , Lu Yao , Handan Zhang","doi":"10.1016/j.mcat.2024.114609","DOIUrl":"10.1016/j.mcat.2024.114609","url":null,"abstract":"<div><div>Sulfur poisoning is an intractable challenge for NH3-SCR catalyst. In this issue, the immanent reasons for MnOx-CeO2/Ti-bearing blast furnace slag catalyst deactivation resulting from SO2 were elaborated by catalytic activity evaluation, BET, XRD, XPS, NH3-TPD, H2-TPR and in-situ DRIFTS analysis. Results showed that MnOx-CeO2/Ti-bearing blast furnace slag catalyst followed E-R reaction mechanism and performed 100 % NO conversion at 175 °C, whereas its sulfur resistance was unsatisfactory and the deactivation degree became more severe with SO2 concentration increasing. SO2 reacted with NH3 to generate (NH4)2SO4 and NH4HSO4 deposits, blocking catalyst pores and covering active sites. SO2 also interacted with MnOx-CeO2 active components to form MnSO4 and Ce2(SO4)3, which restricted the electron transfers of Mn4+/Mnn+ and Ce3+/Ce4+. Besides, the newly formed sulfur-containing acidic sites also competed with the original active sites for NH3 adsorption, thereby hindering the SCR reaction. Physical purging could not realize regeneration of SO2-poisoning catalyst, but hyperthermic treatment was an efficient solution.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"569 ","pages":"Article 114609"},"PeriodicalIF":3.9,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142554857","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

Use of red-mud (MRM) in industrial catalysis: Selective conversion of biomass derived furfural to furfuryl alcohol using Ni-MRM – preparation, characterization and activity studies – elucidating mechanism of hydrogenation using DFT 在工业催化中使用红泥（MRM）：利用 Ni-MRM 将生物质衍生的糠醛选择性转化为糠醇--制备、表征和活性研究--利用 DFT 阐明氢化机理

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-10-18 DOI: 10.1016/j.mcat.2024.114617

Subhashree Mishra , Neha Kamal , Arup Kumar De , Indrajit Sinha , Amulya Prasad Panda , R.K. Dey , Rajaram Bal

{"title":"Use of red-mud (MRM) in industrial catalysis: Selective conversion of biomass derived furfural to furfuryl alcohol using Ni-MRM – preparation, characterization and activity studies – elucidating mechanism of hydrogenation using DFT","authors":"Subhashree Mishra , Neha Kamal , Arup Kumar De , Indrajit Sinha , Amulya Prasad Panda , R.K. Dey , Rajaram Bal","doi":"10.1016/j.mcat.2024.114617","DOIUrl":"10.1016/j.mcat.2024.114617","url":null,"abstract":"<div><div>Conversion of furfural (FFL) to furfuryl alcohol (FOL) using nickel loaded modified red mud (Ni-MRM) was developed with an aim to eliminate toxic Cu-Cr catalyst or precious metal catalyst currently used industrially. Ni-MRM was characterized using various advanced instruments such as XRD, TEM, TPR, BET and XPS. Thermal stability of the material was computed using Kissinger-Akahira-Sonuse (KAS) model. Ni-MRM catalytic activity was studied with variation of parameters. A 15 % Ni-loading on MRM (Ni(15 %)-MRM) shows significant product selectivity (>90 %) in optimized reaction conditions. Density functional theory (DFT) was used for calculation of adsorption energy, charge of the metal at the material active sites. The theoretical calculation shows that H2 molecule adsorbed upon electron rich Ni surface facilitate bond cleavage to initiate the reaction with adsorbed furfural molecule. Ni-MRM could be reused without significant loss of material catalytic activity for production of furfuryl alcohol. The work also shows effective utilization of properties of red mud for selective transformation of furfural, a bio-renewable material, to value added products.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"569 ","pages":"Article 114617"},"PeriodicalIF":3.9,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142554800","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

Enhanced Lewis acidity on modified H-ZSM-5 catalysed 5-hydroxymethylfurfural oxidation in aqueous solvent 改性 H-ZSM-5 在水性溶剂中催化 5- 羟甲基糠醛氧化时增强的路易斯酸性

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-10-17 DOI: 10.1016/j.mcat.2024.114610

Rahul Gautam, Neeraj Sharma, Kanika Saini, Shunmugavel Saravanamurugan

引用次数: 0

Co-N-C catalyst with single atom active sites for base-free aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid under mild conditions 具有单原子活性位点的 Co-N-C 催化剂，用于在温和条件下将 5-羟甲基糠醛无碱有氧氧化为 2,5-呋喃二甲酸

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-10-17 DOI: 10.1016/j.mcat.2024.114616

Sohaib Hameed , Xiaoli Pan , Weixiang Guan , Aiqin Wang

引用次数: 0

Regulating the location relationship between Cu nanoparticles and Pt atoms to enhance the catalytic hydroisomerization performance: Together or apart? 调节铜纳米颗粒与铂原子之间的位置关系，提高催化加氢异构化性能：在一起还是分开？

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-10-17 DOI: 10.1016/j.mcat.2024.114620

Hao Qin, Hui Wan, Guofeng Guan

{"title":"Regulating the location relationship between Cu nanoparticles and Pt atoms to enhance the catalytic hydroisomerization performance: Together or apart?","authors":"Hao Qin, Hui Wan, Guofeng Guan","doi":"10.1016/j.mcat.2024.114620","DOIUrl":"10.1016/j.mcat.2024.114620","url":null,"abstract":"<div><div>Single atom catalysts have been recently reported as the efficient catalysts for hydroisomerization compared to the conventional nanoparticle catalyst. Despite the fascinating advantage in enhancing the metal activity or reducing the catalyst cost, the long-term stability of the single atom catalyst seemed not that satisfactory, especially when reacting under atmospheric pressure. Herein, Pt single atom catalysts were combined with Cu nanoparticles by different means to explore a new way to improve the catalytic performance. Cu nanoparticles were located away from Pt sites to form a binary catalyst, or acted as the support of Pt atoms to form a single atom alloy (SAA) catalyst. With the binary catalyst Pt1–0.1Cu@CS, the conversion of the n-heptane after time on stream of 50 h increased to 70.3 %, higher than Pt1@CS (47.3 %). Besides, excessive Cu nanoparticles in the binary catalyst were found rather harmful to the catalysis instead. However, the SAA catalyst Pt1Cu@SAPO-11 showed a poor activity in hydroisomerization compared to Pt1@CS, indicating that the alloy structure should go against the activation of reactant. The roles of Pt atoms and Cu nanoparticles in different catalysts were discussed in detail. The reaction mechanism of hydroisomerization was refined with the different functions of the dual metal sites. This work might be instructive for the design of single atom catalysts combined with metal nanoparticles.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"569 ","pages":"Article 114620"},"PeriodicalIF":3.9,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142446443","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

Engineering the structure defects of ceria-zirconia-praseodymia solid solutions for diesel soot catalytic elimination 利用铈-氧化锆-镨固溶体的结构缺陷来催化消除柴油机烟尘

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-10-16 DOI: 10.1016/j.mcat.2024.114623

Dezhou Luo , Na Zhang , Chunying Chen , Zhi Chen , Sisi Qin , Qin He , Zhengzheng Yang

{"title":"Engineering the structure defects of ceria-zirconia-praseodymia solid solutions for diesel soot catalytic elimination","authors":"Dezhou Luo , Na Zhang , Chunying Chen , Zhi Chen , Sisi Qin , Qin He , Zhengzheng Yang","doi":"10.1016/j.mcat.2024.114623","DOIUrl":"10.1016/j.mcat.2024.114623","url":null,"abstract":"<div><div>Creating structure defects in ceria-based solid solution catalysts is a crucial yet challenging task. Herein, urea-assisted synthesis strategy was designed for ceria-zirconia-praseodymia catalyst (CeZrPrOx) to create lattice defects; its effects on catalyst structure, physical-chemical properties and catalytic diesel soot purification activity were systematically investigated. Raman and X-ray photoelectron spectroscopy (XPS) findings indicate that the urea-assisted synthesized catalyst (CeZrPrOx-U) has remarkably more Ce3+ proportion (structure defects), oxygen vacancies and surface reactive oxygen species (O22- and O2-). Temperature-programmed reduction by hydrogen (H2-TPR) and temperature-programmed desorption by oxygen (O2-TPD) results further prove that the oxygen migration of the CeZrPrOx-U is definitely enhanced. Compared to the conventional CeZrPrOx catalyst, the bulk lattice oxygen of the CeZrPrOx-U can be migrated to the surface to generate surface reactive oxygen species more easily. As a consequence, the prepared CeZrPrOx-U catalyst exhibits obviously better catalytic diesel soot purification activity. Therefore, this study suggests that engineering the structure defects in CeZrPrOx catalyst is an effective approach to improve physical-chemical properties and enhance the soot catalytic elimination activity of the catalyst.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"569 ","pages":""},"PeriodicalIF":3.9,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142442085","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

What size of Cun clusters loaded on poly(heptazine imide) have better catalytic performance for acetylene semi-hydrogenation? 在聚(庚嗪亚胺)上负载多大尺寸的 Cun 簇对乙炔半加氢具有更好的催化性能？

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-10-13 DOI: 10.1016/j.mcat.2024.114605

Xiaoxiao Chen , Yi Li , Yaofeng Yuan , Wei Lin

{"title":"What size of Cun clusters loaded on poly(heptazine imide) have better catalytic performance for acetylene semi-hydrogenation?","authors":"Xiaoxiao Chen , Yi Li , Yaofeng Yuan , Wei Lin","doi":"10.1016/j.mcat.2024.114605","DOIUrl":"10.1016/j.mcat.2024.114605","url":null,"abstract":"<div><div>Development of earth-abundant, low-cost and easily synthesizable catalysts for the semi-hydrogenation of acetylene is urgently needed. Here, we have systematically investigated the structure, electronic properties, hydrogen dissociation, and acetylene semi-hydrogenation activity and selectivity of poly(heptazine imide) (PHI) loaded with different sizes of Cun (n = 1,2,4,13) clusters (Cun/PHI) by density functional theory calculations. The results show that Cu4/PHI with tetrahedral configuration has a better hydrogenation activity in the acetylene semi-hydrogenation reaction with H adsorbed in the vicinity of acetylene and subsequent intermediates in a non-bridge position, resulting in a smaller hydrogenation energy barrier. In addition, the top Cu atom transfers a large number of electrons to the bottom Cu atoms and PHI, and only a small number of electrons transfer to ethylene, resulting in weak adsorption of ethylene and easy desorption, which makes it good selectivity and therefore it can be used as a candidate catalyst for the semi-hydrogenation of acetylene. This study provides insights into the design of catalysts with suitable size clusters loaded on carbon nitride materials for efficient acetylene semi-hydrogenation reactions.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"569 ","pages":"Article 114605"},"PeriodicalIF":3.9,"publicationDate":"2024-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142433652","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

F127 assisted synthesis of Bi promoted Co3O4 catalyst for catalyzing N2O decomposition in presence of impurity gases F127 辅助合成用于在杂质气体存在时催化 N2O 分解的 Bi 促进 Co3O4 催化剂

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-10-13 DOI: 10.1016/j.mcat.2024.114604

Keyi Wang, Yuanting Du, Yang Li, Xingkun Qi, Weijun Shan, Haibiao Yu, Ying Xiong

{"title":"F127 assisted synthesis of Bi promoted Co3O4 catalyst for catalyzing N2O decomposition in presence of impurity gases","authors":"Keyi Wang, Yuanting Du, Yang Li, Xingkun Qi, Weijun Shan, Haibiao Yu, Ying Xiong","doi":"10.1016/j.mcat.2024.114604","DOIUrl":"10.1016/j.mcat.2024.114604","url":null,"abstract":"<div><div>In this paper, Bi promoted Co3O4 catalysts used for catalyzing N2O decomposition were successfully prepared by improved sol-gel method with the assistance of F127. It was found that the doping of additive Bi not only did not change the unique “Yardang Landform” microstructure of the 3.0F-Co3O4, but also prompted Co3O4 to expose more active crystal planes, such as (422), (533) and (620). Moreover, the doping of the additive Bi also enhanced the catalyst's specific surface area, and further weakened the surface Co-O bond. The optimum 3.0F-Bi0.015Co catalyst achieved >88 % N2O conversion (2000 ppmv N2O/Ar, GHSV=20,000 h−1) at 300 °C, and its corresponding TOF value increased from 1.50 × 10−3 s−1 for 3.0F-Co3O4 to 3.63 × 10−3 s−1. Meanwhile, the Ea of 3.0F-Bi0.015Co was as low as 47.0 kJ mol−1. Most importantly, the catalyst has good resistance to O2 and H2O. Under the harsh condition (both 5 vol.% O2, 100 ppmv NO and 2 vol.% H2O were coexisted in the reaction system), the N2O conversion over the 3.0F-Bi0.015Co catalyst can be stable above 90 % at 400 °C.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"569 ","pages":"Article 114604"},"PeriodicalIF":3.9,"publicationDate":"2024-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142433653","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

Unveiling the phenol direct carboxylation reaction mechanism at ZrO2 surface 揭示 ZrO2 表面苯酚直接羧化反应机理

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-10-13 DOI: 10.1016/j.mcat.2024.114606

Kaihua Zhang , Changru Ma , Sebastien Paul , Jeremie Zaffran

{"title":"Unveiling the phenol direct carboxylation reaction mechanism at ZrO2 surface","authors":"Kaihua Zhang , Changru Ma , Sebastien Paul , Jeremie Zaffran","doi":"10.1016/j.mcat.2024.114606","DOIUrl":"10.1016/j.mcat.2024.114606","url":null,"abstract":"<div><div>In the present context of environmental concerns, sustainable solutions must be proposed to dispose of waste CO2, a well-known greenhouse gas. Among the various emerging projects, upgrading CO2 molecule into high-value added chemicals appears to be very promising. More particularly, the carboxylation of aromatic compounds to (di-) acid aromatic monomers is of great interest for the high performance polymer industry. Focusing on the direct phenol carboxylation to para-hydroxybenzoic acid as a model reaction, the reactivity of ZrO2 was investigated in this paper, this material being recently reported in various experimental works for its catalytic efficiency. For the first time, we established the phenol carboxylation mechanism at the surface of a metal oxide material, showing that the reaction can only proceed through an Eley-Rideal mechanism. In this mechanism, CO2 is strongly chemisorbed at the surface, whereas phenol is physisorbed close to the CO2 adsorbate. Besides, while the monoclinic and the tetragonal phases often coexist in ZrO2 particles, we demonstrated that only the monoclinic geometry exhibits a substantial activity. However, the selectivity remains a major challenge, the ortho- isomer being the most abundant product, as in the original Kolbe-Schmitt method. While most of the processes generally reported in literature for the direct carboxylation of phenol are achieved in liquid media, a very few theoretical knowledge is available to describe such a process at solid surfaces. Therefore, we expect the present manuscript to be a pioneer work, aiming at providing a better understanding of metal oxide surface reactivity, paving the road to the rational design of efficient solid catalysts for aromatics carboxylation reactions.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"569 ","pages":"Article 114606"},"PeriodicalIF":3.9,"publicationDate":"2024-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142433651","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

Enhanced low-temperature methane oxidation over Pd supported Mn-doped NiO catalyst Pd 支持的掺锰 NiO 催化剂的低温甲烷氧化能力增强

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-10-13 DOI: 10.1016/j.mcat.2024.114611

Xiaoying Zhou , Shiyu Fang , Zihao Hu , Zuliang Wu , Jing Li , Wei Wang , Jiali Zhu , Shuiliang Yao , Erhao Gao

{"title":"Enhanced low-temperature methane oxidation over Pd supported Mn-doped NiO catalyst","authors":"Xiaoying Zhou , Shiyu Fang , Zihao Hu , Zuliang Wu , Jing Li , Wei Wang , Jiali Zhu , Shuiliang Yao , Erhao Gao","doi":"10.1016/j.mcat.2024.114611","DOIUrl":"10.1016/j.mcat.2024.114611","url":null,"abstract":"<div><div>This study introduces a novel catalyst system comprising Pd nanoparticles loaded onto Mn-doped NiO for the efficient oxidation of methane (CH4) at low temperatures. The loading of Pd nanoparticles onto the Mn-doped support has yielded a catalyst with exceptional activity and stability, as evidenced by the lowest T50 temperature of 276 °C and a CH4 conversion reaching 97% at 325 °C. The catalyst demonstrates optimized reaction kinetics with the lowest activation energy of 69.2 kJ mol–1. The catalyst's superior performance is attributed to the synergistic effects of the Pd/Mn-NiO composite, which include a higher Pd2+/Pd4+ ratio, increased adsorptive oxygen concentration (Oads/Ototal), and a reduced Ni3+/Ni2+ ratio. These characteristics collectively enhance the catalytic activity for CH4 oxidation. The Mars-van Krevelen mechanism underpins the oxidation process, with Pd2+ identified as the principal active site for CH4 adsorption and dissociation. Diffuse reflectance infrared Fourier transform spectroscopy coupled with mass spectrometry elucidates the pathway of surface reactive oxygen species in the formation of key intermediates, such as formates, and underscores the accelerated decomposition of carbonate facilitated by the Pd modification on the Mn-NiO surface. The findings signify a significant advancement in the development of catalysts for environmental and energy-related applications, particularly in the mitigation of CH4 emissions.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"569 ","pages":"Article 114611"},"PeriodicalIF":3.9,"publicationDate":"2024-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142433767","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