Catalysis TodayPub Date : 2024-11-10DOI: 10.1016/j.cattod.2024.115122
Mufeedah Muringa Kandy, Thasnim P Mohammed, Akhila George, Muniyandi Sankaralingam
{"title":"Biomimetic methodology as a sustainable tool for enhanced photocatalytic reduction of CO2","authors":"Mufeedah Muringa Kandy, Thasnim P Mohammed, Akhila George, Muniyandi Sankaralingam","doi":"10.1016/j.cattod.2024.115122","DOIUrl":"10.1016/j.cattod.2024.115122","url":null,"abstract":"<div><div>In this current technological world, the unrestrained release of CO<sub>2</sub> negatively impacts the atmosphere by global warming. The capture of CO<sub>2</sub> and converting it into accessible solar fuels is a prominent scientific and technological breakthrough that tackles both the rising climate change and energy crisis issues. The dual beneficial approach focusing on solar-energy-driven reduction of CO<sub>2</sub> to valuable energy fuels is one of the most promising sustainable strategies. In consideration of this, it has been recently observed that biomimetic strategies that incorporate intricate structural design with massive functional components offer a sustainable technological feature. Inspired by the remarkably efficient process of photosynthesis in nature, the fabrication of synthetic leaves for artificial photosynthesis emerges as an attractive avenue that addresses the dual challenges of climate change and energy scarcity with inventive and sustainable methods. This review deals with the fabrication of biomimetic materials with high surface area and efficient charge transfer mechanisms, to improve photocatalytic performance and develop sustainable solutions for CO<sub>2</sub> capture and conversion into solar fuels. The research highlights that the current challenges hinder the advancements of the process from its nascent stage and outlines future research endeavors necessary to elevate it from a rudimentary artificial leaf concept to a commercially viable artificial tree technology with significant industrial value.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"447 ","pages":"Article 115122"},"PeriodicalIF":5.2,"publicationDate":"2024-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142748446","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}
Catalysis TodayPub Date : 2024-11-08DOI: 10.1016/j.cattod.2024.115124
Mrinal Kanti Adak, Hirak Kumar Basak, Biswarup Chakraborty
{"title":"Establishing the oxygen evolution reaction pathway on iron-oxy-hydroxide through electro-kinetic study","authors":"Mrinal Kanti Adak, Hirak Kumar Basak, Biswarup Chakraborty","doi":"10.1016/j.cattod.2024.115124","DOIUrl":"10.1016/j.cattod.2024.115124","url":null,"abstract":"<div><div>Electrokinetic analyses harnessing intrinsic reaction parameters of the electrocatalytic oxygen evolution reaction (OER) shed light on the reaction mechanism. Given the superior stability of the iron oxy-hydroxide under alkaline OER conditions, α-FeO(OH) and γ-FeO(OH) are often found to be the active catalyst. Herein, nanocrystalline α-FeO(OH) and γ-FeO(OH) materials are used as catalysts to perform alkaline OER and detailed electrokinetic studies are conducted to establish the reaction pathway. The intrinsic parameters like anodic transfer coefficient (α<sub>a</sub>), specific exchange current density (j<sub>0,s</sub>), activation energy (<span><math><msubsup><mrow><mi>E</mi></mrow><mrow><mi>a</mi></mrow><mrow><mn>0</mn></mrow></msubsup></math></span>), and reaction order (m) are experimentally determined for both FeO(OH) phases. To obtain these important parameters, OER is performed with α-FeO(OH) and γ-FeO(OH) deposited on nickel foam as anode while varying the cell temperature from 298 K to 343 K and electrolyte concentrations from 0.05 M to 2.0 M KOH. The <em>j</em><sub><em>0,s</em></sub> values for α-FeO(OH) and γ-FeO(OH) are almost comparable 2.5 ± 0.5 × 10<sup>−3</sup> mA cm<sup>−2</sup> highlighting a similar rate of electron transfer. The activation energy barrier for OER on α-FeO(OH) and γ-FeO(OH) is identified to be 9.45 kJ mol<sup>−1</sup> and 8.06 kJ mol<sup>−1</sup>, respectively and the values are manyfold less compared to that observed for previously reported IrO<sub>2</sub> or NiFeO<sub>x</sub> materials emphasizing a faster kinetics on the FeO(OH) surface. The first-order reaction is determined from the electrolyte concentration variation suggesting the dissociation of O-H could be the rate-determining step (RDS) which is contrary to the mechanism proposed for IrO<sub>2</sub> or NiFeO<sub>x</sub> where the O-O bond formation was found to be rate-limiting. Extracting the intrinsic reaction parameters from the electro-kinetics study, the OER pathway on the FeO(OH) surface has been established here.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"446 ","pages":"Article 115124"},"PeriodicalIF":5.2,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142658823","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}
Catalysis TodayPub Date : 2024-11-07DOI: 10.1016/j.cattod.2024.115115
Lorena T. Pérez-Poyatos, Sergio Morales-Torres, Luisa M. Pastrana-Martínez, Francisco J. Maldonado-Hódar
{"title":"Sulfur-doped carbon/TiO2 composites for ethylene photo-oxidation. Enhanced performance by doping TiO2 phases with sulfur by mobile species inserted on the carbon support","authors":"Lorena T. Pérez-Poyatos, Sergio Morales-Torres, Luisa M. Pastrana-Martínez, Francisco J. Maldonado-Hódar","doi":"10.1016/j.cattod.2024.115115","DOIUrl":"10.1016/j.cattod.2024.115115","url":null,"abstract":"<div><div>The performance of carbon xerogel/TiO<sub>2</sub> composites in ethylene photo-oxidation was analyzed under dynamic conditions considering various parameters, namely sulfur doping, dry <em>vs.</em> humid conditions and type of radiation (ultraviolet, UV, <em>vs.</em> visible light, Vis). The catalysts were synthesized using an acid-catalyzed sol-gel process and characterized with complementary techniques, including SEM/EDX, XRD, XPS and physical adsorption of N<sub>2</sub> and CO<sub>2</sub>, among others. The performance of samples in ethylene removal by adsorption and photo-oxidation under dynamic flow was discussed and related with their physicochemical properties and the experimental conditions. Although ethylene adsorption was hindered by doping and humidity, both factors were found to enhance photoactivity by promoting the formation of highly oxidant hydroxyl radicals (HO<sup>•</sup>). The composites showed an improved catalytic performance compared to bare TiO<sub>2</sub>, with sulfur improving the activity by approximately 8 %. The presence of the carbon material also enhanced the performance under Vis radiation by nearly 25 %. It was suggested that sulfur species could migrate from the carbon support to the TiO<sub>2</sub> nanoparticles during carbonization, forming Ti-O-S bonds. This finding constitutes a novel, cost-effective, sustainable and scalable method for the preparation of supported and doped TiO<sub>2</sub> nanocomposites.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"446 ","pages":"Article 115115"},"PeriodicalIF":5.2,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142658792","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}
Catalysis TodayPub Date : 2024-11-06DOI: 10.1016/j.cattod.2024.115118
Mariana V. Rodrigues , Paloma Vinaches , Carla C. Polo , Marlon M. Silva , Ana F. Suzana , Wonsuk Cha , Sibele B. Pergher , Amélie Rochet , Florian Meneau
{"title":"In situ visualisation of zeolite anisotropic framework flexibility during catalysis","authors":"Mariana V. Rodrigues , Paloma Vinaches , Carla C. Polo , Marlon M. Silva , Ana F. Suzana , Wonsuk Cha , Sibele B. Pergher , Amélie Rochet , Florian Meneau","doi":"10.1016/j.cattod.2024.115118","DOIUrl":"10.1016/j.cattod.2024.115118","url":null,"abstract":"<div><div>Zeolites exhibit framework flexibility driving their chemical and catalytic properties. Since the zeolitic pores are extremely small, a slight strain generated in the crystal induces compelling changes in shape, connectivity, accessibility, and the framework chemical properties. These modifications affected the adsorption and desorption of reactants/products and the diffusion within the channels during reaction. Using <em>in situ</em> 3D Bragg coherent X-ray diffraction imaging, we unveil the dynamics of the zeolite structure during catalysis, contraction and/or expansion of its framework also known as zeolite framework flexibility. We imaged three-dimensionally a single faujasite zeolite crystal during the ethanol dehydration reaction revealing anisotropic lattice dynamics simultaneously to guest molecules formation. Understanding zeolite flexibility could permit to tune zeolites properties towards potentially higher adsorption and selectivity.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"446 ","pages":"Article 115118"},"PeriodicalIF":5.2,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142658797","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}
{"title":"Tetravalent metals modulated Zn-based layered double hydroxides and their mixed metal oxides for catalytic depolymerization of carbonyl-coordinating plastic waste","authors":"Savita Soni , Sonika Kumari , Ajay Sharma , Shashi Kant Bhatia , Anil Kumar Sharma","doi":"10.1016/j.cattod.2024.115136","DOIUrl":"10.1016/j.cattod.2024.115136","url":null,"abstract":"<div><div>Plastic waste generation has become a global issue and presents a significant challenge concerning degradability in the environment. This poses a serious threat and adverse impact on the health of living creature and the environment ecosystem. The up-/re-cycling of plastic waste through catalytic depolymerization is becoming a sustainable way to reduce economic concerns about production and serious environmental impacts. Here, in the present study an effort has been made for the development of catalysts for efficient recycling of carbonyl group containing polymer waste [Polyethylene terephthalate (PET) and polycarbonate (PC)]. The sequential preparation of ZnM<sup>IV</sup>- and ZnAlM<sup>IV</sup>- LDHs (layered double hydroxides) (M<sup>IV</sup>= Zr and Ti) and their respective mixed metal oxide (MMOs) based catalytic materials, has been carried out by one-pot co-precipitation and calcination methods. The structural parameters were examined through the various characterisation techniques including XRD, FTIR, TEM, SEM, and EDS. The layered structure, high crystalline nature and hexagonal 2D-sheet/flakes like morphology with average particle size ranging from ∼14–51 nm [for LDHs] and ∼6–21 nm [for MMOs] were observed. Depolymerization of PET and PC using LDHs/MMOs catalyst in ethylene glycols (EG) produced bis(2-hydroxyethyl terephthalate) (BHET) and bisphenol A (BPA) monomers as main products, respectively. The catalyst quantity, concentration of solvent, recyclability of catalysts, reaction duration, and crystallization time have also been further investigated for better yield during catalytic glycolysis. The isolated monomers were further characterized by using melting point, mass spectroscopy, <sup>1</sup>H NMR, <sup>13</sup>C NMR and FTIR analysis. The order of catalytic activities of prepared samples as ZnTi-LDH˃ ZnAlTi-LDH ˃ ZnTi-MMO˃ ZnAlZr-LDH˃ ZnAlTi-MMO˃ ZnZr-LDH in PET depolymerization while in case of PC, the order as ZnTi-LDH˃ ZnAlTi-LDH ˃ ZnZr-LDH˃ ZnAlZr-LDH˃ ZnZr-MMO˃ ZnAlZr-MMO˃ ZnTi-MMO˃ ZnAlTi-MMO were observed. LDH samples showed higher catalytic conversion than their respective MMOs during PET and PC depolymerization into monomers BHET and BPA with % yield of ∼76–83 % and ∼81–89 %, respectively. ZnTi-LDH shows high catalytic efficacy in depolymerization of PET and PC with yield of (∼82 %) BHET monomer and (89 %) BPA. This catalyst displayed good recyclability more than eight cycles during this catalytic glycolysis study.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"446 ","pages":"Article 115136"},"PeriodicalIF":5.2,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142658796","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}
Catalysis TodayPub Date : 2024-11-05DOI: 10.1016/j.cattod.2024.115123
Tanmoy Ghosh , Imran Khan , Subhajit Saha
{"title":"Pyrocatalytic removal of Cr(VI) by MoS2 nanosheets under controlled thermal fluctuation","authors":"Tanmoy Ghosh , Imran Khan , Subhajit Saha","doi":"10.1016/j.cattod.2024.115123","DOIUrl":"10.1016/j.cattod.2024.115123","url":null,"abstract":"<div><div>Traditionally, photocatalysts have been considered as effective tool to combat water pollution caused by Cr(VI) contamination. However, absence of sunlight in night and poor transmittance in the waste water restrict their wide-spread practical applications. Herein, two dimensional MoS<sub>2</sub> nanosheets have been employed as pyrocatalyst for round-o-clock utilization of natural temperature fluctuation and consequent reduction of Cr(VI). MoS<sub>2</sub> pyrocatalysts have been synthesized via facile hydrothermal technique and further characterized by XRD, XPS, SEM technique. The developed pyrocatalyst exhibits ∼95 % removal of 80 ppm Cr(VI) under thermal cycles between 20 ºC and 70 ºC. Moreover, the pyrocatalyst can effectively harness natural temperature variation for the catalytic reduction of Cr(VI) in just 30 days. The excited electrons generated during the temperature variation are identified as active species responsible for Cr(VI) reduction. The results and concept presented here may bring new possibilities for the removal of heavy metal ions in waste water treatment technology.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"446 ","pages":"Article 115123"},"PeriodicalIF":5.2,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142658824","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}
Catalysis TodayPub Date : 2024-11-05DOI: 10.1016/j.cattod.2024.115121
Jussara V.R. Vieira, Tassia C.P. Pereira, Carlos H.F. da Cunha, Davi D. Petrolini, Ana C.M. Tello, Alice M. Lima, Yasmin O. Carvalho, André L.R. Garcia, Ernesto A. Urquieta-Gonzalez, João B.O. dos Santos, Patrícia M. Lima, José M.C. Bueno
{"title":"Isothermal conversion of methane to methanol over Cu-CHA using different oxidants","authors":"Jussara V.R. Vieira, Tassia C.P. Pereira, Carlos H.F. da Cunha, Davi D. Petrolini, Ana C.M. Tello, Alice M. Lima, Yasmin O. Carvalho, André L.R. Garcia, Ernesto A. Urquieta-Gonzalez, João B.O. dos Santos, Patrícia M. Lima, José M.C. Bueno","doi":"10.1016/j.cattod.2024.115121","DOIUrl":"10.1016/j.cattod.2024.115121","url":null,"abstract":"<div><div>Methane oxidation to methanol in cyclic processes using CuO-zeolites has traditionally employed O<sub>2</sub> and N<sub>2</sub>O as oxidants. This study explores the use of Cu-CHA zeolite, demonstrating that CO<sub>2</sub> can substitute O<sub>2</sub> in an isothermal reaction at 400 °C, analogous to previous findings using Cu-MAZ. The use of <em>in situ</em> UV-Vis diffuse reflectance spectroscopy (UV-Vis DRS) and density functional theory (DFT) theoretical calculations identified the formation of a binuclear copper hydroxide complex, Z-[CuOH-HOCu]<sup>2+</sup>-Z, on the Cu-CHA. Initial treatment using CO<sub>2</sub> led to marginally superior catalytic activity, compared to the use of O<sub>2</sub> alone, indicating the stability of the Z-[CuOH-HOCu]<sup>2+</sup>-Z complex against self-reduction at 400 °C. In subsequent cycles, activation with O<sub>2</sub> facilitated the oxidation of adsorbed methanol, yielding water and reconstituting the active sites. Conversely, activation with CO<sub>2</sub> led to the partial desorption of methanol, precluding water production and subsequent catalyst regeneration. The findings suggested that both O<sub>2</sub> and CO<sub>2</sub> activations necessitated a post-reaction water extraction step, followed by thermal treatment to replenish the active sites. Importantly, the results indicated that CO<sub>2</sub> could be used as a viable alternative oxidant to O<sub>2</sub> in this catalytic process, potentially enhancing the sustainability of industrial methanol production.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"446 ","pages":"Article 115121"},"PeriodicalIF":5.2,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142658795","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}
Catalysis TodayPub Date : 2024-11-01DOI: 10.1016/j.cattod.2024.115091
Xuantao Deng , Xia Wang , Weikun Chen, Na Chen, Linmin Ye , Jianwei Zheng, Youzhu Yuan
{"title":"Effect of metal nanoparticles on TiO2 for enhanced photocatalytic N-methylation of piperazine","authors":"Xuantao Deng , Xia Wang , Weikun Chen, Na Chen, Linmin Ye , Jianwei Zheng, Youzhu Yuan","doi":"10.1016/j.cattod.2024.115091","DOIUrl":"10.1016/j.cattod.2024.115091","url":null,"abstract":"<div><div>Direct <em>N</em>-alkylation of amines, such as piperazine, with alcohols via photocatalysis is a promising method, where the incorporation of metal nanoparticles (NPs) into photocatalysts significantly influences catalytic performance. Here, we report TiO<sub>2</sub> photocatalysts impregnated with various NPs using the photodeposition method (labelled as M/TiO<sub>2</sub>, where M includes Pt, Pd, Au, Ag, Cu, and Co) for the <em>N</em>-methylation of piperazine with methanol. Specifically, Pt/TiO<sub>2</sub> and Pd/TiO<sub>2</sub> catalysts achieved conversions of 64.3% and 50.9%, respectively, within 4 h, displaying distinct selectivities. Pt/TiO<sub>2</sub> predominantly yielded enamine intermediate with a selectivity of 95.4%, while Pd/TiO<sub>2</sub> mainly produced <em>N</em>-methylpiperazine with a selectivity of 83.6%. Through comprehensive characterizations and control experiments, we found that both Pt NPs and Pd NPs enhance the light absorption and promote photogenerated electron-hole separation. However, Pd NPs facilitate the formation of Pd–H active species and contain more sites for the adsorption of enamine, thereby favoring the hydrogenation of the enamine intermediate to produce <em>N</em>-methylpiperazine. This study underscores the pivotal role of metal NPs in modulating the outcomes of photocatalytic <em>N</em>-methylation reactions on TiO<sub>2</sub>.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"446 ","pages":"Article 115091"},"PeriodicalIF":5.2,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142593182","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}
Catalysis TodayPub Date : 2024-10-31DOI: 10.1016/j.cattod.2024.115120
Claudio Roberto Almeida de Abreu , Lucas Ribeiro Francisco , Raimundo Crisóstomo Rabelo-Neto , Rodrigo de Paiva Floro Bonfim , Marcelo Eduardo Huguenin Maia da Costa , Fábio Bellot Noronha , Priscilla Magalhães de Souza , Fabio Souza Toniolo
{"title":"Effect of rhenium on the activity of ZrO2-supported copper catalysts for hydrodeoxygenation of m-cresol","authors":"Claudio Roberto Almeida de Abreu , Lucas Ribeiro Francisco , Raimundo Crisóstomo Rabelo-Neto , Rodrigo de Paiva Floro Bonfim , Marcelo Eduardo Huguenin Maia da Costa , Fábio Bellot Noronha , Priscilla Magalhães de Souza , Fabio Souza Toniolo","doi":"10.1016/j.cattod.2024.115120","DOIUrl":"10.1016/j.cattod.2024.115120","url":null,"abstract":"<div><div>This work studies the effect of adding different loadings of Re on the performance of ZrO<sub>2</sub>-supported Cu catalysts for hydrodeoxygenation (HDO) of m-cresol. H<sub>2</sub>-TPR and XPS show a synergistic effect between Cu and Re, decreasing the reduction temperature of both metals and promoting the reduction of Re oxide. Moreover, the addition of Re changes Cu dispersion and acid properties of all catalysts. High Re contents results in a coverage of Cu surface. Catalytic tests reveal that HDO reaction rate and product distribution vary considerably depending on the Re loading. Cu catalyst was inactive for HDO reaction, forming only hydrogenation products. In contrast, Re catalyst stood out for its high capacity to promote HDO reaction, with significant production of toluene. For the bimetallic catalysts, the addition of Re increases HDO reaction rate from 0 to 0.39 mmol g<sub>metal</sub><sup>−1</sup> min<sup>−1</sup> and the selectivity towards toluene (0–82.6 %), whereas the formation of hydrogenation and dehydration products decreases.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"446 ","pages":"Article 115120"},"PeriodicalIF":5.2,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142593183","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}
Catalysis TodayPub Date : 2024-10-31DOI: 10.1016/j.cattod.2024.115114
Jiali Zheng , Zhihui Li , Dongsheng Zhang , Xinqiang Zhao , Qian Zhao , Yanji Wang
{"title":"IL/MIL-101-NH2 heterogeneous catalyst prepared by acid-base self-assembly for hydrodeoxygenation of 2,5-tetrahydrofurandicarboxylic acid to adipic acid","authors":"Jiali Zheng , Zhihui Li , Dongsheng Zhang , Xinqiang Zhao , Qian Zhao , Yanji Wang","doi":"10.1016/j.cattod.2024.115114","DOIUrl":"10.1016/j.cattod.2024.115114","url":null,"abstract":"<div><div>Bio-based route for preparing adipic acid (AA) from 5-hydroxymethylfurfural is the direction for achieving green and sustainable AA production. In light of the challenges, such as corrosion and difficulties in recycling of I<sup>-</sup> containing homogeneous catalyst, large amount, high cost, and significant mass transfer resistance of ionic liquid (IL) catalyst, encountered in the current hydrodeoxygenation of 2,5-tetrahydrofurandicarboxylic acid (THFDCA) to AA process. Herein, 1-sulfobutyl-3-methylimidazolium iodide IL ([HSO<sub>3</sub>-b-mim]·I) was used to functionalize MIL-101-NH<sub>2</sub> through acid-base self-assembly approach, hence, a heterogeneous catalyst, IL/MIL-101-NH<sub>2</sub> was designed and applied in the hydrodeoxygenation of THFDCA to bio-based AA for the first time. When reacted at 180 °C for 2 h, the THFDCA conversion and AA yield were 100 % and 99.9 %, respectively. Moreover, IL/MIL-101-NH<sub>2</sub> exhibited remarkable stability and could be reused multiple times with minimal loss in activity. XRD, SEM, FT-IR, BET, XPS, and TG results revealed that the functionalization process involved the reaction between HSO<sub>3</sub> in the IL and NH<sub>2</sub> in MIL-101-NH<sub>2</sub>, forming a salt that chemically bonded the IL to MIL-101-NH<sub>2</sub>, thereby enhancing stability. The excellent hydrodeoxygenation activity was attributed to the synergistic effect of the Lewis acid site (Cr<sup>3+</sup>) and the Lewis base nucleophilic site (I<sup>-</sup>) within IL/MIL-101-NH<sub>2</sub>.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"446 ","pages":"Article 115114"},"PeriodicalIF":5.2,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142593184","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}