Pub Date : 2024-10-23DOI: 10.1016/j.cattod.2024.115110
T.A. Zepeda
Here reports the modulation of selectivity in Fischer-Tropsch synthesis through the control of cobalt reducibility within a hexagonal mesoporous silica (HMS) framework. Cobalt loading, varied from 3 % to 12.5 wt%, generated different surface and bulk cobalt species that interact variably with the support, significantly influencing their reducibility and the resultant catalytic behavior. This variation significantly affected the reducibility of the cobalt species, influencing on the catalytic behavior. The control of reducibility and stability of Co species is contingent on the cobalt loading. Higher cobalt content enhances the reducibility of Co species, shifting product selectivity from long-chain hydrocarbons to lighter olefins and oxygenates. At a TOS of 4 h, the active phase predominantly involves metallic Co species, while CO2 and oxygenates formation is closely linked to the pair Co0-Co2+ active phase. After a TOS of 120 h, samples with higher cobalt content (6.1–15.8 % wt.) exhibited notable deactivation and changes in selectivity and hydrocarbon distribution. These changes were associated with the formation of a Co2C phase, which inhibits methane formation and chain growth while enhancing the production of lower olefins and oxygenates through a synergistic interaction at the Co0 and Co2C interface, also improves the WGS reaction, thereby increasing CO2 selectivity.
本文报告了通过控制六方介孔二氧化硅（HMS）框架内的钴还原性来调节费托合成中的选择性。钴的负载量从 3% 到 12.5 wt% 不等，产生了不同的表面和块体钴物种，这些钴物种与支持物的相互作用各不相同，极大地影响了它们的还原性和由此产生的催化行为。这种变化极大地影响了钴物种的还原性，从而影响了催化行为。钴物种的还原性和稳定性取决于钴的负载量。钴含量越高，钴物种的还原性越强，产品选择性从长链烃类转向较轻的烯烃和含氧化合物。在 4 小时的总反应时间内，活性相主要涉及金属 Co 物种，而 CO2 和含氧化合物的形成则与一对 Co0-Co2+ 活性相密切相关。在 120 小时的 TOS 之后，钴含量较高的样品（6.1-15.8% wt.）表现出明显的失活以及选择性和碳氢化合物分布的变化。这些变化与 Co2C 相的形成有关，Co2C 相通过 Co0 和 Co2C 界面的协同作用，抑制了甲烷的形成和链增长，同时提高了低级烯烃和含氧化合物的产量，还改善了 WGS 反应，从而提高了二氧化碳的选择性。
{"title":"Selectivity modulation in Fischer-Tropsch synthesis through reducibility control of cobalt-species containing HMS framework","authors":"T.A. Zepeda","doi":"10.1016/j.cattod.2024.115110","DOIUrl":"10.1016/j.cattod.2024.115110","url":null,"abstract":"<div><div>Here reports the modulation of selectivity in Fischer-Tropsch synthesis through the control of cobalt reducibility within a hexagonal mesoporous silica (HMS) framework. Cobalt loading, varied from 3 % to 12.5 wt%, generated different surface and bulk cobalt species that interact variably with the support, significantly influencing their reducibility and the resultant catalytic behavior. This variation significantly affected the reducibility of the cobalt species, influencing on the catalytic behavior. The control of reducibility and stability of Co species is contingent on the cobalt loading. Higher cobalt content enhances the reducibility of Co species, shifting product selectivity from long-chain hydrocarbons to lighter olefins and oxygenates. At a TOS of 4 h, the active phase predominantly involves metallic Co species, while CO<sub>2</sub> and oxygenates formation is closely linked to the pair Co<sup>0</sup>-Co<sup>2+</sup> active phase. After a TOS of 120 h, samples with higher cobalt content (6.1–15.8 % wt.) exhibited notable deactivation and changes in selectivity and hydrocarbon distribution. These changes were associated with the formation of a Co<sub>2</sub>C phase, which inhibits methane formation and chain growth while enhancing the production of lower olefins and oxygenates through a synergistic interaction at the Co<sup>0</sup> and Co<sub>2</sub>C interface, also improves the WGS reaction, thereby increasing CO<sub>2</sub> selectivity.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"445 ","pages":"Article 115110"},"PeriodicalIF":5.2,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142531573","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}
The progress in civilization can be related to the development of newer technological development and associated energy demand to run those systems. The personalized healthcare systems, the depletion of conventional fossil fuel reserve led us to think about alternative energy storage devices. Thus, it is important to develop energy storage materials with the property of good mechanical strength and stability for longer hours. Zn-air batteries (ZAB) show the promises to be an alternative of Li-air batteries for this purpose. ZABs can fulfill our need of stringent requirements such as high energy density, cost-effectiveness and it is safer as compared to Li-ion batteries. The stability of zinc in aqueous and air environments makes ZAB technology more reliable and effective for small to large-scale flexible electronics. To further enhance its efficiency, different scientific materials and methods have been developed over decades, of which this review provides detailed insight into the parameters and mechanisms related to the key components of the ZAB for enhancing the performance of ZAB. We summarized the working mechanism of overall reversible-ZABs and then independently we explained the mechanism and problems associated with cathode, anode, and electrolyte, followed by the current breakthrough related to each. Aspects such as role of optimal eg occupancy in bifunctional activity, inhibition of zinc dendrite, and gel polymer electrolytes with enhanced conductivity and strength are specifically highlighted. To facilitate a broad discussion among different research communities, important scientific hurdles and their potential solution related to R-ZABs are also summarized.
{"title":"Chemistry in rechargeable zinc-air battery: A mechanistic overview","authors":"Arkaj Singh, Ravinder Sharma, Akriti Gautam, Bhavnish Kumar, Sneha Mittal, Aditi Halder","doi":"10.1016/j.cattod.2024.115108","DOIUrl":"10.1016/j.cattod.2024.115108","url":null,"abstract":"<div><div>The progress in civilization can be related to the development of newer technological development and associated energy demand to run those systems. The personalized healthcare systems, the depletion of conventional fossil fuel reserve led us to think about alternative energy storage devices. Thus, it is important to develop energy storage materials with the property of good mechanical strength and stability for longer hours. Zn-air batteries (ZAB) show the promises to be an alternative of Li-air batteries for this purpose. ZABs can fulfill our need of stringent requirements such as high energy density, cost-effectiveness and it is safer as compared to Li-ion batteries. The stability of zinc in aqueous and air environments makes ZAB technology more reliable and effective for small to large-scale flexible electronics. To further enhance its efficiency, different scientific materials and methods have been developed over decades, of which this review provides detailed insight into the parameters and mechanisms related to the key components of the ZAB for enhancing the performance of ZAB. We summarized the working mechanism of overall reversible-ZABs and then independently we explained the mechanism and problems associated with cathode, anode, and electrolyte, followed by the current breakthrough related to each. Aspects such as role of optimal e<sub>g</sub> occupancy in bifunctional activity, inhibition of zinc dendrite, and gel polymer electrolytes with enhanced conductivity and strength are specifically highlighted. To facilitate a broad discussion among different research communities, important scientific hurdles and their potential solution related to R-ZABs are also summarized.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"445 ","pages":"Article 115108"},"PeriodicalIF":5.2,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142552748","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}
Pub Date : 2024-10-22DOI: 10.1016/j.cattod.2024.115102
Sandeep Nigam , Chiranjib Majumder
Bimetallic clusters, as the name suggests, are known to act as bifunctional catalyst. Therefore, it is possible to tune the composition of the catalyst to achieve the best performance for a specific reaction. In the first part of this work, we explore the geometric and electronic structures of various Ag-Pt bimetallic clusters and find the right composition for ORR, one of the most sought-after reactions in the field of energy materials. We have considered Ag-Pt bimetallic clusters in both free and on Al2O3(0001) support. The results reveal that the equilibrium structures of the bimetallic AgnPtm (n+m ≤ 12 atoms) clusters are governed by a balance of competing interactions (Pt-Pt vs Ag-Pt vs cluster-support interactions). Whilst the isolated decamer cluster with 5:5 or 6:4 composition (Ag6Pt4 and Ag5Pt5) shows atomically segregated structures, Ag rich clusters (Ag9Pt1–3) prefer to form core-shell pattern where Pt forms the core surrounded by Ag atoms. In general, these clusters adopt pseudo-planar structure on alumina support following the surface template. Analysis of the electronic structure shows that Al2O3 surface induces significant broadening in the energy states of the bimetallic cluster, which in turn facilitates higher mixing between d-states of the Ag and Pt in the complex. Finally, the d-band centre descriptor model has been utilized to underscore the chemical reactivity of these bimetallic clusters. Remarkably, the Ag6Pt4@Al2O3 cluster with d-band centre at −2.68 eV is found to be in “just right” zone for ORR. This is further corroborated by the reduction (∼ 25 %) in oxidation reaction enthalpy of the Ag6Pt4@Al2O3 than standard Pt(111) catalytic surface.
双金属团簇，顾名思义，具有双功能催化剂的作用。因此，可以通过调节催化剂的组成来实现特定反应的最佳性能。在这项工作的第一部分，我们探索了各种银铂双金属团簇的几何和电子结构，并找到了用于 ORR（能源材料领域最热门的反应之一）的合适成分。我们研究了游离和Al2O3(0001)支撑下的银铂双金属团簇。研究结果表明，双金属 AgnPtm（n+m ≤ 12 个原子）团簇的平衡结构受相互竞争的相互作用（Pt-Pt 与 Ag-Pt 之间的相互作用以及团簇与支撑物之间的相互作用）的影响。组成比例为 5:5 或 6:4 的孤立十聚体团簇（Ag6Pt4 和 Ag5Pt5）显示出原子隔离结构，而富含 Ag 的团簇（Ag9Pt1-3）则倾向于形成核壳模式，其中铂形成核心，周围环绕着 Ag 原子。一般来说，这些团簇在氧化铝载体上按照表面模板采用伪平面结构。对电子结构的分析表明，Al2O3 表面使双金属团簇的能态显著拓宽，这反过来又促进了复合物中银和铂的 d 态之间的混合。最后，利用 d 带中心描述模型强调了这些双金属簇的化学反应活性。值得注意的是，发现 d 波段中心在 -2.68 eV 的 Ag6Pt4@Al2O3 簇处于 ORR 的 "恰到好处 "区域。与标准铂（111）催化表面相比，Ag6Pt4@Al2O3 的氧化反应焓降低了 25%，进一步证实了这一点。
{"title":"Tailoring reactivity of small Ag/Pt bimetallic cluster for ORR: A comprehensive study using density functional theory approach","authors":"Sandeep Nigam , Chiranjib Majumder","doi":"10.1016/j.cattod.2024.115102","DOIUrl":"10.1016/j.cattod.2024.115102","url":null,"abstract":"<div><div>Bimetallic clusters, as the name suggests, are known to act as bifunctional catalyst. Therefore, it is possible to tune the composition of the catalyst to achieve the best performance for a specific reaction. In the first part of this work, we explore the geometric and electronic structures of various Ag-Pt bimetallic clusters and find the right composition for ORR, one of the most sought-after reactions in the field of energy materials. We have considered Ag-Pt bimetallic clusters in both free and on Al<sub>2</sub>O<sub>3</sub>(0001) support. The results reveal that the equilibrium structures of the bimetallic Ag<sub>n</sub>Pt<sub>m</sub> (n+m ≤ 12 atoms) clusters are governed by a balance of competing interactions (<em>Pt-Pt vs Ag-Pt vs cluster-support interactions</em>). Whilst the isolated decamer cluster with 5:5 or 6:4 composition (Ag<sub>6</sub>Pt<sub>4</sub> and Ag<sub>5</sub>Pt<sub>5</sub>) shows atomically segregated structures, Ag rich clusters (Ag<sub>9</sub>Pt<sub>1–3</sub>) prefer to form core-shell pattern where Pt forms the core surrounded by Ag atoms. In general, these clusters adopt pseudo-planar structure on alumina support following the surface template. Analysis of the electronic structure shows that Al<sub>2</sub>O<sub>3</sub> surface induces significant broadening in the energy states of the bimetallic cluster, which in turn facilitates higher mixing between <em>d</em>-states of the Ag and Pt in the complex. Finally, the <em>d</em>-band centre descriptor model has been utilized to underscore the chemical reactivity of these bimetallic clusters. Remarkably, the Ag<sub>6</sub>Pt<sub>4</sub>@Al<sub>2</sub>O<sub>3</sub> cluster with <em>d</em>-band centre at −2.68 eV is found to be in “just right” zone for ORR. This is further corroborated by the reduction (∼ 25 %) in oxidation reaction enthalpy of the Ag<sub>6</sub>Pt<sub>4</sub>@Al<sub>2</sub>O<sub>3</sub> than standard Pt(111) catalytic surface.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"445 ","pages":"Article 115102"},"PeriodicalIF":5.2,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142552722","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}
Pub Date : 2024-10-21DOI: 10.1016/j.cattod.2024.115106
Luís Fernando Wentz Brum , Maurício Dalla Costa Rodrigues da Silva , Cristiane dos Santos , Giovani Pavoski , Denise Crocce Romano Espinosa , William Leonardo da Silva
Niobium is a metal that has been attracting great interest in producing high-technology materials, in which niobium oxide nanoparticles (Nb2O5-NPs) are inserted. In this context, the present study aims to develop and characterize structurally and morphologically niobium (V) oxide nanoparticles (Nb2O5-NPs) by the green synthesis method from pecan nutshell (C. illinoinensis) extract. Nb2O5-NPs were characterized by Attenuated Total Reflection Fourier Transform Infrared (ATR-FTIR), Scanning Electron Microscopy (SEM), X-ray diffraction (XRD) and N2 porosimetry (BET/BJH method). The antioxidant potential of the pecan nutshell extract was determined for the quantification of phenolic compounds and flavonoids. The XRD diffractogram showed that the Nb2O5-NPs presented a semicrystalline structure with the presence of the pseudohexagonal phase of Nb2O5. The ATR-FTIR spectrum confirmed the presence of a band vibration of the Nb-O at 600 cm−1. The Nb2O5-NPs presented spherical morphology according to the SEM micrography with a specific surface area of 1.72 m2 g−1 and 36.31 nm pore diameter (isotherm type III) by the N2 porosimetry. The pecan nutshell extract showed the presence of polyphenols (336.8 mgAG mL−1) and flavonoids (200.1 mgCt mL−1), demonstrating the high potential to act as a bioreducing and stabilizing agent for the green synthesis of Nb2O5-NPs. Therefore, the green synthesis of Nb2O5-NPs is feasible with potential application in different fields.
{"title":"Green synthesis of niobium (V) oxide nanoparticles using pecan nutshell (Carya illinoinensis) and evaluation of its antioxidant activity","authors":"Luís Fernando Wentz Brum , Maurício Dalla Costa Rodrigues da Silva , Cristiane dos Santos , Giovani Pavoski , Denise Crocce Romano Espinosa , William Leonardo da Silva","doi":"10.1016/j.cattod.2024.115106","DOIUrl":"10.1016/j.cattod.2024.115106","url":null,"abstract":"<div><div>Niobium is a metal that has been attracting great interest in producing high-technology materials, in which niobium oxide nanoparticles (Nb<sub>2</sub>O<sub>5</sub>-NPs) are inserted. In this context, the present study aims to develop and characterize structurally and morphologically niobium (V) oxide nanoparticles (Nb<sub>2</sub>O<sub>5</sub>-NPs) by the green synthesis method from pecan nutshell (<em>C. illinoinensis</em>) extract. Nb<sub>2</sub>O<sub>5</sub>-NPs were characterized by Attenuated Total Reflection Fourier Transform Infrared (ATR-FTIR), Scanning Electron Microscopy (SEM), X-ray diffraction (XRD) and N<sub>2</sub> porosimetry (BET/BJH method). The antioxidant potential of the pecan nutshell extract was determined for the quantification of phenolic compounds and flavonoids. The XRD diffractogram showed that the Nb<sub>2</sub>O<sub>5</sub>-NPs presented a semicrystalline structure with the presence of the pseudohexagonal phase of Nb<sub>2</sub>O<sub>5</sub>. The ATR-FTIR spectrum confirmed the presence of a band vibration of the Nb-O at 600 cm<sup>−1</sup>. The Nb<sub>2</sub>O<sub>5</sub>-NPs presented spherical morphology according to the SEM micrography with a specific surface area of 1.72 m<sup>2</sup> g<sup>−1</sup> and 36.31 nm pore diameter (isotherm type III) by the N<sub>2</sub> porosimetry. The pecan nutshell extract showed the presence of polyphenols (336.8 mgAG mL<sup>−1</sup>) and flavonoids (200.1 mgCt mL<sup>−1</sup>), demonstrating the high potential to act as a bioreducing and stabilizing agent for the green synthesis of Nb<sub>2</sub>O<sub>5</sub>-NPs. Therefore, the green synthesis of Nb<sub>2</sub>O<sub>5</sub>-NPs is feasible with potential application in different fields.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"445 ","pages":"Article 115106"},"PeriodicalIF":5.2,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142531570","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}
Pub Date : 2024-10-20DOI: 10.1016/j.cattod.2024.115103
Mohd Fazil , Jahangeer Ahmed , Tokeer Ahmad
Monophasic 1, 2.5, and 5 % Zn-decorated TiO2 nanocatalysts have been fabricated by environmentally benign hydrothermal synthesis by avoiding expensive chemicals. As- prepared nanostructures have been investigated utilizing various sophisticated instruments like XRD, scanning and transmission electron microscopy, EDAX, Raman, optoelectronics as well as BET Surface Area studies. 2.5 % Zn- decorated TiO2 was found to have superior photocatalytic performance, exhibiting an H2 formation of 25.55 mmol in 8 hours and average H2 generation of 3.15 mmolh−1 at 170 W light intensity. Additionally, electrochemical investigations showed that 5 % and 2.5 % Zn-doped TiO2 had a higher cathodic and anodic current density of 10 mA/cm2 at −0.95, indicating that it has a higher HER catalytic activity, respectively. The synergistic impact of pristine TiO2 and Zn-incorporated TiO2 nanocatalysts is responsible for the increased kinetics of H2 evolution, as it increases the separation and transfer of photo-charged (e-/h+ pair) carriers and decreases redox potential for HER.
{"title":"Enhanced photo/electrocatalytic efficiency of Zn-decorated TiO2 nanostructures for sustainable hydrogen evolution","authors":"Mohd Fazil , Jahangeer Ahmed , Tokeer Ahmad","doi":"10.1016/j.cattod.2024.115103","DOIUrl":"10.1016/j.cattod.2024.115103","url":null,"abstract":"<div><div>Monophasic 1, 2.5, and 5 % Zn-decorated TiO<sub>2</sub> nanocatalysts have been fabricated by environmentally benign hydrothermal synthesis by avoiding expensive chemicals. As- prepared nanostructures have been investigated utilizing various sophisticated instruments like XRD, scanning and transmission electron microscopy, EDAX, Raman, optoelectronics as well as BET Surface Area studies. 2.5 % Zn- decorated TiO<sub>2</sub> was found to have superior photocatalytic performance, exhibiting an H<sub>2</sub> formation of 25.55 mmol<span><math><msubsup><mrow><mi>g</mi></mrow><mrow><mi>cat</mi></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msubsup></math></span> in 8 hours and average H<sub>2</sub> generation of 3.15 mmol<span><math><msubsup><mrow><mi>g</mi></mrow><mrow><mi>cat</mi></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msubsup></math></span>h<sup>−1</sup> at 170 W light intensity. Additionally, electrochemical investigations showed that 5 % and 2.5 % Zn-doped TiO<sub>2</sub> had a higher cathodic and anodic current density of 10 mA/cm<sup>2</sup> at −0.95, indicating that it has a higher HER catalytic activity, respectively. The synergistic impact of pristine TiO<sub>2</sub> and Zn-incorporated TiO<sub>2</sub> nanocatalysts is responsible for the increased kinetics of H<sub>2</sub> evolution, as it increases the separation and transfer of photo-charged (e<sup>-</sup>/h<sup>+</sup> pair) carriers and decreases redox potential for HER.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"445 ","pages":"Article 115103"},"PeriodicalIF":5.2,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142531572","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}
Pub Date : 2024-10-19DOI: 10.1016/j.cattod.2024.115101
Sudarshan Sarkar, Chandan Upadhyay
Tanneries and textile industries significantly impact aquatic ecosystems through the discharge of effluents containing heavy metals, dyes, and metal-resistant bacterial pathogens. This review examines the potential of layered double hydroxides (LDHs) for addressing these environmental challenges. It offers a comprehensive analysis of LDH morphology, synthesis techniques, and performance in wastewater remediation. LDHs are ionic lamellar hydroxides, containing two different metal cations in the main layers and anionic species in the interlayer, have attracted substantial research interest due to their ease of synthesis and unique properties. This review distinguishes itself by correlating various synthesis methods for LDHs directly with their efficacy in wastewater remediation, offering insights not typically covered in other reviews. Furthermore, the review explores the critical role of interlayer anions, such as carbonate and sulfate, in determining its influence in the structural, chemical, and physical properties of LDHs. It also addresses how modifications with graphitic carbon nitride (gC3N4) and graphene-based materials enhance LDH’s performance by increasing surface area, delaying charge recombination, and improving adsorption and photocatalytic activity. he review evaluates the impact of these factors on the removal of pollutants from wastewater and provides an in-depth discussion of the mechanisms involved in pollutant removal, including adsorption, ion exchange, and photocatalysis. It also highlights the antibacterial properties of LDHs, particularly when combined with advanced materials, demonstrating their potential antimicrobial efficacy. In addition to presenting a fresh perspective on the correlation between synthesis methods and performance outcomes, this review offers a comprehensive overview of the limitations and challenges associated with LDH technologies. It provides valuable insights into the optimization process and practical considerations, making it an essential resource for advancing LDH technologies in real-world wastewater treatment applications.
{"title":"Layered double hydroxides for industrial wastewater remediation: A review","authors":"Sudarshan Sarkar, Chandan Upadhyay","doi":"10.1016/j.cattod.2024.115101","DOIUrl":"10.1016/j.cattod.2024.115101","url":null,"abstract":"<div><div>Tanneries and textile industries significantly impact aquatic ecosystems through the discharge of effluents containing heavy metals, dyes, and metal-resistant bacterial pathogens. This review examines the potential of layered double hydroxides (LDHs) for addressing these environmental challenges. It offers a comprehensive analysis of LDH morphology, synthesis techniques, and performance in wastewater remediation. LDHs are ionic lamellar hydroxides, containing two different metal cations in the main layers and anionic species in the interlayer, have attracted substantial research interest due to their ease of synthesis and unique properties. This review distinguishes itself by correlating various synthesis methods for LDHs directly with their efficacy in wastewater remediation, offering insights not typically covered in other reviews. Furthermore, the review explores the critical role of interlayer anions, such as carbonate and sulfate, in determining its influence in the structural, chemical, and physical properties of LDHs. It also addresses how modifications with graphitic carbon nitride (gC<sub>3</sub>N<sub>4</sub>) and graphene-based materials enhance LDH’s performance by increasing surface area, delaying charge recombination, and improving adsorption and photocatalytic activity. he review evaluates the impact of these factors on the removal of pollutants from wastewater and provides an in-depth discussion of the mechanisms involved in pollutant removal, including adsorption, ion exchange, and photocatalysis. It also highlights the antibacterial properties of LDHs, particularly when combined with advanced materials, demonstrating their potential antimicrobial efficacy. In addition to presenting a fresh perspective on the correlation between synthesis methods and performance outcomes, this review offers a comprehensive overview of the limitations and challenges associated with LDH technologies. It provides valuable insights into the optimization process and practical considerations, making it an essential resource for advancing LDH technologies in real-world wastewater treatment applications.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"445 ","pages":"Article 115101"},"PeriodicalIF":5.2,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142531571","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}
Pub Date : 2024-10-18DOI: 10.1016/j.cattod.2024.115099
Gabrielle A.R. da Silva , Thamires M. de L.O. da Silva , João Paulo da S.Q. Menezes , Elizabeth Cristina T. Veloso , Gizele C. Fontes-Sant’Ana , Noemi Raquel C. Huaman , Rodrigo Brackmann , Marta A.P. Langone
The development of heterogeneous biocatalysts allows the expansion of the application of enzymes in different industrial processes, favoring the establishment of clean technologies. This work investigates the capacity of nickel ferrite magnetic nanoparticles (NiFe2O4) as a support for lipase B from Candida antarctica (CalB) immobilization. The adsorption capacity of the support revealed a maximum value of 15 mgprotein/gsupport, according to the Langmuir isotherm model. Efficiency immobilization by physical adsorption was low (21.3 %), and CalB was covalently immobilized after functionalization of NiFe2O4 with APTMS (3-aminopropyl trimethoxysilane) and activation with glutaraldehyde (GA), showing higher immobilization yield (62.9 %). The spinel ferrite NiFe2O4 was characterized by many physicochemical analyses. The enzyme derivatives obtained (NiFe2O4-CalB and NiFe2O4-APTMS-GA-CalB) were evaluated in the synthesis of alkyl esters. Despite no production was observed in the transesterification reactions, esterification led to 37.3 ± 1.0 % and 62.1 ± 0.2 % of oleic acid conversions using NiFe2O4-APTMS-GA-CalB and NiFe2O4-CalB, respectively. After 4 cycles, NiFe2O4-CalB maintained 92 % of its initial activity. Nickel ferrite magnetic nanoparticles form an efficient heterogeneous catalyst with lipase, which could be used to remove the content of free fatty acids (FFAs), like oleic acid, present in cheap raw materials to produce biodiesel.
{"title":"Ethyl esters synthesis catalyzed by lipase B from Candida antarctica immobilized on NiFe2O4 magnetic nanoparticles","authors":"Gabrielle A.R. da Silva , Thamires M. de L.O. da Silva , João Paulo da S.Q. Menezes , Elizabeth Cristina T. Veloso , Gizele C. Fontes-Sant’Ana , Noemi Raquel C. Huaman , Rodrigo Brackmann , Marta A.P. Langone","doi":"10.1016/j.cattod.2024.115099","DOIUrl":"10.1016/j.cattod.2024.115099","url":null,"abstract":"<div><div>The development of heterogeneous biocatalysts allows the expansion of the application of enzymes in different industrial processes, favoring the establishment of clean technologies. This work investigates the capacity of nickel ferrite magnetic nanoparticles (NiFe<sub>2</sub>O<sub>4</sub>) as a support for lipase B from <em>Candida antarctica</em> (CalB) immobilization. The adsorption capacity of the support revealed a maximum value of 15 mg<sub>protein</sub>/g<sub>support,</sub> according to the Langmuir isotherm model. Efficiency immobilization by physical adsorption was low (21.3 %), and CalB was covalently immobilized after functionalization of NiFe<sub>2</sub>O<sub>4</sub> with APTMS (3-aminopropyl trimethoxysilane) and activation with glutaraldehyde (GA), showing higher immobilization yield (62.9 %). The spinel ferrite NiFe<sub>2</sub>O<sub>4</sub> was characterized by many physicochemical analyses. The enzyme derivatives obtained (NiFe<sub>2</sub>O<sub>4</sub>-CalB and NiFe<sub>2</sub>O<sub>4</sub>-APTMS-GA-CalB) were evaluated in the synthesis of alkyl esters. Despite no production was observed in the transesterification reactions, esterification led to 37.3 ± 1.0 % and 62.1 ± 0.2 % of oleic acid conversions using NiFe<sub>2</sub>O<sub>4</sub>-APTMS-GA-CalB and NiFe<sub>2</sub>O<sub>4</sub>-CalB, respectively. After 4 cycles, NiFe<sub>2</sub>O<sub>4</sub>-CalB maintained 92 % of its initial activity. Nickel ferrite magnetic nanoparticles form an efficient heterogeneous catalyst with lipase, which could be used to remove the content of free fatty acids (FFAs), like oleic acid, present in cheap raw materials to produce biodiesel.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"445 ","pages":"Article 115099"},"PeriodicalIF":5.2,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142552810","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}
Pub Date : 2024-10-11DOI: 10.1016/j.cattod.2024.115085
Adriele Sabrina Todero , Fabiana de Oliveira Pereira , Paloma Truccolo Reato , Diana Finkler , Alexander Junges , Rogério Marcos Dallago , Katia Bernardo-Gusmão , Marcelo Luis Mignoni
Mesoporous materials such as the Mobil Composition of Matter (MCM), play a crucial role in the chemical fixation of carbon dioxide (CO2). These materials exhibit a porous structure with intermediate-sized pores, providing a high surface area and a uniform pore distribution. The objective of this study is to synthesize the mesoporous material MCM-48 using the ionic solid chloride of 1-hexadecyl-3-methylimidazolium ([C16MI]Cl) as a directing agent and tetraethoxysilane (TEOS) as a silica precursor and apply this material as a catalyst in the cycloaddition reaction of CO2 to propylene oxide to produce propylene carbonate. Compounds such as graphene, aluminum, and niobium are employed in different Si/compound molar ratios (1, 5, and 10) to enhance the material properties. The Nb/Graphene-MCM-48 material with a Si/Nb ratio of 10 demonstrated the best catalytic performance in the CO2 cycloaddition, achieving a yield of 85 % and a selectivity of 99 % for propylene carbonate. The results demonstrate that MCMs are highly efficient in the selective conversion of CO2 into cyclic carbonate, offering promising applications for CO2 emission mitigation. This study advances decarbonization and sustainable development, aligning with the Sustainable Development Goals (SDGs) 3 (Good Health and Well-Being), 9 (Industry, Innovation, and Infrastructure), 12 (Responsible Consumption and Production), and 15 (Life on Land) by promoting technologies that reduce environmental impact and support sustainable industrial practices.
美孚物质成分（MCM）等介孔材料在二氧化碳（CO2）的化学固定过程中发挥着至关重要的作用。这些材料呈现出具有中等大小孔隙的多孔结构，提供了高表面积和均匀的孔隙分布。本研究的目的是以 1-十六烷基-3-甲基咪唑离子固体氯化物（[C16MI]Cl）为引导剂，以四乙氧基硅烷（TEOS）为二氧化硅前驱体，合成介孔材料 MCM-48，并将该材料用作二氧化碳与环氧丙烷发生环加成反应生成碳酸丙烯酯的催化剂。在不同的硅/化合物摩尔比（1、5 和 10）下使用石墨烯、铝和铌等化合物，以增强材料的性能。硅/铌比为 10 的铌/石墨烯-MCM-48 材料在二氧化碳环化反应中表现出最佳催化性能，对碳酸丙烯酯的产率达到 85%，选择性达到 99%。研究结果表明，MCMs 在将 CO2 选择性转化为环碳酸酯方面具有很高的效率，在减少 CO2 排放方面具有广阔的应用前景。这项研究通过推广可减少环境影响和支持可持续工业实践的技术，推进了脱碳和可持续发展，符合可持续发展目标（SDGs）3（良好的健康和福祉）、9（工业、创新和基础设施）、12（负责任的消费和生产）和 15（陆地生活）。
{"title":"Synthesis and reactivity of Nb/graphene-MCM-48 and Al/graphene-MCM-48 IN CO2 chemical fixation","authors":"Adriele Sabrina Todero , Fabiana de Oliveira Pereira , Paloma Truccolo Reato , Diana Finkler , Alexander Junges , Rogério Marcos Dallago , Katia Bernardo-Gusmão , Marcelo Luis Mignoni","doi":"10.1016/j.cattod.2024.115085","DOIUrl":"10.1016/j.cattod.2024.115085","url":null,"abstract":"<div><div>Mesoporous materials such as the <em>Mobil Composition of Matter</em> (MCM), play a crucial role in the chemical fixation of carbon dioxide (CO<sub>2</sub>). These materials exhibit a porous structure with intermediate-sized pores, providing a high surface area and a uniform pore distribution. The objective of this study is to synthesize the mesoporous material MCM-48 using the ionic solid chloride of 1-hexadecyl-3-methylimidazolium ([C16MI]Cl) as a directing agent and tetraethoxysilane (TEOS) as a silica precursor and apply this material as a catalyst in the cycloaddition reaction of CO2 to propylene oxide to produce propylene carbonate. Compounds such as graphene, aluminum, and niobium are employed in different Si/compound molar ratios (1, 5, and 10) to enhance the material properties. The Nb/Graphene-MCM-48 material with a Si/Nb ratio of 10 demonstrated the best catalytic performance in the CO<sub>2</sub> cycloaddition, achieving a yield of 85 % and a selectivity of 99 % for propylene carbonate. The results demonstrate that MCMs are highly efficient in the selective conversion of CO2 into cyclic carbonate, offering promising applications for CO<sub>2</sub> emission mitigation. This study advances decarbonization and sustainable development, aligning with the Sustainable Development Goals (SDGs) 3 (Good Health and Well-Being), 9 (Industry, Innovation, and Infrastructure), 12 (Responsible Consumption and Production), and 15 (Life on Land) by promoting technologies that reduce environmental impact and support sustainable industrial practices.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"445 ","pages":"Article 115085"},"PeriodicalIF":5.2,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142532060","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}
Pub Date : 2024-10-11DOI: 10.1016/j.cattod.2024.115092
Kanhaiya Saini , Reetu Sharma , Amit Kumar Sharma , Balaram Pani , Anjana Sarkar
The primary focus of this review is the wide range of techniques available for generating α-MoO3 nanostructures. Some examples of these processes are hydrothermal method, solvothermal method, sol-gel methods, spray pyrolysis chemical, thermal evaporation, and own heterostructures. The various crystal and electronic structures of α-MoO3 offer a wealth of possibilities for the discovery of electrocatalysts that are suited for the creation of hydrogen through the splitting of water molecules. The orthorhombic form of α-MoO3 has showed potential electrocatalytic activity for the hydrogen evolution reaction (HER), while the polymorph has shown poor oxygen evolution reaction (OER) activity. This is the case even though both forms have been investigated. The as-prepared nanostructures were found to be effective photocatalysts for the breakdown of acridine orange when exposed to ultraviolet light. A high photocatalytic property was shown by the generated mixed morphology, which consisted of hexagonal nanoplatelets and nano bars, in order to breakdown the carcinogenic Acridine Orange dye. In addition, as a result of their 1-Dimensional and 2-Dimensional nanostructure feature, they are capable of being recycled with relative ease while maintaining their photocatalytic activity. In order to highlight the potential of α-MoO3 heterogeneous nanostructures for electrocatalytic and photocatalytic processes like CO2 reduction, hydrogen evolution, and pollutant degradation, this review will analyze and summarize recent developments in these areas. Also covered in this article are number of contemporary difficulties as well as prospective research directions based on α-MoO3 nanostructures.
{"title":"An exploration of tailoring of hetero-nanostructures of α-MoO3 for efficient electrocatalytic and photocatalytic applications","authors":"Kanhaiya Saini , Reetu Sharma , Amit Kumar Sharma , Balaram Pani , Anjana Sarkar","doi":"10.1016/j.cattod.2024.115092","DOIUrl":"10.1016/j.cattod.2024.115092","url":null,"abstract":"<div><div>The primary focus of this review is the wide range of techniques available for generating α-MoO<sub>3</sub> nanostructures. Some examples of these processes are hydrothermal method, solvothermal method, sol-gel methods, spray pyrolysis chemical, thermal evaporation, and own heterostructures. The various crystal and electronic structures of α-MoO<sub>3</sub> offer a wealth of possibilities for the discovery of electrocatalysts that are suited for the creation of hydrogen through the splitting of water molecules. The orthorhombic form of α-MoO<sub>3</sub> has showed potential electrocatalytic activity for the hydrogen evolution reaction (HER), while the polymorph has shown poor oxygen evolution reaction (OER) activity. This is the case even though both forms have been investigated. The as-prepared nanostructures were found to be effective photocatalysts for the breakdown of acridine orange when exposed to ultraviolet light. A high photocatalytic property was shown by the generated mixed morphology, which consisted of hexagonal nanoplatelets and nano bars, in order to breakdown the carcinogenic Acridine Orange dye. In addition, as a result of their 1-Dimensional and 2-Dimensional nanostructure feature, they are capable of being recycled with relative ease while maintaining their photocatalytic activity. In order to highlight the potential of α-MoO<sub>3</sub> heterogeneous nanostructures for electrocatalytic and photocatalytic processes like CO<sub>2</sub> reduction, hydrogen evolution, and pollutant degradation, this review will analyze and summarize recent developments in these areas. Also covered in this article are number of contemporary difficulties as well as prospective research directions based on α-MoO<sub>3</sub> nanostructures.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"445 ","pages":"Article 115092"},"PeriodicalIF":5.2,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142531569","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}
Pub Date : 2024-10-11DOI: 10.1016/j.cattod.2024.115098
Rosana Balzer , Alexander Sachse , Jean-Dominique Comparot , Maria do Carmo Martins Alves , Jonder Morais , Katia Bernardo-Gusmão , Anderson Joel Schwanke
The porous engineering of clay nanoarchitectures (PCN) achieved from a well-known but little-explored commercial organoclay C-20A is reported. Thorough characterizations (by XRD, TGA, N2 sorption, ICP, SEM, TEM, 27Al MAS NMR, DR UV-Vis, XPS, Py-FTIR and H2-TPR) confirmed a delaminated structure presenting a specific surface area of 504 m² g−1, twelve times higher than the sodic montmorillonite used as reference and featuring a new pore system comprising a size range from supermicropores to small mesopores (1.3–10 nm). The role of these PCN as support of manganese oxide for the gas-phase total catalytic oxidation of volatile organic compounds (VOCs) was evaluated. PCN with 5 % of Mn resulted in a higher nanoparticle dispersion (10 nm) compared to the sodic montmorillonite (17 nm). The highest catalytic activity was reached with PCN containing 10 % of Mn achieving a benzene, toluene and ortho-xylene oxidation of 54 %, 39 % and 34 %, respectively, at 350 °C. The catalyst was stable up to 36 h under these conditions.
{"title":"Engineering porous clay nanoarchitectures from unusual commercial organoclay: Supported manganese oxide as stable catalysts in the total oxidation of volatile organic compounds","authors":"Rosana Balzer , Alexander Sachse , Jean-Dominique Comparot , Maria do Carmo Martins Alves , Jonder Morais , Katia Bernardo-Gusmão , Anderson Joel Schwanke","doi":"10.1016/j.cattod.2024.115098","DOIUrl":"10.1016/j.cattod.2024.115098","url":null,"abstract":"<div><div>The porous engineering of clay nanoarchitectures (PCN) achieved from a well-known but little-explored commercial organoclay C-20A is reported. Thorough characterizations (by XRD, TGA, N<sub>2</sub> sorption, ICP, SEM, TEM, <sup>27</sup>Al MAS NMR, DR UV-Vis, XPS, Py-FTIR and H<sub>2</sub>-TPR) confirmed a delaminated structure presenting a specific surface area of 504 m² g<sup>−1</sup>, twelve times higher than the sodic montmorillonite used as reference and featuring a new pore system comprising a size range from supermicropores to small mesopores (1.3–10 nm). The role of these PCN as support of manganese oxide for the gas-phase total catalytic oxidation of volatile organic compounds (VOCs) was evaluated. PCN with 5 % of Mn resulted in a higher nanoparticle dispersion (10 nm) compared to the sodic montmorillonite (17 nm). The highest catalytic activity was reached with PCN containing 10 % of Mn achieving a benzene, toluene and <em>ortho</em>-xylene oxidation of 54 %, 39 % and 34 %, respectively, at 350 °C. The catalyst was stable up to 36 h under these conditions.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"445 ","pages":"Article 115098"},"PeriodicalIF":5.2,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142532061","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}
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