首页 > 最新文献

Catalysts最新文献

英文 中文
Study on the Inhibition of Hydrogen Evolution Reaction by Electrocatalytic Reduction of Carbon Dioxide Using Elsholtzia Harchowensis Biochar 利用 Elsholtzia Harchowensis 生物炭通过电催化还原二氧化碳抑制氢气进化反应的研究
IF 3.9 3区 化学 Q1 Environmental Science Pub Date : 2024-02-27 DOI: 10.3390/catal14030172
Wei Liu, Shiqi Chen, Ziwei Mei, Liang Li, Hong Tao
With the widespread application of plant remediation technology in the field of soil remediation, there was an increasing stock of hyperaccumulating plant tissues containing heavy metals, but there was currently a lack of effective disposal methods. In the preliminary research process, researchers used the copper hyperaccumulating plant Elsholtzia Harchowensis to prepare biochar material electrodes and successfully used them in the electrocatalytic reduction of carbon dioxide (CO2) process. Due to the previous research being conducted in aqueous solutions, the hydrogen evolution reaction (HER) on the working electrode surface has a certain impact on the Faraday efficiency (FE) of carbon-containing products. In order to further improve the electrocatalytic reduction performance of biochar materials, this study was based on B- and N-doped biochar prepared from Elsholtzia Harchowensis as raw material. The influence mechanisms of electrode surface hydrophobicity and electrolyte components (PC/water) on the CO2RR and HER were studied, respectively. After dropwise coating PTFE on the surface of Cu/C-BN material, the hydrophobicity of Cu/C-BN-PT material was improved, and the effect on the active sites of the catalyst was relatively small without changing the structure and elemental characteristics of the original electrode. In a 1.0 M KHCO3 solution, the Faraday efficiency of H2 in Cu/C-BN-PT material decreased by 20.1% compared to Cu/C-BN at −0.32 V (vs. RHE), indicating that changing the hydrophilicity of the material can significantly inhibit the HER. In a solution of PC/water at a ratio of 9:1 (V:V), the FE of converting CO2 to methane (CH4) at −0.32 V (vs. RHE) reached 12.0%, and the FE of carbon monoxide (CO) reached 64.7%. The HER was significantly inhibited, significantly improving the selectivity of electrocatalytic CO2.
随着植物修复技术在土壤修复领域的广泛应用,含重金属的超积累植物组织存量越来越大,但目前缺乏有效的处理方法。在前期研究过程中,研究人员利用铜超积累植物 Elsholtzia Harchowensis 制备了生物炭材料电极,并成功将其用于二氧化碳(CO2)的电催化还原过程。由于之前的研究是在水溶液中进行的,工作电极表面的氢进化反应(HER)对含碳产物的法拉第效率(FE)有一定影响。为了进一步提高生物炭材料的电催化还原性能,本研究以 Elsholtzia Harchowensis 为原料制备了掺 B 和掺 N 的生物炭。分别研究了电极表面疏水性和电解质成分(PC/水)对 CO2RR 和 HER 的影响机理。在 Cu/C-BN 材料表面滴涂 PTFE 后,Cu/C-BN-PT 材料的疏水性得到改善,对催化剂活性位点的影响相对较小,且未改变原电极的结构和元素特性。在 1.0 M KHCO3 溶液中,Cu/C-BN-PT 材料中 H2 的法拉第效率比 -0.32 V 时的 Cu/C-BN 降低了 20.1%(相对于 RHE),这表明改变材料的亲水性可以显著抑制 HER。在比例为 9:1 (V:V) 的 PC/ 水溶液中,-0.32 V(相对于 RHE)时将 CO2 转化为甲烷(CH4)的 FE 达到 12.0%,将一氧化碳(CO)转化为甲烷(CH4)的 FE 达到 64.7%。HER 受到了明显的抑制,显著提高了电催化 CO2 的选择性。
{"title":"Study on the Inhibition of Hydrogen Evolution Reaction by Electrocatalytic Reduction of Carbon Dioxide Using Elsholtzia Harchowensis Biochar","authors":"Wei Liu, Shiqi Chen, Ziwei Mei, Liang Li, Hong Tao","doi":"10.3390/catal14030172","DOIUrl":"https://doi.org/10.3390/catal14030172","url":null,"abstract":"With the widespread application of plant remediation technology in the field of soil remediation, there was an increasing stock of hyperaccumulating plant tissues containing heavy metals, but there was currently a lack of effective disposal methods. In the preliminary research process, researchers used the copper hyperaccumulating plant Elsholtzia Harchowensis to prepare biochar material electrodes and successfully used them in the electrocatalytic reduction of carbon dioxide (CO2) process. Due to the previous research being conducted in aqueous solutions, the hydrogen evolution reaction (HER) on the working electrode surface has a certain impact on the Faraday efficiency (FE) of carbon-containing products. In order to further improve the electrocatalytic reduction performance of biochar materials, this study was based on B- and N-doped biochar prepared from Elsholtzia Harchowensis as raw material. The influence mechanisms of electrode surface hydrophobicity and electrolyte components (PC/water) on the CO2RR and HER were studied, respectively. After dropwise coating PTFE on the surface of Cu/C-BN material, the hydrophobicity of Cu/C-BN-PT material was improved, and the effect on the active sites of the catalyst was relatively small without changing the structure and elemental characteristics of the original electrode. In a 1.0 M KHCO3 solution, the Faraday efficiency of H2 in Cu/C-BN-PT material decreased by 20.1% compared to Cu/C-BN at −0.32 V (vs. RHE), indicating that changing the hydrophilicity of the material can significantly inhibit the HER. In a solution of PC/water at a ratio of 9:1 (V:V), the FE of converting CO2 to methane (CH4) at −0.32 V (vs. RHE) reached 12.0%, and the FE of carbon monoxide (CO) reached 64.7%. The HER was significantly inhibited, significantly improving the selectivity of electrocatalytic CO2.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140427452","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}
引用次数: 0
One-Step Synthesis of Ultrathin High-Entropy Layered Double Hydroxides for Ampere-Level Water Oxidation 一步法合成用于安培级水氧化的超薄高熵层状双氢氧化物
IF 3.9 3区 化学 Q1 Environmental Science Pub Date : 2024-02-27 DOI: 10.3390/catal14030171
Jianlei Jing, Wei Liu, Tianshui Li, Xiaoqian Ding, Wenhai Xu, Mengze Ma, Daojin Zhou, Yaping Li, Xiaoming Sun
The development of high-entropy anodes, known for their excellent catalytic activity for water oxidation, can depress the energy consumption of hydrogen production by water electrolysis. However, the complex preparation methods and poor stability hindered their practical application. In this work, a one-step co-precipitation method has been modified to rapidly synthesize ultrathin high-entropy layered double hydroxide containing Ni, Co, Fe, Cr, Zn. Through the rational selection of metal elements, the stability of the optimized anode under Ampere-level current density has been significantly improved. Compared to NiFe-LDH, the active site leaching of high-entropy LDH is reduced by 42.7%, and as a result, it achieves a performance decay that is approximately eight times lower than that of NiFe-LDH. Experiment results show that the active sites in the high-entropy LDH can maintain a relatively low oxidation state both before and after activation, thus preventing material deactivation caused by excessive oxidation.
众所周知,高熵阳极具有出色的水氧化催化活性,开发这种阳极可以降低水电解制氢的能耗。然而,复杂的制备方法和较差的稳定性阻碍了它们的实际应用。本研究改进了一步共沉淀法,快速合成了含有 Ni、Co、Fe、Cr、Zn 的超薄高熵层状双氢氧化物。通过合理选择金属元素,优化后的阳极在安培级电流密度下的稳定性显著提高。与 NiFe-LDH 相比,高熵 LDH 的活性位点浸出减少了 42.7%,因此其性能衰减比 NiFe-LDH 低约八倍。实验结果表明,高熵 LDH 的活性位点在活化前后都能保持相对较低的氧化状态,从而避免了过度氧化导致的材料失活。
{"title":"One-Step Synthesis of Ultrathin High-Entropy Layered Double Hydroxides for Ampere-Level Water Oxidation","authors":"Jianlei Jing, Wei Liu, Tianshui Li, Xiaoqian Ding, Wenhai Xu, Mengze Ma, Daojin Zhou, Yaping Li, Xiaoming Sun","doi":"10.3390/catal14030171","DOIUrl":"https://doi.org/10.3390/catal14030171","url":null,"abstract":"The development of high-entropy anodes, known for their excellent catalytic activity for water oxidation, can depress the energy consumption of hydrogen production by water electrolysis. However, the complex preparation methods and poor stability hindered their practical application. In this work, a one-step co-precipitation method has been modified to rapidly synthesize ultrathin high-entropy layered double hydroxide containing Ni, Co, Fe, Cr, Zn. Through the rational selection of metal elements, the stability of the optimized anode under Ampere-level current density has been significantly improved. Compared to NiFe-LDH, the active site leaching of high-entropy LDH is reduced by 42.7%, and as a result, it achieves a performance decay that is approximately eight times lower than that of NiFe-LDH. Experiment results show that the active sites in the high-entropy LDH can maintain a relatively low oxidation state both before and after activation, thus preventing material deactivation caused by excessive oxidation.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140427268","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}
引用次数: 0
Impact of Copper(II)-Imidazole Complex Modification on Polycrystalline TiO2: Insights into Formation, Characterization, and Photocatalytic Performance 铜(II)-咪唑络合物修饰对多晶 TiO2 的影响:对形成、表征和光催化性能的见解
IF 3.9 3区 化学 Q1 Environmental Science Pub Date : 2024-02-26 DOI: 10.3390/catal14030169
Ganeshraja Ayyakannu Sundaram, Rajkumar Kanniah, Krishnamoorthy Anbalagan, Kaviyarasan Kulandaivelu, H. Valdés
Micrometer-sized polycrystalline anatase particles are widely used in materials and life sciences, serving as essential components in photocatalytic materials. The ability to tailor their composition, shape, morphology, and functionality holds significant importance. In this study, we identified and examined the non-destructive route of Copper(II) implantation at the surface of polycrystalline TiO2. The [Cu(en)(Im)2]2+ complex ion demonstrated a remarkable affinity to concentrate and bind with the semiconductor’s surface, such as anatase, forming a surface-bound adduct: ≡TiO2 + [Cu(en)(Im)2]2+ → ≡TiO2//[Cu(en)(Im)2]2+. The misalignment of Fermi levels in TiO2//[Cu(en)(Im)2]2+ triggered electron transfer, leading to the reduction of the metal center, releasing Copper(I) in the process. Although less efficient, the released Copper(I) encountered a highly favorable environment, resulting in the formation of the surface complex TiO2:CuIIsc. The implanted Cu(I) was converted back into Cu(II) due to re-oxidation by dissolved oxygen. The penetration of the metal ion into the surface level of the polycrystalline TiO2 lattice was influenced by surface residual forces, making surface grafting of the Cu(II) ion inevitable due to surface chemistry. FTIR, UV–vis, Raman, XRD, EPR, and surface morphological (SEM, EDAX, and HRTEM) analyses identified the typical surface grafting of the Cu(II) cluster complex on the anatase surface matrix. Moreover, the XRD results also showed the formation of an impure phase. The TiO2 polycrystalline materials, modified by the incorporation of copper complexes, demonstrated an enhanced visible-light photocatalytic capability in the degradation of Rhodamine B dye in aqueous solutions. This modification significantly improved the efficiency of the photocatalytic process, expanding the applicability of TiO2 to visible light wavelengths. These studies open up the possibility of using copper complexes grafted on metal oxide surfaces for visible-light active photocatalytic applications. Moreover, this investigation not only showcases the improved visible-light photocatalytic behavior of copper-modified TiO2 polycrystalline materials, but also underscores the broader implications of this improvement in the advancement of sustainable and efficient water treatment technologies.
微米级多晶锐钛矿颗粒广泛应用于材料和生命科学领域,是光催化材料的重要组成部分。定制其成分、形状、形态和功能的能力具有重要意义。在本研究中,我们确定并研究了在多晶 TiO2 表面植入铜(II)的非破坏性途径。[Cu(en)(Im)2]2+复合物离子表现出显著的亲和力,能集中并与锐钛矿等半导体表面结合,形成表面结合加合物:≡TiO2 + [Cu(en)(Im)2]2+ → ≡TiO2//[Cu(en)(Im)2]2+。TiO2//[Cu(en)(Im)2]2+ 中费米级的错位引发了电子转移,导致金属中心还原,并在此过程中释放出铜(I)。虽然效率较低,但释放出的铜(I)遇到了非常有利的环境,从而形成了表面复合物 TiO2:CuIIsc。由于溶解氧的再氧化作用,植入的铜(I)又转化为铜(II)。金属离子渗入多晶 TiO2 晶格的表层受到表面残余力的影响,因此由于表面化学作用,Cu(II)离子不可避免地会发生表面接枝。傅立叶变换红外光谱、紫外-可见光谱、拉曼光谱、XRD、EPR 和表面形貌(SEM、EDAX 和 HRTEM)分析确定了 Cu(II)簇复合物在锐钛矿表面基质上的典型表面接枝。此外,XRD 结果也表明形成了不纯相。通过加入铜络合物改性的 TiO2 多晶材料在降解水溶液中的罗丹明 B 染料时表现出了更强的可见光光催化能力。这种改性大大提高了光催化过程的效率,将二氧化钛的适用范围扩大到了可见光波段。这些研究为将接枝在金属氧化物表面的铜络合物用于可见光活性光催化应用提供了可能性。此外,这项研究不仅展示了铜改性 TiO2 多晶材料在可见光光催化行为方面的改进,还强调了这种改进在推进可持续高效水处理技术方面的广泛意义。
{"title":"Impact of Copper(II)-Imidazole Complex Modification on Polycrystalline TiO2: Insights into Formation, Characterization, and Photocatalytic Performance","authors":"Ganeshraja Ayyakannu Sundaram, Rajkumar Kanniah, Krishnamoorthy Anbalagan, Kaviyarasan Kulandaivelu, H. Valdés","doi":"10.3390/catal14030169","DOIUrl":"https://doi.org/10.3390/catal14030169","url":null,"abstract":"Micrometer-sized polycrystalline anatase particles are widely used in materials and life sciences, serving as essential components in photocatalytic materials. The ability to tailor their composition, shape, morphology, and functionality holds significant importance. In this study, we identified and examined the non-destructive route of Copper(II) implantation at the surface of polycrystalline TiO2. The [Cu(en)(Im)2]2+ complex ion demonstrated a remarkable affinity to concentrate and bind with the semiconductor’s surface, such as anatase, forming a surface-bound adduct: ≡TiO2 + [Cu(en)(Im)2]2+ → ≡TiO2//[Cu(en)(Im)2]2+. The misalignment of Fermi levels in TiO2//[Cu(en)(Im)2]2+ triggered electron transfer, leading to the reduction of the metal center, releasing Copper(I) in the process. Although less efficient, the released Copper(I) encountered a highly favorable environment, resulting in the formation of the surface complex TiO2:CuIIsc. The implanted Cu(I) was converted back into Cu(II) due to re-oxidation by dissolved oxygen. The penetration of the metal ion into the surface level of the polycrystalline TiO2 lattice was influenced by surface residual forces, making surface grafting of the Cu(II) ion inevitable due to surface chemistry. FTIR, UV–vis, Raman, XRD, EPR, and surface morphological (SEM, EDAX, and HRTEM) analyses identified the typical surface grafting of the Cu(II) cluster complex on the anatase surface matrix. Moreover, the XRD results also showed the formation of an impure phase. The TiO2 polycrystalline materials, modified by the incorporation of copper complexes, demonstrated an enhanced visible-light photocatalytic capability in the degradation of Rhodamine B dye in aqueous solutions. This modification significantly improved the efficiency of the photocatalytic process, expanding the applicability of TiO2 to visible light wavelengths. These studies open up the possibility of using copper complexes grafted on metal oxide surfaces for visible-light active photocatalytic applications. Moreover, this investigation not only showcases the improved visible-light photocatalytic behavior of copper-modified TiO2 polycrystalline materials, but also underscores the broader implications of this improvement in the advancement of sustainable and efficient water treatment technologies.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140428458","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}
引用次数: 1
Resilient Enzymes through Immobilisation: Stable NDP Polyphosphate Phosphotransferase from Ruegeria pomeroyi for Nucleotide Regeneration 通过固定化实现弹性酶:用于核苷酸再生的 Ruegeria pomeroyi 稳定 NDP 多磷酸磷酸转移酶
IF 3.9 3区 化学 Q1 Environmental Science Pub Date : 2024-02-24 DOI: 10.3390/catal14030165
Kristin Hölting, Sebastian Götz, M. Aßmann, P. Bubenheim, Andreas Liese, Jürgen Kuballa
Immobilisation plays an important role in the industrial application of enzymes. The stabilisation and reusability of immobilised enzymes reduce the cost of the catalyst and facilitate their use in continuously operated reactors. For this purpose, an applicable type of immobilisation needs to be identified. In this study, we investigate the conversion of CDP and PolyP to CTP by NDP polyphosphate phosphotransferase 3 from Ruegeria pomeroyi (RpPPK2-3) and describe the covalent immobilisation of RpPPK2-3. In order to select a suitable carrier for the immobilisation of RpPPK2-3, a screening with different amino methacrylate (glutaraldehyde-pre-activated) and epoxy methacrylate carriers was carried out. The epoxy methacrylate carrier ECR8209M (Purolite®) was found to be the most suitable. With a half-life of 462 d when stored at 6 °C and a 50-fold reusability with a 93% residual activity, the immobilised enzyme showed a higher stability compared to the soluble enzyme with a half-life of 0.04 d. Although the half-life of the soluble enzyme could be increased to 32 d by adding PPi, it could not reach the stability of the immobilisate. Due to the resilience of the immobilisate, it is suitable for application in continuous reactor set-ups, e.g., packed-bed reactors.
固定化在酶的工业应用中发挥着重要作用。固定化酶的稳定性和可重复使用性降低了催化剂的成本,便于在连续运行的反应器中使用。为此,需要确定一种适用的固定化类型。在本研究中,我们研究了 Ruegeria pomeroyi(RpPPK2-3)的 NDP 多磷酸磷酸转移酶 3 将 CDP 和 PolyP 转化为 CTP 的过程,并描述了 RpPPK2-3 的共价固定化。为了选择适合固定 RpPPK2-3 的载体,研究人员筛选了不同的甲基丙烯酸氨基酯(戊二醛预活化)和甲基丙烯酸环氧酯载体。结果发现环氧甲基丙烯酸酯载体 ECR8209M(Purolite®)最为合适。与半衰期为 0.04 d 的可溶性酶相比,固定化酶显示出更高的稳定性。虽然通过添加 PPi,可溶性酶的半衰期可延长至 32 d,但仍无法达到固定化酶的稳定性。由于固定化物的弹性,它适合应用于连续反应器装置,如填料床反应器。
{"title":"Resilient Enzymes through Immobilisation: Stable NDP Polyphosphate Phosphotransferase from Ruegeria pomeroyi for Nucleotide Regeneration","authors":"Kristin Hölting, Sebastian Götz, M. Aßmann, P. Bubenheim, Andreas Liese, Jürgen Kuballa","doi":"10.3390/catal14030165","DOIUrl":"https://doi.org/10.3390/catal14030165","url":null,"abstract":"Immobilisation plays an important role in the industrial application of enzymes. The stabilisation and reusability of immobilised enzymes reduce the cost of the catalyst and facilitate their use in continuously operated reactors. For this purpose, an applicable type of immobilisation needs to be identified. In this study, we investigate the conversion of CDP and PolyP to CTP by NDP polyphosphate phosphotransferase 3 from Ruegeria pomeroyi (RpPPK2-3) and describe the covalent immobilisation of RpPPK2-3. In order to select a suitable carrier for the immobilisation of RpPPK2-3, a screening with different amino methacrylate (glutaraldehyde-pre-activated) and epoxy methacrylate carriers was carried out. The epoxy methacrylate carrier ECR8209M (Purolite®) was found to be the most suitable. With a half-life of 462 d when stored at 6 °C and a 50-fold reusability with a 93% residual activity, the immobilised enzyme showed a higher stability compared to the soluble enzyme with a half-life of 0.04 d. Although the half-life of the soluble enzyme could be increased to 32 d by adding PPi, it could not reach the stability of the immobilisate. Due to the resilience of the immobilisate, it is suitable for application in continuous reactor set-ups, e.g., packed-bed reactors.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140433535","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}
引用次数: 0
Liquid-Phase Selective Oxidation of Methane to Methane Oxygenates 液相选择性氧化甲烷生成甲烷氧合物
IF 3.9 3区 化学 Q1 Environmental Science Pub Date : 2024-02-24 DOI: 10.3390/catal14030167
J. Kang, Eun Duck Park
Methane is an abundant and relatively clean fossil fuel resource; therefore, its utilization as a chemical feedstock has a major impact on the chemical industry. However, its inert nature makes direct conversion into value-added products difficult under mild conditions. Compared to the gas-phase selective oxidation of methane, there have been several recent advances in the liquid-phase conversion of methane. This review categorizes the reports on the liquid-phase selective oxidation of methane according to the solvent and oxidant used. The advantages and disadvantages of each approach are discussed. High yields of methyl bisulfate as a methanol precursor can be achieved using SO3 in sulfuric acid; however, more attention should be paid to the separation process and overall economic analysis. However, the aqueous-phase selective oxidation of methane with in situ generated H2O2 is quite promising from an environmental point of view, provided that an economical reducing agent can be used. Based on the current state-of-the-art on this topic, directions for future research are proposed.
甲烷是一种丰富且相对清洁的化石燃料资源,因此,将其用作化学原料对化学工业具有重大影响。然而,甲烷的惰性使其很难在温和条件下直接转化为增值产品。与甲烷的气相选择性氧化相比,最近在甲烷的液相转化方面取得了一些进展。本综述根据所使用的溶剂和氧化剂对有关甲烷液相选择性氧化的报告进行了分类。并讨论了每种方法的优缺点。使用硫酸中的 SO3 可以获得作为甲醇前体的高产率硫酸氢甲酯;但应更多地关注分离过程和总体经济分析。不过,从环保的角度来看,利用原位生成的 H2O2 对甲烷进行水相选择性氧化是非常有前景的,但前提是必须使用经济的还原剂。根据该课题的最新进展,提出了今后的研究方向。
{"title":"Liquid-Phase Selective Oxidation of Methane to Methane Oxygenates","authors":"J. Kang, Eun Duck Park","doi":"10.3390/catal14030167","DOIUrl":"https://doi.org/10.3390/catal14030167","url":null,"abstract":"Methane is an abundant and relatively clean fossil fuel resource; therefore, its utilization as a chemical feedstock has a major impact on the chemical industry. However, its inert nature makes direct conversion into value-added products difficult under mild conditions. Compared to the gas-phase selective oxidation of methane, there have been several recent advances in the liquid-phase conversion of methane. This review categorizes the reports on the liquid-phase selective oxidation of methane according to the solvent and oxidant used. The advantages and disadvantages of each approach are discussed. High yields of methyl bisulfate as a methanol precursor can be achieved using SO3 in sulfuric acid; however, more attention should be paid to the separation process and overall economic analysis. However, the aqueous-phase selective oxidation of methane with in situ generated H2O2 is quite promising from an environmental point of view, provided that an economical reducing agent can be used. Based on the current state-of-the-art on this topic, directions for future research are proposed.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140434579","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}
引用次数: 0
Impact of Metal Impregnation of Commercial Zeolites in the Catalytic Pyrolysis of Real Mixture of Post-Consumer Plastic Waste 商用沸石的金属浸渍对消费后塑料废弃物真实混合物催化热解的影响
IF 3.9 3区 化学 Q1 Environmental Science Pub Date : 2024-02-24 DOI: 10.3390/catal14030168
M.F. Paucar-Sánchez, M. Calero, G. Blázquez, Rafael R. Solís, M. J. Muñoz-Batista, M. A. Martín-Lara
This work reports the study of the catalytic pyrolysis of rejected plastic fractions collected from municipal solid waste whose mechanical recovery is not plausible due to technical or poor conservation issues. The chemical recycling using catalytic pyrolysis was carried out over commercial zeolites formulas, i.e., HY and HZSM-5, in which Ni or Co metals were deposited at two different loadings (1 and 5%, wt.). The presence of these transition metals on the zeolitic supports impacted the total production of compounds existing in the liquid oil. The samples were characterized in terms of structural, chemical, and morphologic properties, and the production of different fuel fractions (gasoline, light cycle oil, and heavy cycle oil) was correlated with a combined parameter defined as a ratio of Acidity/BET area.
这项工作报告了对从城市固体废物中收集的废塑料碎片进行催化热解的研究,由于技术或保存不当等问题,这些碎片无法进行机械回收。利用催化热解的化学回收是在商用沸石配方(即 HY 和 HZSM-5)上进行的,其中镍或钴金属以两种不同的负载量(1% 和 5%,重量比)沉积。这些过渡金属在沸石支持物上的存在影响了液态油中现有化合物的总产量。对样品的结构、化学和形态特性进行了表征,不同燃料馏分(汽油、轻循环油和重循环油)的产量与酸度/BET 面积比值的综合参数相关联。
{"title":"Impact of Metal Impregnation of Commercial Zeolites in the Catalytic Pyrolysis of Real Mixture of Post-Consumer Plastic Waste","authors":"M.F. Paucar-Sánchez, M. Calero, G. Blázquez, Rafael R. Solís, M. J. Muñoz-Batista, M. A. Martín-Lara","doi":"10.3390/catal14030168","DOIUrl":"https://doi.org/10.3390/catal14030168","url":null,"abstract":"This work reports the study of the catalytic pyrolysis of rejected plastic fractions collected from municipal solid waste whose mechanical recovery is not plausible due to technical or poor conservation issues. The chemical recycling using catalytic pyrolysis was carried out over commercial zeolites formulas, i.e., HY and HZSM-5, in which Ni or Co metals were deposited at two different loadings (1 and 5%, wt.). The presence of these transition metals on the zeolitic supports impacted the total production of compounds existing in the liquid oil. The samples were characterized in terms of structural, chemical, and morphologic properties, and the production of different fuel fractions (gasoline, light cycle oil, and heavy cycle oil) was correlated with a combined parameter defined as a ratio of Acidity/BET area.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140435113","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}
引用次数: 0
Enhancing Stability of γ-Al2O3-Supported NiCu Catalysts by Impregnating Basic Oxides in the Hydrodeoxygenation of Anisole 在苯甲醚的加氢脱氧反应中通过浸渍碱性氧化物提高γ-Al2O3支撑的镍铜催化剂的稳定性
IF 3.9 3区 化学 Q1 Environmental Science Pub Date : 2024-02-24 DOI: 10.3390/catal14030166
T. Vandevyvere, Maarten K. Sabbe, J. Thybaut, J. Lauwaert
Basic oxides such as CaO and MgO were added to a γ-Al2O3 support in NiCu-catalyzed hydrodeoxygenation of anisole. A commercial CaO-MgO-γ-Al2O3 was compared to a benchmark γ-Al2O3 and in-house variants with sequential oxide impregnation prior to NiCu impregnation. CaO did not have a significant impact on activity compared to the benchmark, while MgO improved NiCu dispersion, enhancing activity. Co-impregnation of CaO and MgO resulted in intermediate activity. Despite decreased demethoxylation, likely due to moderated support acidity, both CaO-modified and the commercially supported catalysts showed improved stability over 48 h Time On Stream.
在 NiCu 催化的苯甲醚加氢脱氧反应中,将 CaO 和 MgO 等碱性氧化物添加到 γ-Al2O3 支持物中。将商用 CaO-MgO-γ-Al2O3 与基准 γ-Al2O3 和内部变体进行了比较,后者在镍铜浸渍之前进行了连续的氧化物浸渍。与基准相比,氧化钙对活性的影响不大,而氧化镁则改善了镍铜的分散,提高了活性。同时浸渍 CaO 和 MgO 会导致中间活性。尽管脱甲氧基化程度降低,这可能是由于载体酸度降低所致,但经过 CaO 改性的催化剂和商用载体催化剂在 48 小时的通气时间内都显示出更高的稳定性。
{"title":"Enhancing Stability of γ-Al2O3-Supported NiCu Catalysts by Impregnating Basic Oxides in the Hydrodeoxygenation of Anisole","authors":"T. Vandevyvere, Maarten K. Sabbe, J. Thybaut, J. Lauwaert","doi":"10.3390/catal14030166","DOIUrl":"https://doi.org/10.3390/catal14030166","url":null,"abstract":"Basic oxides such as CaO and MgO were added to a γ-Al2O3 support in NiCu-catalyzed hydrodeoxygenation of anisole. A commercial CaO-MgO-γ-Al2O3 was compared to a benchmark γ-Al2O3 and in-house variants with sequential oxide impregnation prior to NiCu impregnation. CaO did not have a significant impact on activity compared to the benchmark, while MgO improved NiCu dispersion, enhancing activity. Co-impregnation of CaO and MgO resulted in intermediate activity. Despite decreased demethoxylation, likely due to moderated support acidity, both CaO-modified and the commercially supported catalysts showed improved stability over 48 h Time On Stream.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140435416","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}
引用次数: 0
Estimating the Anti-Viral Performance of Photocatalytic Materials: The Correlation between Air Purification Efficiency and Severe Acute Respiratory Syndrome Coronavirus 2 Inactivation 估算光催化材料的抗病毒性能:空气净化效率与严重急性呼吸系统综合征冠状病毒 2 灭活之间的相关性
IF 3.9 3区 化学 Q1 Environmental Science Pub Date : 2024-02-23 DOI: 10.3390/catal14030163
Tsuyoshi Ochiai, T. Nagai, Kengo Hamada, Tomoyuki Tobe, Daisuke Aoki, K. Sunada, H. Ishiguro
The coronavirus disease 2019 pandemic has increased the demand for anti-viral products. Photocatalytic materials are used to develop coatings and air purifiers that inactivate severe acute respiratory syndrome coronavirus 2. However, the methods for evaluating the anti-viral performance of photocatalytic materials are time-consuming. To address this problem, herein, we propose a screening test for the anti-viral performance of photocatalytic materials based on the ‘acetaldehyde decomposition test’—an air purification efficiency test used to evaluate the decomposition performance of photocatalytic materials. This test is suitable for screening multiple samples and conditions in a short period. The temporal variation in the acetaldehyde concentration was approximated using an exponential function, similar to the temporal variation in the viral infection values. Thereafter, the slope of the regression line for the acetaldehyde concentration over time was used as an indicator in the screening tests. When the anti-viral performance and acetaldehyde decomposition tests were conducted on the same photocatalytic material, a correlation was observed between the slopes of the regression lines. Overall, the proposed screening test shows good potential for evaluating the anti-viral performance of photocatalytic materials.
冠状病毒疾病 2019 年的大流行增加了对抗病毒产品的需求。光催化材料被用于开发可灭活严重急性呼吸系统综合征冠状病毒 2 的涂层和空气净化器。然而,评估光催化材料抗病毒性能的方法非常耗时。为解决这一问题,我们在此提出一种基于 "乙醛分解试验 "的光催化材料抗病毒性能筛选试验--这是一种用于评估光催化材料分解性能的空气净化效率试验。该测试适用于在短时间内筛选多种样品和条件。乙醛浓度的时间变化用指数函数近似表示,类似于病毒感染值的时间变化。此后,乙醛浓度随时间变化的回归线斜率被用作筛选测试的指标。在同一光催化材料上进行抗病毒性能和乙醛分解测试时,可以观察到回归线斜率之间存在相关性。总之,所提出的筛选测试显示出评估光催化材料抗病毒性能的良好潜力。
{"title":"Estimating the Anti-Viral Performance of Photocatalytic Materials: The Correlation between Air Purification Efficiency and Severe Acute Respiratory Syndrome Coronavirus 2 Inactivation","authors":"Tsuyoshi Ochiai, T. Nagai, Kengo Hamada, Tomoyuki Tobe, Daisuke Aoki, K. Sunada, H. Ishiguro","doi":"10.3390/catal14030163","DOIUrl":"https://doi.org/10.3390/catal14030163","url":null,"abstract":"The coronavirus disease 2019 pandemic has increased the demand for anti-viral products. Photocatalytic materials are used to develop coatings and air purifiers that inactivate severe acute respiratory syndrome coronavirus 2. However, the methods for evaluating the anti-viral performance of photocatalytic materials are time-consuming. To address this problem, herein, we propose a screening test for the anti-viral performance of photocatalytic materials based on the ‘acetaldehyde decomposition test’—an air purification efficiency test used to evaluate the decomposition performance of photocatalytic materials. This test is suitable for screening multiple samples and conditions in a short period. The temporal variation in the acetaldehyde concentration was approximated using an exponential function, similar to the temporal variation in the viral infection values. Thereafter, the slope of the regression line for the acetaldehyde concentration over time was used as an indicator in the screening tests. When the anti-viral performance and acetaldehyde decomposition tests were conducted on the same photocatalytic material, a correlation was observed between the slopes of the regression lines. Overall, the proposed screening test shows good potential for evaluating the anti-viral performance of photocatalytic materials.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140436660","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}
引用次数: 0
Kinetics of Electrocatalytic Oxygen Reduction Reaction over an Activated Glassy Carbon Electrode in an Alkaline Medium 碱性介质中活性玻璃碳电极的电催化氧还原反应动力学
IF 3.9 3区 化学 Q1 Environmental Science Pub Date : 2024-02-23 DOI: 10.3390/catal14030164
M. Siddika, Nazmul Hosen, R. H. Althomali, J. Al-Humaidi, Mohammed M. Rahman, M. Hasnat
Hydrogen peroxide is a promising substitute for fossil fuels because it produces non-hazardous by-products. In this work, a glassy carbon GC was anodized in sulphuric acid at +1.8 V to prepare the working electrode. It was utilized to investigate the oxygen reduction reaction (ORR) in a basic medium containing 0.1 M NaOH as a supporting electrolyte. The objective of this investigation was to synthesize hydrogen peroxide. X-ray photoelectron spectroscopy (XPS), electrochemical impedance spectroscopy (EIS), linear polarization, cyclic voltammetry (CV), and rotating disk electrode voltammetry (RDE) were performed for characterization and investigation of the catalytic properties. The RDE analysis confirmed that oxygen reduction reactions followed two electrons’ process at an activated GC electrode. Hence, the prepared electrode generated hydrogen peroxide from molecular oxygen at a potential of around −0.35 V vs. Ag/AgCl (sat. KCl), significantly lower than the pristine GC surface. The transfer coefficient, standard reduction potential, and standard rate constant were estimated to be 0.75, −0.27 V, and 9.5 × 10−3 cm s−1, respectively.
过氧化氢是一种很有前途的化石燃料替代品,因为它不会产生有害的副产品。在这项研究中,在 +1.8 V 的硫酸中对玻璃碳 GC 进行了阳极氧化处理,以制备工作电极。它被用来研究在含有 0.1 M NaOH 作为支撑电解质的碱性介质中的氧还原反应(ORR)。这项研究的目的是合成过氧化氢。研究人员采用 X 射线光电子能谱 (XPS)、电化学阻抗能谱 (EIS)、线性极化、循环伏安法 (CV) 和旋转盘电极伏安法 (RDE) 对催化特性进行了表征和研究。RDE 分析证实,在活化的 GC 电极上,氧还原反应遵循双电子过程。因此,制备的电极从分子氧生成过氧化氢的电位约为 -0.35 V,相对于 Ag/AgCl(饱和氯化钾),明显低于原始 GC 表面。据估计,转移系数、标准还原电位和标准速率常数分别为 0.75、-0.27 V 和 9.5 × 10-3 cm s-1。
{"title":"Kinetics of Electrocatalytic Oxygen Reduction Reaction over an Activated Glassy Carbon Electrode in an Alkaline Medium","authors":"M. Siddika, Nazmul Hosen, R. H. Althomali, J. Al-Humaidi, Mohammed M. Rahman, M. Hasnat","doi":"10.3390/catal14030164","DOIUrl":"https://doi.org/10.3390/catal14030164","url":null,"abstract":"Hydrogen peroxide is a promising substitute for fossil fuels because it produces non-hazardous by-products. In this work, a glassy carbon GC was anodized in sulphuric acid at +1.8 V to prepare the working electrode. It was utilized to investigate the oxygen reduction reaction (ORR) in a basic medium containing 0.1 M NaOH as a supporting electrolyte. The objective of this investigation was to synthesize hydrogen peroxide. X-ray photoelectron spectroscopy (XPS), electrochemical impedance spectroscopy (EIS), linear polarization, cyclic voltammetry (CV), and rotating disk electrode voltammetry (RDE) were performed for characterization and investigation of the catalytic properties. The RDE analysis confirmed that oxygen reduction reactions followed two electrons’ process at an activated GC electrode. Hence, the prepared electrode generated hydrogen peroxide from molecular oxygen at a potential of around −0.35 V vs. Ag/AgCl (sat. KCl), significantly lower than the pristine GC surface. The transfer coefficient, standard reduction potential, and standard rate constant were estimated to be 0.75, −0.27 V, and 9.5 × 10−3 cm s−1, respectively.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140436963","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}
引用次数: 0
Enzymes in Biomedical, Cosmetic and Food Application 酶在生物医学、化妆品和食品中的应用
IF 3.9 3区 化学 Q1 Environmental Science Pub Date : 2024-02-22 DOI: 10.3390/catal14030162
Chia-Hung Kuo, Haibo Wang, C. Shieh
Enzymes play an important role in biomedical, cosmetic and food applications, and their effects are mainly related to their specific reactions and catalytic activity [...]
酶在生物医学、化妆品和食品应用中发挥着重要作用,其效果主要与其特定反应和催化活性有关 [...]
{"title":"Enzymes in Biomedical, Cosmetic and Food Application","authors":"Chia-Hung Kuo, Haibo Wang, C. Shieh","doi":"10.3390/catal14030162","DOIUrl":"https://doi.org/10.3390/catal14030162","url":null,"abstract":"Enzymes play an important role in biomedical, cosmetic and food applications, and their effects are mainly related to their specific reactions and catalytic activity [...]","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140438123","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}
引用次数: 0
期刊
Catalysts
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1