Catalysis Science & Technology最新文献

{"title":"Computational thermostability engineering of a nitrile hydratase using synergetic energy and correlated configuration for redesigning enzymes (SECURE) strategy†","authors":"Jinling Xu, Haisheng Zhou, Jiaqi Xu, Ziyuan Wang, Zhonglang Yu, Zhe Wang, Hongyu Zhang, Haoran Yu, Jianping Wu and Lirong Yang","doi":"10.1039/D3CY01102J","DOIUrl":"https://doi.org/10.1039/D3CY01102J","url":null,"abstract":"<p >Nitrile hydratase (NHase), an excellent biocatalyst, has been widely used for the production of amides, but the exothermic hydration reaction leads to its rapid inactivation, hindering its industrial applications, which requires the thermostability of NHase to be enhanced. In this study, employing NHase from <em>Bordetella petrii</em> DSM 12804 (NHAB) as the object, a computational strategy using synergetic energy and correlated configuration for redesigning enzymes (SECURE) was proposed to prune the reasonable mutant library and assemble effective single mutations, thus maximizing the thermostability of NHAB. Among the mutants, the best variant, A6M/B4M, combined six mutations in its α-subunit (S30T, A71D, A74D, A78R, S81T, and A133P) and four mutations in its β-subunit (L25F, G27Y, N59P, and A173N), showing an increase in <em>T</em><small>_m</small> by 13.2 °C, an 866.0-fold prolonged half-life at 50 °C, and an 11.2% increase in activity. Then, the catalytic efficiency dramatically increased to 249.5 g L<small>⁻¹</small> acrylamide in 5 batches compared with that of 166.5 g L<small>⁻¹</small> by the wild type in 3 batches. Finally, the synergistic effect on the mutant represented by an overall change in structure and newly formed intermolecular interactions through dynamic simulations accounted for the enhanced thermostability. Thus, SECURE was demonstrated to be practical for the redesign of multimeric NHase, which also provided guidance for computational thermostability engineering of other industrial biocatalysts.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 20","pages":" 5880-5891"},"PeriodicalIF":5.0,"publicationDate":"2023-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41228562","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Investigation of the effect of thermal annealing of Ni-cobaltite nanoparticles on their structure, electronic properties and performance as catalysts for the total oxidation of dimethyl ether†","authors":"Daniel Onana Mevoa, Stephane Kenmoe, Muhammad Waqas, Dick Hartmann Douma, Daniel Manhouli Daawe, Katia Nchimi Nono, Ralph Gebauer and Patrick Mountapmbeme Kouotou","doi":"10.1039/D3CY00807J","DOIUrl":"https://doi.org/10.1039/D3CY00807J","url":null,"abstract":"&lt;p &gt;Herein, we report the influence of thermal annealing on the structural and redox properties, optical band gap (&lt;em&gt;E&lt;/em&gt;&lt;small&gt;&lt;sup&gt;Opt&lt;/sup&gt;&lt;/small&gt;&lt;small&gt;&lt;sub&gt;g&lt;/sub&gt;&lt;/small&gt;) and electrical conductivity (&lt;em&gt;σ&lt;/em&gt;) of Ni-doped Co&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt;O&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt; nanoparticles (NPs). The influence of annealing on the catalytic performance is also studied. Coprecipitation technique was employed to prepare single oxides (Ni&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt; and Co&lt;small&gt;&lt;sub&gt;3&lt;/sub&gt;&lt;/small&gt;O&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt;) and Ni-cobaltite oxides (NiCo&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt;), which were annealed at different temperatures. The samples were characterized in terms of structure (XRD), surface specific area (&lt;em&gt;S&lt;/em&gt;&lt;small&gt;&lt;sub&gt;BET&lt;/sub&gt;&lt;/small&gt;), morphology (SEM), chemical composition (EDS/XPS), redox properties (H&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;-TPR), optical band gap (&lt;em&gt;E&lt;/em&gt;&lt;small&gt;&lt;sup&gt;Opt&lt;/sup&gt;&lt;/small&gt;&lt;small&gt;&lt;sub&gt;g&lt;/sub&gt;&lt;/small&gt;) and conductivity &lt;em&gt;σ&lt;/em&gt;. In addition, the conversion of dimethyl ether (DME) was achieved over all samples at low temperature. Overall, NiCo&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt; exhibits outstanding catalytic behaviour, surpassing single oxides. However, a notable difference in performance among NiCo&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt; samples was observed. The catalytic behaviour is discussed with respect to the quality of reducibility, the ratio of active species (O&lt;small&gt;&lt;sub&gt;Lat&lt;/sub&gt;&lt;/small&gt;/O&lt;small&gt;&lt;sub&gt;Ads&lt;/sub&gt;&lt;/small&gt;), the lowest &lt;em&gt;E&lt;/em&gt;&lt;small&gt;&lt;sup&gt;Opt&lt;/sup&gt;&lt;/small&gt;&lt;small&gt;&lt;sub&gt;g&lt;/sub&gt;&lt;/small&gt; and the good &lt;em&gt;σ&lt;/em&gt;. H&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;-TPR, &lt;em&gt;E&lt;/em&gt;&lt;small&gt;&lt;sup&gt;Opt&lt;/sup&gt;&lt;/small&gt;&lt;small&gt;&lt;sub&gt;g&lt;/sub&gt;&lt;/small&gt; and &lt;em&gt;σ&lt;/em&gt; analysis were used to gain a deeper insight into the reaction process occurring at the surface of each of the catalysts. NiCo&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt; samples annealed at 450 and 500 °C cannot be reduced in the reaction temperature range (150 to 225 °C), suggesting that the process occurs &lt;em&gt;via&lt;/em&gt; a surface mechanism. However, NiCo&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt; annealed at 350 °C is reduced under the reaction conditions within the temperature range from 200 to 350 °C, attesting that DME oxidation proceeds through an intrafacial redox process in this case. Using density functional theory (DFT) calculations, the adsorption and dissociation of DME on the catalytically relevant NiCo&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;O&lt;small&gt;&lt;sub&gt;4&lt;/sub&gt;&lt;/small&gt; (001) surface was investigated. DME adsorbs preferentially on top the Co&lt;small&gt;&lt;sup&gt;3+&lt;/sup&gt;&lt;/small&gt; site in a degenerate state: intact and single dehydrogenated molecules have very similar binding energies (−0.76 eV and −0.77 eV, respectively). The presence of surface vacancies in the vicinity of the adsorption site leads to the most interesting catalytic pathway. The activatio","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 20","pages":" 6041-6058"},"PeriodicalIF":5.0,"publicationDate":"2023-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41228582","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Phosphating core–shell graphdiyne/CuI/Cu3P S-scheme heterojunction confirmed with in situ XPS characterization for efficient photocatalytic hydrogen production†","authors":"Jie He, Xinyu Miao, Youlin Wu and Zhiliang Jin","doi":"10.1039/D3CY00850A","DOIUrl":"https://doi.org/10.1039/D3CY00850A","url":null,"abstract":"<p >Graphdiyne (GDY), a new 2D hybrid carbon material, has been praised for its distinct structure and chemical properties since its synthesis in 2010. In recent years, graphdiyne has been continuously applied and studied in photocatalysis, where it has shown excellent photocatalytic performance. In this paper, the core–shell encapsulated ternary catalyst graphdiyne/CuI/Cu<small>₃</small>P is obtained by phosphatizing the partial CuI phosphate on the outer surface to Cu<small>₃</small>P. The calcined ternary catalysts are closely connected with each other, with larger contact area, more active sites and faster electron transfer efficiency, thus greatly improving the hydrogen evolution rate. The double S-scheme heterojunction structure can effectively separate electron holes and induce the directional migration of electrons, maintaining the best redox ability of the catalyst to achieve more effective photocatalytic hydrogen evolution reactions. Graphdiyne/CuI/Cu<small>₃</small>P showed good hydrogen evolution efficiency, and the H<small>₂</small> production efficiency was conspicuously improved. In this work, the structure and energy band of the catalyst were studied through <em>in situ</em> XPS and DFT calculations, among others, to verify the possible formation of a double S-scheme heterojunction between graphdiyne, cuprous iodide and cuprous phosphide. The preparation method of the catalysts is simple and effective, providing ideas and strategies for designing high-performance catalysts.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5610-5624"},"PeriodicalIF":5.0,"publicationDate":"2023-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41084809","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Three-dimensional ordered macroporous cerium–manganese composite oxide for NO oxidation†","authors":"Canyang Qu, Ping Wang, Miao He, Cheng Yang, Jing Xiong, Xiaohua Sun, Yuechang Wei and Zhenxing Li","doi":"10.1039/D3CY01059G","DOIUrl":"https://doi.org/10.1039/D3CY01059G","url":null,"abstract":"<p >NO<small>_<em>x</em></small> is one of the main sources of air pollution, which primarily comes from automobile exhausts. Rare earth-based catalysts for NO oxidation have excellent oxygen storage and release performance and good structural stability. Herein, a series of three-dimensional ordered microporous (3DOM) cerium–manganese composite oxide catalysts with different cerium–manganese ratios for NO oxidation were prepared by the sol–gel method. The 3DOM structure improves the contact efficiency of the NO, soot and the catalyst. By incorporating Mn<small>³⁺</small> ions into the cerium oxide lattice, a Ce–Mn solid solution forms with an ordered macroporous structure, and the interaction between cerium and manganese significantly increases the amount of reactive oxygen species. The catalyst with the optimal cerium–manganese ratio (1 : 2) was able to achieve a conversion rate of 62% at 250 °C, and the highest conversion rate reached 98%, which is far higher than pure cerium oxide and pure manganese oxide catalysts. This work provides a promising catalyst for NO oxidation and soot combustion applications.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 20","pages":" 5989-5997"},"PeriodicalIF":5.0,"publicationDate":"2023-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41228592","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Iron-catalysed highly selective hydroalkoxycarbonylation of alkynes using CO as C1 source†","authors":"Tanuja Tewari, Rohit Kumar and Samir H. Chikkali","doi":"10.1039/D3CY00843F","DOIUrl":"https://doi.org/10.1039/D3CY00843F","url":null,"abstract":"<p >Though precious and rare, late-transition metals have been extensively used in metal-catalysed carbonylation reactions in organic transformations. On the other hand, base metals are abundant and cheap, but their practical utilization in carbonylation reactions is rarely explored. Here, we report iron-catalysed hydroalkoxycarbonylation of alkynes to α,β-unsaturated esters in one pot. A readily available iron precursor [Fe<small>₂</small>(CO)<small>₉</small>] in the presence of a diimine ligand <strong>L7</strong> catalyzes the conversion of alkynes to α,β-unsaturated esters under 10 bar CO pressure. This operationally simple protocol tolerates various functional groups and allows facile access to about 40 α,β-unsaturated esters. The synthetic utility of the reaction has been demonstrated by scaling up the reaction to 1 g and by preparing sunscreen/antifungal agents. The kinetic study suggests that the reaction is an approximate 1st order with respect to the iron catalyst, and the initial rate of the reaction is 3.6 × 10<small>⁻²</small> M h<small>⁻¹</small>. Mechanistic investigations using NMR spectroscopy indicated the existence of an [Fe–H] intermediate, and control experiments using a radical trapping reagent and EPR revealed the absence of any radical species in the reaction.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5549-5555"},"PeriodicalIF":5.0,"publicationDate":"2023-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41084779","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tuning of the electronic, photocatalytic and optical properties of Janus XWAZ2 (X = S, Se, Te; A = Si, Ge; Z = N, P, As) monolayers via strain and external electric field†","authors":"Zhen Gao, Xin He, Yao He and Kai Xiong","doi":"10.1039/D3CY00901G","DOIUrl":"https://doi.org/10.1039/D3CY00901G","url":null,"abstract":"<p >Owing to their unique structure and properties, two-dimensional Janus materials have garnered significant attention in the field of photocatalytic water decomposition. In this study, we have conducted a comprehensive investigation of the stability, photocatalytic, and optical properties of monolayer 2D Janus XWAZ<small>₂</small> (X = S, Se, Te; A = Si, Ge; Z = N, P, As) using first-principles calculations. Our findings reveal that the inherent dipole of Janus XWAZ<small>₂</small> induces noticeable band bending, resulting in favorable band edge positions and making it an effective photocatalyst. The internal electric field in the structure efficiently separates electrons and holes on different surfaces, effectively suppressing recombination and ensuring high photocatalytic activity. In addition, we explored the modulation of the band gap of the XWAZ<small>₂</small> (X = S, Se, Te; A = Si, Ge; Z = N, P, As) monolayer through biaxial strain and applied an external electric field, further tuning its photocatalytic and optical properties. This study provides valuable insights into the photocatalytic water-splitting of Janus structures and paves the way for future research in this field.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5718-5733"},"PeriodicalIF":5.0,"publicationDate":"2023-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41084818","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Insights into the synergistic catalytic mechanism on the customized dual sites of an efficient ORR catalyst†","authors":"Jinyu Zhao, Xu Chen, Jie Lian, Yu Gao, Yixing Zhang and Xiaomin Wang","doi":"10.1039/D3CY01066J","DOIUrl":"https://doi.org/10.1039/D3CY01066J","url":null,"abstract":"<p >PtCo alloys as compelling catalysts for the oxygen reduction reaction (ORR) have been loaded on heteroatom-modified carbon carriers in recent years to modulate their electronic structure and influence their interaction with intermediates. However, the actual active sites remain unclear and their interaction with intermediates is still controversial. Herein, PtCo/PC catalysts were synthesized by loading PtCo alloys on P-modified carbon carriers, and their catalytic mechanism was investigated using <em>in situ</em> Raman spectroscopy. In the results, the distorted and disordered PtCo alloy sites and the P-C defect sites are pinpointed and clarified as the double active sites for such catalysts. Among which, PtCo/PC-2 has the most abundant active sites, an optimal hierarchical porous structure, and the strongest Co–P binding, thereby showing ORR activity and stability. Combined with <em>in situ</em> Raman analysis, it exposits that the doped P atom in PtCo/PC-2 possesses strong electron-donating ability, which indirectly helps Pt function as an electron reservoir to donate electrons for OOH* on PtCo alloy sites, and directly weakens the adsorption energy of OOH* on P–C defect sites. Furthermore, the dynamic evolution of OOH* discloses that the double active sites on PtCo/PC-2 synergistically promote the ORR process <em>via</em> an associative pathway.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 20","pages":" 5959-5968"},"PeriodicalIF":5.0,"publicationDate":"2023-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41228589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Correction: Design of gold catalysts for activation of H2 and H-donor molecules: transfer hydrogenation and CO2 hydrogenation","authors":"Jhonatan Luiz Fiorio, Lais Reis Borges, Tomaz Neves-Garcia, Danielle Kimie Kikuchi, Raíza Rosa Garcia Guerra and Liane Marcia Rossi","doi":"10.1039/D3CY90065G","DOIUrl":"https://doi.org/10.1039/D3CY90065G","url":null,"abstract":"<p >Correction for ‘Design of gold catalysts for activation of H<small>₂</small> and H-donor molecules: transfer hydrogenation and CO<small>₂</small> hydrogenation’ by Jhonatan Luiz Fiorio <em>et al.</em>, <em>Catal. Sci. Technol.</em>, 2023, <strong>13</strong>, 3205–3215, https://doi.org/10.1039/D2CY01920E.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 18","pages":" 5462-5463"},"PeriodicalIF":5.0,"publicationDate":"2023-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2023/cy/d3cy90065g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"7164191","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Crystal facet dependence of the ketonization of propionic acid on anatase TiO2†","authors":"Jiao Huang, Liwen Li, Xiaoxia Wu, Yonghua Guo, Zijun Yang, Hua Wang, Qingfeng Ge and Xinli Zhu","doi":"10.1039/D3CY00917C","DOIUrl":"https://doi.org/10.1039/D3CY00917C","url":null,"abstract":"<p >Exploring reactions on well-defined surfaces may contribute to a better understanding of structure–activity relationships for metal oxide-mediated reactions. Herein, anatase TiO<small>₂</small> with predominantly exposed (101), (100) and (001) facets were synthesized and tested for vapor-phase ketonization of propionic acid. The intrinsic ketonization rates based on both mass and surface area at 350 °C increase following the order of TiO<small>₂</small>(100) &lt; TiO<small>₂</small>(101) &lt; TiO<small>₂</small>(001), with the corresponding turnover frequency based on the density of the acid–base pair being 51.8, 71.3, and 185.2 h<small>⁻¹</small>, respectively. The ketonization rate cannot be correlated with either acid/base property or concentration of oxygen vacancies, but an integral band intensity ratio of monodentate/bidentate propionate, suggesting that the monodentate configuration is likely the more reactive intermediate toward C–C coupling. Density functional theory calculation of propionic acid adsorption indicates that the high activity of ketonization results from the longer shortest Ti<small>_5c</small>–Ti<small>_5c</small> distance, and the square arrangement of surface Ti<small>_5c</small> centers in the nearly flat surface of the (001) facet. These results indicate that the surface geometrical structure of the metal oxide plays a crucial role in the ketonization of carboxylic acids, and the minority (001) facet on the surface may predominantly contribute to the overall activity in ketonization on anatase TiO<small>₂</small>. Our results also suggest that facet engineering may greatly enhance the C–C coupling reactions mediated on the acid–base pair of the metal oxide.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 20","pages":" 5924-5937"},"PeriodicalIF":5.0,"publicationDate":"2023-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41228586","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Direct methylation of benzene with methane over Co/MFI catalysts generated by self-dispersion of Co(OH)2†","authors":"Kazu Okumura, Kai Tanaka, Akimichi Ohtsuki, Hikaru Iiyoshi and Naonobu Katada","doi":"10.1039/D3CY00305A","DOIUrl":"https://doi.org/10.1039/D3CY00305A","url":null,"abstract":"<p >A methane–benzene reaction was performed over Co/MFI prepared with an aqueous solution of Co(OAc)<small>₂</small> and MFI zeolite. Co(OH)<small>₂</small> was deposited on the MFI zeolite when the Co(OAc)<small>₂</small> solution was stirred at 343 K in the presence of MFI. A decline of the h-peak in NH<small>₃</small> TPD occurred during the loading of Co on MFI. Further thermal treatment at 573–773 K caused the spontaneous formation of the atomically dispersed Co species, which was observed with Co K-edge XAFS. The toluene formation rate of the catalyst prepared with Co(OAc)<small>₂</small> was proportional to the Co loading and was higher than that prepared with Co(NO<small>₃</small>)<small>₂</small> due to the large amount of supported Co.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 20","pages":" 5969-5977"},"PeriodicalIF":5.0,"publicationDate":"2023-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41228590","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}