The catalytic conversion of naturally rich and renewable biomass into high-value chemicals is of great significance for pursuing a sustainable future and a green economy. The preparation of pentanediol from furfuryl alcohol is an important means of high-value conversion of biomass. The Pt-based catalyst supported on MgO was applied to the selective hydrogenation of biomass furfuryl alcohol to prepare pentanediol. By adjusting parameters such as catalyst loading, reduction temperature, reaction temperature, and pressure, a highly active catalyst was designed and the optimal catalytic hydrogenation conditions were determined. The hydrogenation experiment results showed that the selectivity of the 2Pt/MgO-200 catalyst for 1,2-pentanediol and 1,5-pentanediol reached 59.4% and 15.2%, respectively, under 160 °C and 1 MPa hydrogen pressure. The catalyst was characterized by X-ray powder diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectrometer (XPS), CO2-temperature programmed desorption (CO2-TPD), and other methods. The characterization results indicate that the reduction temperature has a significant impact on the metal Pt, and an appropriate reduction temperature is beneficial for the hydrogenation performance of the catalyst. In addition, the basic sites on the carrier are also another important factor affecting the activity of the catalyst. In addition, stability tests were conducted on the catalyst, and the reasons for catalyst deactivation were studied using methods such as thermogravimetric analysis (TGA) and Fourier transform infrared spectroscopy (FT-IR). The results showed that the activity of the catalyst decreased after five cycles, and the deactivation was due to the hydrolysis of the carrier, the increase in metal particle size, and the surface adsorption of organic matter.
{"title":"Selective Hydrogenolysis of Furfuryl Alcohol to Pentanediol over Pt Supported on MgO","authors":"Yuhao Yang, Qiao‐Ling Liu, Zhongyi Liu","doi":"10.3390/catal14040223","DOIUrl":"https://doi.org/10.3390/catal14040223","url":null,"abstract":"The catalytic conversion of naturally rich and renewable biomass into high-value chemicals is of great significance for pursuing a sustainable future and a green economy. The preparation of pentanediol from furfuryl alcohol is an important means of high-value conversion of biomass. The Pt-based catalyst supported on MgO was applied to the selective hydrogenation of biomass furfuryl alcohol to prepare pentanediol. By adjusting parameters such as catalyst loading, reduction temperature, reaction temperature, and pressure, a highly active catalyst was designed and the optimal catalytic hydrogenation conditions were determined. The hydrogenation experiment results showed that the selectivity of the 2Pt/MgO-200 catalyst for 1,2-pentanediol and 1,5-pentanediol reached 59.4% and 15.2%, respectively, under 160 °C and 1 MPa hydrogen pressure. The catalyst was characterized by X-ray powder diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectrometer (XPS), CO2-temperature programmed desorption (CO2-TPD), and other methods. The characterization results indicate that the reduction temperature has a significant impact on the metal Pt, and an appropriate reduction temperature is beneficial for the hydrogenation performance of the catalyst. In addition, the basic sites on the carrier are also another important factor affecting the activity of the catalyst. In addition, stability tests were conducted on the catalyst, and the reasons for catalyst deactivation were studied using methods such as thermogravimetric analysis (TGA) and Fourier transform infrared spectroscopy (FT-IR). The results showed that the activity of the catalyst decreased after five cycles, and the deactivation was due to the hydrolysis of the carrier, the increase in metal particle size, and the surface adsorption of organic matter.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140374325","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}
Olga M. Zhigalina, Olga S. Morozova, D. Khmelenin, A. A. Firsova, Olga V. Silchenkova, G. Vorobieva, A. Bukhtiyarov, Evgeny N. Cherkovskiy, V. G. Basu
An effect of Cu powder dispersion and morphology on the surface structure and the physical–chemical and catalytic properties of Cu–CeO2 catalysts prepared by mechanochemical synthesis was studied in the preferential CO oxidation in a H2-rich stream (CO-PROX). Two catalysts, produced by 30 min ball-milling from CeO2 and 8 mass% of copper powders and with particle sizes of several tens (dendrite-like Cu) and 50–200 nm (spherical Cu obtained with levitation-jet method), respectively, were characterized by X-ray diffraction and electron microscopy methods, a temperature-programmed reduction with CO and H2, and with Fourier-transform infrared spectroscopy. The catalyst synthesized from the “large-scale” dendrite-like Cu powder, whose surface consisted of CuxO (Cu+) agglomerates located directly on the surface of facetted CeO2 crystals with a CeO2(111) and CeO2(100) crystal planes exposition, was approximately two times less active at 120–160 °C than the catalyst synthesized from the fine Cu powder, whose surface consisted of CuxO (Cu2+) clusters of 4–6 nm in size located on the steps of facetted CeO2 nanocrystals. Although a large part of CO2 reacted with a ceria surface to give carbonate-like species, no blockage of CO-activating centers was observed due to the surface architecture. The surface structure formed by the use of highly dispersed Cu powder is found to be a key factor responsible for the catalytic activity.
在富含 H2- 的气流中优先进行 CO 氧化（CO-PROX）时，研究了铜粉分散和形态对机械化学合成法制备的 Cu-CeO2 催化剂的表面结构、物理化学和催化特性的影响。通过 X 射线衍射和电子显微镜方法、CO 和 H2 的温度编程还原以及傅立叶变换红外光谱法对两种催化剂进行了表征。由 "大型 "树枝状 Cu 粉末合成的催化剂在 120-160 °C时的活性大约是由细小 Cu 粉末合成的催化剂的两倍，后者的表面由位于刻面 CeO2 纳米晶体台阶上的 4-6 nm 大小的 CuxO（Cu2+）团簇组成。虽然大部分二氧化碳与铈表面发生反应，生成类似碳酸盐的物质，但由于表面结构的原因，没有观察到二氧化碳活化中心被阻塞。使用高度分散的铜粉末形成的表面结构是催化活性的关键因素。
{"title":"Effect of Copper Particle Size on the Surface Structure and Catalytic Activity of Cu–CeO2 Nanocomposites Prepared by Mechanochemical Synthesis in the Preferential CO Oxidation in a H2-Rich Stream (CO-PROX)","authors":"Olga M. Zhigalina, Olga S. Morozova, D. Khmelenin, A. A. Firsova, Olga V. Silchenkova, G. Vorobieva, A. Bukhtiyarov, Evgeny N. Cherkovskiy, V. G. Basu","doi":"10.3390/catal14040222","DOIUrl":"https://doi.org/10.3390/catal14040222","url":null,"abstract":"An effect of Cu powder dispersion and morphology on the surface structure and the physical–chemical and catalytic properties of Cu–CeO2 catalysts prepared by mechanochemical synthesis was studied in the preferential CO oxidation in a H2-rich stream (CO-PROX). Two catalysts, produced by 30 min ball-milling from CeO2 and 8 mass% of copper powders and with particle sizes of several tens (dendrite-like Cu) and 50–200 nm (spherical Cu obtained with levitation-jet method), respectively, were characterized by X-ray diffraction and electron microscopy methods, a temperature-programmed reduction with CO and H2, and with Fourier-transform infrared spectroscopy. The catalyst synthesized from the “large-scale” dendrite-like Cu powder, whose surface consisted of CuxO (Cu+) agglomerates located directly on the surface of facetted CeO2 crystals with a CeO2(111) and CeO2(100) crystal planes exposition, was approximately two times less active at 120–160 °C than the catalyst synthesized from the fine Cu powder, whose surface consisted of CuxO (Cu2+) clusters of 4–6 nm in size located on the steps of facetted CeO2 nanocrystals. Although a large part of CO2 reacted with a ceria surface to give carbonate-like species, no blockage of CO-activating centers was observed due to the surface architecture. The surface structure formed by the use of highly dispersed Cu powder is found to be a key factor responsible for the catalytic activity.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140376473","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}
Water splitting is considered a renewable and eco−friendly technique for future clean energy requirements to realize green hydrogen production, which is, to a large extent, hindered by the oxygen evolution reaction (OER) process. In recent years, two−dimensional (2D) carbon−based electrocatalysts have drawn sustained attention owing to their good electrical conductivity, unique physicochemical properties, and excellent electrocatalytic performance. Particularly, it is easy for 2D carbon−based materials to form nanocomposites, which further provides an effective strategy for electrocatalytic applications. In this review, we discuss recent advances in synthetic methods, structure−property relationships, and a basic understanding of electrocatalytic mechanisms of 2D carbon−based electrocatalysts for water oxidation. In detail, precious, non−precious metal−doped, and non−metallic 2D carbon−based electrocatalysts, as well as 2D carbon−based confined electrocatalysts, are introduced to conduct OER. Finally, current challenges, opportunities, and perspectives for further research directions of 2D carbon−based nanomaterials are outlined. This review can provide significant comprehension of high−performance 2D carbon−based electrocatalysts for water-splitting applications.
{"title":"Recent Developments in Two-Dimensional Carbon-Based Nanomaterials for Electrochemical Water Oxidation: A Mini Review","authors":"Yuxin Zhao, Siyuan Niu, Baichuan Xi, Zurong Du, Ting Yu, Tongtao Wan, Chaojun Lei, Siliu Lyu","doi":"10.3390/catal14040221","DOIUrl":"https://doi.org/10.3390/catal14040221","url":null,"abstract":"Water splitting is considered a renewable and eco−friendly technique for future clean energy requirements to realize green hydrogen production, which is, to a large extent, hindered by the oxygen evolution reaction (OER) process. In recent years, two−dimensional (2D) carbon−based electrocatalysts have drawn sustained attention owing to their good electrical conductivity, unique physicochemical properties, and excellent electrocatalytic performance. Particularly, it is easy for 2D carbon−based materials to form nanocomposites, which further provides an effective strategy for electrocatalytic applications. In this review, we discuss recent advances in synthetic methods, structure−property relationships, and a basic understanding of electrocatalytic mechanisms of 2D carbon−based electrocatalysts for water oxidation. In detail, precious, non−precious metal−doped, and non−metallic 2D carbon−based electrocatalysts, as well as 2D carbon−based confined electrocatalysts, are introduced to conduct OER. Finally, current challenges, opportunities, and perspectives for further research directions of 2D carbon−based nanomaterials are outlined. This review can provide significant comprehension of high−performance 2D carbon−based electrocatalysts for water-splitting applications.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140381746","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}
Meso-diaminopimelate dehydrogenase (meso-DAPDH) from Corynebacterium glutamicum ATCC13032 (CgDAPDH) is a type I meso-DAPDH that shows obvious preference toward meso-diaminopimelate (meso-DAP) and exhibits almost no amination activity toward 2-keto acids. There are seven distinct conserved insertions and deletions (indels) between type I and type II meso-DAPDH. The current functional analysis of indels is not comprehensive in meso-DAPDH. Continuing from our previous work on these indels, we first examined the functions of the other indels shown as insertion residues in type I CgDAPDH. Alanine mutations in M216, T240, K289, and Q290 lost at least 40% of their activity, highlighting the importance of these four sites in CgDAPDH. Molecular dynamic analysis indicated that the four non-active sites altered the dynamic network of interactions within the protein. Subsequently, these four sites together with the previously identified indel-related residues R180, L176, and H193 were targeted by site-saturation mutagenesis to improve the amination ability of CgDAPDH toward pyruvic acid. The most significant improvement was observed with the mutant CgL176R, which showed a six-fold increase toward pyruvic acid in kcat/Km compared to wild-type CgDAPDH. Overall, our study provides new hotspots and ideas for the subsequent protein engineering of CgDAPDH, which may also be applied to other meso-DAPDHs.
谷氨酸棒杆菌（Corynebacterium glutamicum）ATCC13032（CgDAPDH）的中二氨基庚二酸脱氢酶（meso-DAPDH）是一种 I 型中二氨基庚二酸脱氢酶，对中二氨基庚二酸（meso-DAP）有明显的偏好，对 2-酮酸几乎没有胺化活性。在 I 型和 II 型中-DAPDH 之间有 7 个明显的保守插入和缺失（indels）。目前对介导-DAPDH 的吲哚功能分析还不够全面。在继续之前关于这些吲哚的研究的基础上，我们首先研究了 I 型 CgDAPDH 中显示为插入残基的其他吲哚的功能。M216、T240、K289 和 Q290 中的丙氨酸突变失去了至少 40% 的活性，突出了这四个位点在 CgDAPDH 中的重要性。分子动态分析表明，这四个非活性位点改变了蛋白质内部相互作用的动态网络。随后，针对这四个位点以及之前发现的与吲哚相关的残基 R180、L176 和 H193 进行了位点饱和突变，以提高 CgDAPDH 对丙酮酸的胺化能力。与野生型 CgDAPDH 相比，突变体 CgL176R 对丙酮酸的转化率提高了六倍。总之，我们的研究为后续的 CgDAPDH 蛋白工程提供了新的热点和思路，也可应用于其他中型 DAPDH。
{"title":"Studies on Insertion/Deletion Residues for Functional Analysis and Improved Amination Activity in Meso-DAPDH from Corynebacterium glutamicum","authors":"Yaning Zhang, Jiaying Hao, Yongjun Cao, Wenjun Zhao, Hankun Liu, Xiuzhen Gao, Qinyuan Ma","doi":"10.3390/catal14040220","DOIUrl":"https://doi.org/10.3390/catal14040220","url":null,"abstract":"Meso-diaminopimelate dehydrogenase (meso-DAPDH) from Corynebacterium glutamicum ATCC13032 (CgDAPDH) is a type I meso-DAPDH that shows obvious preference toward meso-diaminopimelate (meso-DAP) and exhibits almost no amination activity toward 2-keto acids. There are seven distinct conserved insertions and deletions (indels) between type I and type II meso-DAPDH. The current functional analysis of indels is not comprehensive in meso-DAPDH. Continuing from our previous work on these indels, we first examined the functions of the other indels shown as insertion residues in type I CgDAPDH. Alanine mutations in M216, T240, K289, and Q290 lost at least 40% of their activity, highlighting the importance of these four sites in CgDAPDH. Molecular dynamic analysis indicated that the four non-active sites altered the dynamic network of interactions within the protein. Subsequently, these four sites together with the previously identified indel-related residues R180, L176, and H193 were targeted by site-saturation mutagenesis to improve the amination ability of CgDAPDH toward pyruvic acid. The most significant improvement was observed with the mutant CgL176R, which showed a six-fold increase toward pyruvic acid in kcat/Km compared to wild-type CgDAPDH. Overall, our study provides new hotspots and ideas for the subsequent protein engineering of CgDAPDH, which may also be applied to other meso-DAPDHs.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140387180","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}
Xiaoxiao Dong, Chengnan Zhang, P. Patil, Weiwei Li, Xiuting Li
Metal–organic frameworks (MOFs) are regarded as excellent carriers for immobilized enzymes due to their substantial specific surface area, high porosity, and easily tunable pore size. Nevertheless, the use of UIO−66 material is significantly limited in immobilized enzymes due to the absence of active functional groups on its surface. This study comprised the synthesis of UIO−66 and subsequent modification of the proline (Pro) on UIO−66 through post-synthetic modification. UIO−66 and UIO−66/Pro crystals were employed as matrices to immobilize Rhizopus oryzae lipase (ROL). The contact angle demonstrated that the introduction of Pro onto UIO−66 resulted in favorable conformational changes in the structure of ROL. The immobilized enzyme ROL@UIO−66/Pro, produced via the covalent-bonding method, exhibited greater activity (0.064715 U/mg (about 1.73 times that of the free enzyme)) and stability in the ester hydrolysis reaction. The immobilized enzymes ROL@UIO−66 (131.193 mM) and ROL@UIO−66/Pro (121.367 mM), which were synthesized using the covalent-bonding approach, exhibited a lower Km and higher substrate affinity compared to the immobilized enzyme ROL@UIO−66/Pro (24.033 mM) produced via the adsorption method. This lays a solid foundation for the industrialization of immobilized enzymes.
{"title":"Preparation of Proline-Modified UIO−66 Nanomaterials and Investigation of Their Potential in Lipase Immobilization","authors":"Xiaoxiao Dong, Chengnan Zhang, P. Patil, Weiwei Li, Xiuting Li","doi":"10.3390/catal14030180","DOIUrl":"https://doi.org/10.3390/catal14030180","url":null,"abstract":"Metal–organic frameworks (MOFs) are regarded as excellent carriers for immobilized enzymes due to their substantial specific surface area, high porosity, and easily tunable pore size. Nevertheless, the use of UIO−66 material is significantly limited in immobilized enzymes due to the absence of active functional groups on its surface. This study comprised the synthesis of UIO−66 and subsequent modification of the proline (Pro) on UIO−66 through post-synthetic modification. UIO−66 and UIO−66/Pro crystals were employed as matrices to immobilize Rhizopus oryzae lipase (ROL). The contact angle demonstrated that the introduction of Pro onto UIO−66 resulted in favorable conformational changes in the structure of ROL. The immobilized enzyme ROL@UIO−66/Pro, produced via the covalent-bonding method, exhibited greater activity (0.064715 U/mg (about 1.73 times that of the free enzyme)) and stability in the ester hydrolysis reaction. The immobilized enzymes ROL@UIO−66 (131.193 mM) and ROL@UIO−66/Pro (121.367 mM), which were synthesized using the covalent-bonding approach, exhibited a lower Km and higher substrate affinity compared to the immobilized enzyme ROL@UIO−66/Pro (24.033 mM) produced via the adsorption method. This lays a solid foundation for the industrialization of immobilized enzymes.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140080600","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}
The dry reforming of methane (DRM) is a promising method for controlling greenhouse gas emissions by converting CO2 and CH4 into syngas, a mixture of CO and H2. Ni-based catalysts have been intensively investigated for their use in the DRM. However, they are limited by the formation of carbonaceous materials on their surfaces. In this review, we explore carbon-induced catalyst deactivation mechanisms and summarize the recent research progress in controlling and mitigating carbon deposition by developing coke-resistant Ni-based catalysts. This review emphasizes the significance of support, alloy, and catalyst structural strategies, and the importance of comprehending the interactions between catalyst components to achieve improved catalytic performance and stability.
甲烷干重整（DRM）通过将二氧化碳和甲烷转化为合成气（二氧化碳和氢气的混合物），是一种很有前景的控制温室气体排放的方法。人们对 Ni 基催化剂在 DRM 中的应用进行了深入研究。然而，这些催化剂受限于其表面碳质材料的形成。在本综述中，我们探讨了碳引起的催化剂失活机制，并总结了通过开发抗焦镍基催化剂来控制和减少碳沉积的最新研究进展。本综述强调了支撑物、合金和催化剂结构策略的重要性，以及理解催化剂组分之间的相互作用对于提高催化性能和稳定性的重要性。
{"title":"Recent Advances in Coke Management for Dry Reforming of Methane over Ni-Based Catalysts","authors":"Zhen Xu, Eun Duck Park","doi":"10.3390/catal14030176","DOIUrl":"https://doi.org/10.3390/catal14030176","url":null,"abstract":"The dry reforming of methane (DRM) is a promising method for controlling greenhouse gas emissions by converting CO2 and CH4 into syngas, a mixture of CO and H2. Ni-based catalysts have been intensively investigated for their use in the DRM. However, they are limited by the formation of carbonaceous materials on their surfaces. In this review, we explore carbon-induced catalyst deactivation mechanisms and summarize the recent research progress in controlling and mitigating carbon deposition by developing coke-resistant Ni-based catalysts. This review emphasizes the significance of support, alloy, and catalyst structural strategies, and the importance of comprehending the interactions between catalyst components to achieve improved catalytic performance and stability.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140087291","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}
Antía Fdez-Sanromán, Marta Pazos, E. Rosales, Ángeles Sanromán
This comprehensive review explores recent advancements in immobilization strategies for graphitic carbon nitride (g-C3N4), a metal-free photocatalyst that has gained significant attention for its optical and physicochemical properties comparable to traditional photocatalysts like TiO2. However, a critical challenge regarding their application has emerged from the difficulty of its recovery due to its powdery nature. Therefore, several alternatives are being explored to immobilize this material, facilitating its recovery and reuse. This review systematically categorizes various physical and chemical immobilization techniques, providing an in-depth analysis of their advantages, drawbacks, and applications. Techniques such as encapsulation, electrospinning, casting, and coating, along with their adaptations for g-C3N4, are thoroughly examined. Additionally, the impact of these strategies on enhancing the photocatalytic efficiency and operational stability of g-C3N4, particularly in environmental applications, is also assessed. Thus, this review aims to provide valuable insights and guide future research in the realms of photocatalysis and environmental remediation. The review contributes to the understanding of how immobilization strategies can optimize the performance of g-C3N4, furthering its potential applications in sustainable and efficient environmental solutions.
{"title":"Pushing the Operational Barriers for g-C3N4: A Comprehensive Review of Cutting-Edge Immobilization Strategies","authors":"Antía Fdez-Sanromán, Marta Pazos, E. Rosales, Ángeles Sanromán","doi":"10.3390/catal14030175","DOIUrl":"https://doi.org/10.3390/catal14030175","url":null,"abstract":"This comprehensive review explores recent advancements in immobilization strategies for graphitic carbon nitride (g-C3N4), a metal-free photocatalyst that has gained significant attention for its optical and physicochemical properties comparable to traditional photocatalysts like TiO2. However, a critical challenge regarding their application has emerged from the difficulty of its recovery due to its powdery nature. Therefore, several alternatives are being explored to immobilize this material, facilitating its recovery and reuse. This review systematically categorizes various physical and chemical immobilization techniques, providing an in-depth analysis of their advantages, drawbacks, and applications. Techniques such as encapsulation, electrospinning, casting, and coating, along with their adaptations for g-C3N4, are thoroughly examined. Additionally, the impact of these strategies on enhancing the photocatalytic efficiency and operational stability of g-C3N4, particularly in environmental applications, is also assessed. Thus, this review aims to provide valuable insights and guide future research in the realms of photocatalysis and environmental remediation. The review contributes to the understanding of how immobilization strategies can optimize the performance of g-C3N4, furthering its potential applications in sustainable and efficient environmental solutions.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140418119","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}
The removal of contaminants from wastewater, which are produced by human activities, and the development of new means of renewable energy production are the main issues that need to be addressed to solve environmental problems [...]
{"title":"Application of Photocatalysts in Environmental Chemistry","authors":"Paola Semeraro, R. Comparelli","doi":"10.3390/catal14030174","DOIUrl":"https://doi.org/10.3390/catal14030174","url":null,"abstract":"The removal of contaminants from wastewater, which are produced by human activities, and the development of new means of renewable energy production are the main issues that need to be addressed to solve environmental problems [...]","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":null,"pages":null},"PeriodicalIF":3.9,"publicationDate":"2024-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140419103","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}
Antibacterial coordination compounds have attracted tremendous attention ascribed to their excellent designability. However, how the morphological evolution of these complexes influences their antibacterial and physicochemical properties has never been investigated based on proposed mechanisms. Thus, a series of Co–HOAT coordination compounds synthesized from inorganic to organic cobalt sources were prepared. We propose that with the same HOAT ligand, inorganic Co–HOAT nanosheets possess higher sterilization rates compared with organic Co–HOAT nanoparticles. This is explained by the different steric hindrance of cobalt sources. Relatively small steric hindrance could lead to ample active positions for inorganic cobalt ions to coordinate with both N and O atoms in HOAT. Meanwhile, organic Co2+ ions could only unite with N atoms in HOAT. Furthermore, by theoretical calculation, cobalt ions with adequate coordination sites are beneficial for developing nanosheet morphologies. Meanwhile, the Co–HOAT complexes with a lower density of electron clouds present higher sterilization rates due to the anchoring effect of electrostatic attraction. The proposed mechanism is that Co2+ released from compounds could cause multiple toxic effects to bacteria anchored by Co–HOATs. Finally, Co–HOATs’ behaviors have excellent antimicrobial properties without environmental limitations. In conclusion, the Co–HOATs appear to be a potential antibacterial catalyst in the antimicrobial field.
抗菌配位化合物因其出色的可设计性而备受关注。然而，这些配合物的形态演变如何影响它们的抗菌和理化性质，还从未根据提出的机制进行过研究。因此，我们制备了一系列从无机到有机钴源合成的 Co-HOAT 配位化合物。我们认为，与有机 Co-HOAT 纳米粒子相比，在相同的 HOAT 配体下，无机 Co-HOAT 纳米片材具有更高的杀菌率。这是因为钴源的立体阻碍不同。相对较小的立体阻碍可为无机钴离子与 HOAT 中的 N 原子和 O 原子配位提供充足的活性位置。与此同时，有机 Co2+ 离子只能与 HOAT 中的 N 原子结合。此外，通过理论计算，具有足够配位位点的钴离子有利于形成纳米片形态。同时，由于静电吸引的锚定效应，电子云密度较低的 Co-HOAT 复合物具有更高的杀菌率。提出的机理是化合物释放的 Co2+ 可对被 Co-HOATs 固定的细菌产生多种毒性作用。最后，Co-HOATs 的行为具有出色的抗菌特性，不受环境限制。总之，Co-HOATs 似乎是抗菌领域一种潜在的抗菌催化剂。
{"title":"Co–HOAT Complexes Change Their Antibacterial and Physicochemical Properties with Morphological Evolution","authors":"Xiaolin Xu, Mengna Ding, Shiwen Yu, Fujian Lv, Yun Zhang, Yingchun Miao, Zhenfeng Bian, Hexing Li","doi":"10.3390/catal14030173","DOIUrl":"https://doi.org/10.3390/catal14030173","url":null,"abstract":"Antibacterial coordination compounds have attracted tremendous attention ascribed to their excellent designability. However, how the morphological evolution of these complexes influences their antibacterial and physicochemical properties has never been investigated based on proposed mechanisms. Thus, a series of Co–HOAT coordination compounds synthesized from inorganic to organic cobalt sources were prepared. We propose that with the same HOAT ligand, inorganic Co–HOAT nanosheets possess higher sterilization rates compared with organic Co–HOAT nanoparticles. This is explained by the different steric hindrance of cobalt sources. Relatively small steric hindrance could lead to ample active positions for inorganic cobalt ions to coordinate with both N and O atoms in HOAT. Meanwhile, organic Co2+ ions could only unite with N atoms in HOAT. Furthermore, by theoretical calculation, cobalt ions with adequate coordination sites are beneficial for developing nanosheet morphologies. Meanwhile, the Co–HOAT complexes with a lower density of electron clouds present higher sterilization rates due to the anchoring effect of electrostatic attraction. The proposed mechanism is that Co2+ released from compounds could cause multiple toxic effects to bacteria anchored by Co–HOATs. Finally, Co–HOATs’ behaviors have excellent antimicrobial properties without environmental limitations. In conclusion, the Co–HOATs appear to be a potential antibacterial catalyst in the antimicrobial field.","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":"140425385","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}
A. Imgharn, Tingwei Sun, Jimmy Nicolle, Y. Naciri, A. Hsini, A. Albourine, C. Ania
The adequate optical properties, low cost, and thermal stability of graphitic carbon nitride and molybdenum oxide make them both promising materials for photocatalytic applications. However, they both suffer from strong recombination of their photogenerated charge carriers. Therefore, searching for strategies that enable an efficient charge carrier separation is desirable for improving the photocatalytic performance of both semiconductors. In this work, we have synthesized a g-C3N4/MoO3 heterojunction by a facile solid dispersion approach to the pristine semiconductors that allows a uniform dispersion of the two phases in the heterojunction. The resulting hybrid photocatalyst exhibits light absorption features similar to pristine g-C3N4 and presents an improved separation of the photogenerated charge carriers, likely through a Z-scheme between both semiconductor phases, as inferred by photoelectrochemical measurements. As a result, the g-C3N4/MoO3 heterojunction showed better photocatalytic activity than the individual semiconductors and good cycling stability for the degradation of methylparaben and its reaction intermediates. We drew these conclusions based on total organic carbon (TOC) measurements.
氮化石墨碳和氧化钼具有良好的光学特性、低成本和热稳定性，因此都是很有前途的光催化应用材料。然而，它们都存在光生电荷载流子强烈重组的问题。因此，寻找能够实现高效电荷载流子分离的策略是提高这两种半导体光催化性能的理想方法。在这项工作中，我们采用一种简单的固体分散方法合成了 g-C3N4/MoO3 异质结，这种方法可以使两种半导体在异质结中均匀分散。由此产生的混合光催化剂具有与原始 g-C3N4 相似的光吸收特性，并且根据光电化学测量的推断，光生电荷载流子的分离得到了改善，这可能是通过两种半导体相之间的 Z 型结构实现的。因此，g-C3N4/MoO3 异质结在降解苯甲酸甲酯及其反应中间产物方面比单独的半导体具有更好的光催化活性和良好的循环稳定性。我们是根据总有机碳（TOC）的测量结果得出上述结论的。
{"title":"A Simple Approach to Prepare a C3N4/MoO3 Heterojunction with Improved Photocatalytic Performance for the Degradation of Methylparaben","authors":"A. Imgharn, Tingwei Sun, Jimmy Nicolle, Y. Naciri, A. Hsini, A. Albourine, C. Ania","doi":"10.3390/catal14030170","DOIUrl":"https://doi.org/10.3390/catal14030170","url":null,"abstract":"The adequate optical properties, low cost, and thermal stability of graphitic carbon nitride and molybdenum oxide make them both promising materials for photocatalytic applications. However, they both suffer from strong recombination of their photogenerated charge carriers. Therefore, searching for strategies that enable an efficient charge carrier separation is desirable for improving the photocatalytic performance of both semiconductors. In this work, we have synthesized a g-C3N4/MoO3 heterojunction by a facile solid dispersion approach to the pristine semiconductors that allows a uniform dispersion of the two phases in the heterojunction. The resulting hybrid photocatalyst exhibits light absorption features similar to pristine g-C3N4 and presents an improved separation of the photogenerated charge carriers, likely through a Z-scheme between both semiconductor phases, as inferred by photoelectrochemical measurements. As a result, the g-C3N4/MoO3 heterojunction showed better photocatalytic activity than the individual semiconductors and good cycling stability for the degradation of methylparaben and its reaction intermediates. We drew these conclusions based on total organic carbon (TOC) measurements.","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":"140427360","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}
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