The photosynthetic assemblies in bacteria, as critical structures in early evolutionary photosynthesis, are pivotal for understanding the molecular mechanisms of photosynthesis and for the design of artificial photosynthetic systems. In recent decades, various artificial systems based on synthetic molecules have been developed to mimic these photosynthetic assemblies from structures to functions. This review summarizes the latest advancements in mimicking the photosynthetic assembly systems, discussing three fundamental models: the chlorosome and related complexes in green bacteria, the chromatophore and reaction center system in purple bacteria, and the phycobilisome and photosystem II (PSII) in cyanobacteria, along with their representative mimicking systems. We also address the challenges and unexplored areas in the simulation of photosynthetic systems.
{"title":"Towards Artificial Photosynthetic Assemblies Inspired by Photosynthetic Bacteria","authors":"Yifei Han, Zhan-Ting Li, Jia Tian","doi":"10.1002/cctc.202401365","DOIUrl":"https://doi.org/10.1002/cctc.202401365","url":null,"abstract":"The photosynthetic assemblies in bacteria, as critical structures in early evolutionary photosynthesis, are pivotal for understanding the molecular mechanisms of photosynthesis and for the design of artificial photosynthetic systems. In recent decades, various artificial systems based on synthetic molecules have been developed to mimic these photosynthetic assemblies from structures to functions. This review summarizes the latest advancements in mimicking the photosynthetic assembly systems, discussing three fundamental models: the chlorosome and related complexes in green bacteria, the chromatophore and reaction center system in purple bacteria, and the phycobilisome and photosystem II (PSII) in cyanobacteria, along with their representative mimicking systems. We also address the challenges and unexplored areas in the simulation of photosynthetic systems.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"6 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142253397","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}
Electro‐organic synthesis, a method that uses electrical current to drive various organic transformations has garnered significant attention. Simultaneously, heterogeneous electrosynthesis, a process that produces chemicals through electrochemical reactions at the interface between the electrode and an electrolyte. This concept highlights the synergistic potential of heterogeneous electrocatalysts, particularly in their use in cross‐coupling reactions. After thoroughly analyzing existing literature, key examples have been highlighted where heterogeneous electrocatalysts have facilitated the transformation of simple starting materials into useful products. This process lowers energy consumption and reduces waste. We hope this short review sparks the interest among those involved in organic electrosynthesis to explore and use heterogeneous electrocatalysis for coupling reactions.
{"title":"Heterogeneous Electrocatalysts for Electrochemical Cross‐coupling Reactions","authors":"Apurba K Das, Deepak K. K. Kori","doi":"10.1002/cctc.202401491","DOIUrl":"https://doi.org/10.1002/cctc.202401491","url":null,"abstract":"Electro‐organic synthesis, a method that uses electrical current to drive various organic transformations has garnered significant attention. Simultaneously, heterogeneous electrosynthesis, a process that produces chemicals through electrochemical reactions at the interface between the electrode and an electrolyte. This concept highlights the synergistic potential of heterogeneous electrocatalysts, particularly in their use in cross‐coupling reactions. After thoroughly analyzing existing literature, key examples have been highlighted where heterogeneous electrocatalysts have facilitated the transformation of simple starting materials into useful products. This process lowers energy consumption and reduces waste. We hope this short review sparks the interest among those involved in organic electrosynthesis to explore and use heterogeneous electrocatalysis for coupling reactions.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"6 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142268808","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}
Wenjun Yang, Erik Nieuwlands, Ivan Chernyshov, Georgy Filonenko, Evgeny Alexandrovich Pidko
Many catalytic reactions suffer from product inhibition, which especially hard to control in homogeneous hydrogenation due to the scaling relation between the inhibited and active states of the catalyst. We recently reported one such pathway in Mn(I) hydrogenation and demonstrated that addition of alkoxide bases could affect the thermodynamic favorability of this reaction and selectively suppress the product inhibition. Since external reaction promotors are formally not involved in reaction thermodynamics, we set to investigate the explicit molecular interactions behind these apparently environmental effects. Herein, we reveal that the thermodynamic landscape of the inhibitory process exhibits a non‐monotonic dependence on the base concentration. We related this phenomenon to the presence of two dominant mechanisms operating at different base concentrations. Specifically, the base additives can enhance the ionic strength and lower the free energy of the inhibited state at low promotor concentration. At high base concentrations we suggest the formation of highly labile alcohol‐alkoxide clusters which stabilize the free alcohol and make its addition to the catalyst unfavourable, thereby suppressing the inhibition. While relatively weak, such non‐covalent interactions between reactants and reaction environment can cause substantial perturbations to the free energy of catalytic process, ultimately deciding its fate.
{"title":"Concentration‐Dependent Thermodynamics of the Inhibitory Paths in Homogeneous Mn(I) Hydrogenation Catalysis","authors":"Wenjun Yang, Erik Nieuwlands, Ivan Chernyshov, Georgy Filonenko, Evgeny Alexandrovich Pidko","doi":"10.1002/cctc.202401237","DOIUrl":"https://doi.org/10.1002/cctc.202401237","url":null,"abstract":"Many catalytic reactions suffer from product inhibition, which especially hard to control in homogeneous hydrogenation due to the scaling relation between the inhibited and active states of the catalyst. We recently reported one such pathway in Mn(I) hydrogenation and demonstrated that addition of alkoxide bases could affect the thermodynamic favorability of this reaction and selectively suppress the product inhibition. Since external reaction promotors are formally not involved in reaction thermodynamics, we set to investigate the explicit molecular interactions behind these apparently environmental effects. Herein, we reveal that the thermodynamic landscape of the inhibitory process exhibits a non‐monotonic dependence on the base concentration. We related this phenomenon to the presence of two dominant mechanisms operating at different base concentrations. Specifically, the base additives can enhance the ionic strength and lower the free energy of the inhibited state at low promotor concentration. At high base concentrations we suggest the formation of highly labile alcohol‐alkoxide clusters which stabilize the free alcohol and make its addition to the catalyst unfavourable, thereby suppressing the inhibition. While relatively weak, such non‐covalent interactions between reactants and reaction environment can cause substantial perturbations to the free energy of catalytic process, ultimately deciding its fate.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"114 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142253436","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 conversion of CO2 into valuable chemical fuels addresses both environmental pollution and energy scarcity. However, understanding reaction mechanisms and the dynamic catalyst evolution during CO2 reduction remains a challenge to data. In this review, we present a detailed description of recent advanced in situ characterization techniques, which provide a reliable means of monitoring the intermediate evolution during CO2 reduction and the dynamic evolution of the catalyst, respectively. Finally, we provide an outlook on the development of in situ characterization techniques.
{"title":"Recent advances of in situ insights into CO2 reduction toward fuels","authors":"Liang Chen, Chengbin Zhang, Xingchen Jiao","doi":"10.1002/cctc.202401388","DOIUrl":"https://doi.org/10.1002/cctc.202401388","url":null,"abstract":"The conversion of CO2 into valuable chemical fuels addresses both environmental pollution and energy scarcity. However, understanding reaction mechanisms and the dynamic catalyst evolution during CO2 reduction remains a challenge to data. In this review, we present a detailed description of recent advanced in situ characterization techniques, which provide a reliable means of monitoring the intermediate evolution during CO2 reduction and the dynamic evolution of the catalyst, respectively. Finally, we provide an outlook on the development of in situ characterization techniques.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"18 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208895","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 influence of crystal phase of TiO2 on the catalytic performance of transfer hydrogenation using formic acid (HCOOH) over Pd/TiO2 catalyst has not been clarified before. Herein, Pd/TiO2 catalysts with four typical TiO2 crystal phases, i.e., rutile, anatase, brookite and TiO2(B), were synthesized and analyzed. The catalytic results showed that the TiO2 crystal phase could vary the transfer hydrogenation performance of the Pd/TiO2 catalysts by several to tens of times, which was in the following tendency: Pd/Rutile > Pd/Anatase > Pd/Brookite > Pd/TiO2(B). Detailed comparison manifests the Pd dispersion state is obviously different on various TiO2 surfaces, which the relatively small particle size and more metallic are observed on Pd/Rutile and Pd/Anatase catalysts, contributing to the high catalytic performance. The reaction mechanism study further indicates that HCOOH on Pd/Rutile is more liable to be dehydrogenated than that on other Pd/TiO2 catalysts, especially for the transformation of bidentate to monodentate formate. Pd/Brookite shows the relatively highest selectivity of HCOOH dehydration. However, it is difficult for the HCOOH dehydrogenation to occur on Pd/TiO2(B). This work elucidates the roles of TiO2 crystal phase in Pd/TiO2 catalysts for the transfer hydrogenation reaction, which is expected to facilitate the development of efficient catalysts.
{"title":"Effect of TiO2 crystal phase on the catalytic transfer hydrogenation using formic acid over the Pd/TiO2 catalyst","authors":"Shanshan Chen, Licheng Li, Lili Mu, Zelin Hua, Xuejuan Zhao, Chenxuanzhi Ruan","doi":"10.1002/cctc.202401401","DOIUrl":"https://doi.org/10.1002/cctc.202401401","url":null,"abstract":"The influence of crystal phase of TiO2 on the catalytic performance of transfer hydrogenation using formic acid (HCOOH) over Pd/TiO2 catalyst has not been clarified before. Herein, Pd/TiO2 catalysts with four typical TiO2 crystal phases, i.e., rutile, anatase, brookite and TiO2(B), were synthesized and analyzed. The catalytic results showed that the TiO2 crystal phase could vary the transfer hydrogenation performance of the Pd/TiO2 catalysts by several to tens of times, which was in the following tendency: Pd/Rutile > Pd/Anatase > Pd/Brookite > Pd/TiO2(B). Detailed comparison manifests the Pd dispersion state is obviously different on various TiO2 surfaces, which the relatively small particle size and more metallic are observed on Pd/Rutile and Pd/Anatase catalysts, contributing to the high catalytic performance. The reaction mechanism study further indicates that HCOOH on Pd/Rutile is more liable to be dehydrogenated than that on other Pd/TiO2 catalysts, especially for the transformation of bidentate to monodentate formate. Pd/Brookite shows the relatively highest selectivity of HCOOH dehydration. However, it is difficult for the HCOOH dehydrogenation to occur on Pd/TiO2(B). This work elucidates the roles of TiO2 crystal phase in Pd/TiO2 catalysts for the transfer hydrogenation reaction, which is expected to facilitate the development of efficient catalysts.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"7 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208893","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}
From the perspective of reaction kinetics, the catalytic transfer hydrogenation (CTH) reaction of 5‐hydroxymethylfurfural (HMF) was studied in this work. Its hydrogenation product, 2,5‐dimethylfuran (DMF), was a stable and water‐insoluble biofuel alternative to gasoline. In this study, CuCoOx catalysts were used and 2‐propanol (IPA) was the hydrogen donor. The results exhibited that the HMF conversion reached 100% with the complete formation of DMF at 170 °C. Experimental and characterization results revealed that the balance of metal sites and acid sites was critical, which could inhibit the side reactions and enhance the yield of the target product. By adopting the Langmuir‐Hinshelwood‐Hougen‐Watson (LHHW) kinetic model, it was found that direct hydrogen transfer from IPA to HMF predominated over indirect transfer via H2. Moreover, the results revealed that the hydrogenolysis of BHMF to MFA was the rate‐limiting step. The kinetic study in this work is expected to provide valuable insights into the industrial optimization of the CTH reaction of HMF and lay the foundation for the study of hydrogen transfer pathways in this process.
{"title":"Optimization and reaction kinetics of catalytic transfer hydrogenation of 5‐hydroxymethylfurfural to 2, 5‐dimethylfuran over CuCoOx catalysts","authors":"Ziyi Yan, Xiaofeng Wang, Fandi Zeng, Qingbo Li, Xinhua Liang","doi":"10.1002/cctc.202401412","DOIUrl":"https://doi.org/10.1002/cctc.202401412","url":null,"abstract":"From the perspective of reaction kinetics, the catalytic transfer hydrogenation (CTH) reaction of 5‐hydroxymethylfurfural (HMF) was studied in this work. Its hydrogenation product, 2,5‐dimethylfuran (DMF), was a stable and water‐insoluble biofuel alternative to gasoline. In this study, CuCoOx catalysts were used and 2‐propanol (IPA) was the hydrogen donor. The results exhibited that the HMF conversion reached 100% with the complete formation of DMF at 170 °C. Experimental and characterization results revealed that the balance of metal sites and acid sites was critical, which could inhibit the side reactions and enhance the yield of the target product. By adopting the Langmuir‐Hinshelwood‐Hougen‐Watson (LHHW) kinetic model, it was found that direct hydrogen transfer from IPA to HMF predominated over indirect transfer via H2. Moreover, the results revealed that the hydrogenolysis of BHMF to MFA was the rate‐limiting step. The kinetic study in this work is expected to provide valuable insights into the industrial optimization of the CTH reaction of HMF and lay the foundation for the study of hydrogen transfer pathways in this process.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"151 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208894","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}
An enantioselective Michael addition of α‐substituted acyl‐imidazoles to acrolein catalyzed by a nickel‐bisoxazoline complex has been developed. The use of strong Lewis acid TMSOTf as an additive to activate the Michael acceptors proved to be vital to the success of this process. This process tolerates a wide range of acyl‐imidazoles, and a series of conjugate adducts were obtained in high yields and good enantioselectivities. Besides acrolein, β‐ester ennones are also applicable in this process affording the corresponding conjugate adducts in high yields with good diastereoselectivities and enantioselectivites in most cases. The potential utility of the reaction system was confirmed through 2 mmol‐scale reaction and derivatization experiments.
{"title":"Nickel‐Catalyzed Asymmetric Michael Addition of Acyl Imidazoles to Acrolein or β‐Ester Enones","authors":"Qian Shi, Jiani Sun, Jiangbo Wu, Xuehe Lu, Xiaoyu Wu","doi":"10.1002/cctc.202401324","DOIUrl":"https://doi.org/10.1002/cctc.202401324","url":null,"abstract":"An enantioselective Michael addition of α‐substituted acyl‐imidazoles to acrolein catalyzed by a nickel‐bisoxazoline complex has been developed. The use of strong Lewis acid TMSOTf as an additive to activate the Michael acceptors proved to be vital to the success of this process. This process tolerates a wide range of acyl‐imidazoles, and a series of conjugate adducts were obtained in high yields and good enantioselectivities. Besides acrolein, β‐ester ennones are also applicable in this process affording the corresponding conjugate adducts in high yields with good diastereoselectivities and enantioselectivites in most cases. The potential utility of the reaction system was confirmed through 2 mmol‐scale reaction and derivatization experiments.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"7 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208745","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}
Ludivine K/Bidi, Albert Solé-Daura, Teng Zhang, Alix Desjonquères, Josep Maria Poblet, Anna Proust, Jorge J. Carbó, Geoffroy Guillemot
This report investigates the structural differences in a series of titanium complexes constructed from silanol functionalized polyoxometalate (SiloxPOMs) derivatives, designed to create a constrained coordination site for titanium (IV) cations, namely (THA)3[PW9O34(tBuSiO)3Ti(OiPr)] and (THA)3[SbW9O33(tBuSiO)3Ti(OiPr)]. The complexes serve as structural and functional models for titanium‐silicates, facilitating the epoxidation of allylic alcohols and alkenes by aqueous hydrogen peroxide solutions. The different activity and selectivity observed between the two derivatives are attributed to variations in the polyoxotungstic platform used, A‐type–[XW9O34]n–vs B–type –[YW9O33]3–. A combined experimental and theoretical investigation highlights the influence of these structural differences on water interaction and hydrolytic stability, with A‐type structures proving more susceptible to hydrolysis. In addition, the study also delves into the nuclearity of the active sites, a monomeric titanium (IV)‐hydroperoxide [Ti]–(OOH) active species evidenced by diffusion NMR spectroscopy, and the influence of the presence of water on catalytic performance in epoxidation reaction, thus shedding light on the relationship between catalyst stability, intermediates formed and reaction pathway. The study finally demonstrates the suitability of B‐type SiloxPOM derivatives as models for titanium‐silicates, offering insights into their stability and catalytic activity for epoxidation reactions.
本报告研究了一系列由硅烷醇官能化聚氧化铝酸盐（SiloxPOMs）衍生物构建的钛配合物（即 (THA)3[PW9O34(tBuSiO)3Ti(OiPr)] 和 (THA)3[SbW9O33(tBuSiO)3Ti(OiPr)]）的结构差异，这些配合物旨在为钛（IV）阳离子创建一个受限配位位点。这些配合物可作为钛硅酸盐的结构和功能模型，促进过氧化氢水溶液对烯丙基醇和烯烃的环氧化作用。这两种衍生物的不同活性和选择性归因于所使用的多氧钨平台的变化：A 型-[XW9O34]n 与 B 型-[YW9O33]3-。实验和理论相结合的研究强调了这些结构差异对水相互作用和水解稳定性的影响，A 型结构更容易发生水解。此外，研究还深入探讨了活性位点的核性，即通过扩散核磁共振光谱证明的单体过氧化氢钛 [Ti]-(OOH) 活性物种，以及水的存在对环氧化反应催化性能的影响，从而揭示了催化剂稳定性、形成的中间产物和反应途径之间的关系。该研究最终证明了 B 型 SiloxPOM 衍生物作为钛硅酸盐模型的适用性，为了解它们在环氧化反应中的稳定性和催化活性提供了启示。
{"title":"Epoxidation at Isolated Titanium Site Modeled by Ti‐Siloxy‐Polyoxometalates Built on [α–A–XW9O34]9‐ and [α–B–YW9O33]9‐ Comparative Study of their Hydrolytic Stability","authors":"Ludivine K/Bidi, Albert Solé-Daura, Teng Zhang, Alix Desjonquères, Josep Maria Poblet, Anna Proust, Jorge J. Carbó, Geoffroy Guillemot","doi":"10.1002/cctc.202401106","DOIUrl":"https://doi.org/10.1002/cctc.202401106","url":null,"abstract":"This report investigates the structural differences in a series of titanium complexes constructed from silanol functionalized polyoxometalate (SiloxPOMs) derivatives, designed to create a constrained coordination site for titanium (IV) cations, namely (THA)3[PW9O34(tBuSiO)3Ti(OiPr)] and (THA)3[SbW9O33(tBuSiO)3Ti(OiPr)]. The complexes serve as structural and functional models for titanium‐silicates, facilitating the epoxidation of allylic alcohols and alkenes by aqueous hydrogen peroxide solutions. The different activity and selectivity observed between the two derivatives are attributed to variations in the polyoxotungstic platform used, A‐type–[XW9O34]n–vs B–type –[YW9O33]3–. A combined experimental and theoretical investigation highlights the influence of these structural differences on water interaction and hydrolytic stability, with A‐type structures proving more susceptible to hydrolysis. In addition, the study also delves into the nuclearity of the active sites, a monomeric titanium (IV)‐hydroperoxide [Ti]–(OOH) active species evidenced by diffusion NMR spectroscopy, and the influence of the presence of water on catalytic performance in epoxidation reaction, thus shedding light on the relationship between catalyst stability, intermediates formed and reaction pathway. The study finally demonstrates the suitability of B‐type SiloxPOM derivatives as models for titanium‐silicates, offering insights into their stability and catalytic activity for epoxidation reactions.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"107 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142226555","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}
Xuehua Zhang, Li Zhang, Songlei Lv, Guodong Xu, Jiawei Shi, Jing Li, Weiwei Cai
The electrochemical oxygen evolution reaction (OER) can be combined with various reactions to fabricate electrochemical energy conversion and storage devices while the slow kinetics and poor mass transfer capability at high current densities were the key constraints to its large‐scale application. Therefore, this review primarily focuses on design and optimization of mass transfer structures of TM‐metal‐based OER catalysts. Nanostructuring, porous design, and the creation of hierarchical architectures have been applied during catalyst synthesis to enhance the surface area and accessibility, thereby improving mass transfer and catalytic OER efficiency. Strategies including doping, substrate invitation, soft/hard templating has been utilized to accelerate mass transfer as well as the ion/electron conduction efficiency for the overall improvement of OER performance of the catalysts. These developments underline the critical role of advanced material design in achieving high‐performance OER catalysts and highlight the potential of TM‐based materials in cost‐effective and scalable applications.
电化学氧进化反应（OER）可与各种反应相结合，制造出电化学能量转换和存储装置，但其在高电流密度下的缓慢动力学和较差的传质能力是制约其大规模应用的关键因素。因此，本综述主要关注基于 TM 金属的 OER 催化剂传质结构的设计和优化。在催化剂合成过程中，人们采用纳米结构、多孔设计和创建分层结构来提高表面积和可及性，从而改善传质和催化 OER 的效率。利用掺杂、基底邀请、软/硬模板等策略来加速传质以及离子/电子传导效率，从而全面提高催化剂的 OER 性能。这些发展强调了先进材料设计在实现高性能 OER 催化剂中的关键作用，并突出了基于 TM 的材料在具有成本效益和可扩展应用中的潜力。
{"title":"Recent advantages on mass transfer structure construction in transition metal‐based cost‐effective catalyst toward alkaline oxygen evolution","authors":"Xuehua Zhang, Li Zhang, Songlei Lv, Guodong Xu, Jiawei Shi, Jing Li, Weiwei Cai","doi":"10.1002/cctc.202401166","DOIUrl":"https://doi.org/10.1002/cctc.202401166","url":null,"abstract":"The electrochemical oxygen evolution reaction (OER) can be combined with various reactions to fabricate electrochemical energy conversion and storage devices while the slow kinetics and poor mass transfer capability at high current densities were the key constraints to its large‐scale application. Therefore, this review primarily focuses on design and optimization of mass transfer structures of TM‐metal‐based OER catalysts. Nanostructuring, porous design, and the creation of hierarchical architectures have been applied during catalyst synthesis to enhance the surface area and accessibility, thereby improving mass transfer and catalytic OER efficiency. Strategies including doping, substrate invitation, soft/hard templating has been utilized to accelerate mass transfer as well as the ion/electron conduction efficiency for the overall improvement of OER performance of the catalysts. These developments underline the critical role of advanced material design in achieving high‐performance OER catalysts and highlight the potential of TM‐based materials in cost‐effective and scalable applications.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"1 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208898","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}
Dr. Keigo Tashiro, Hikaru Konno, Akihide Yanagita, Shunta Mikami, Prof. Shuhei Shimoda, Erika Taira, Dr. David S. Rivera Rocabado, Prof. Ken-ichi Shimizu, Prof. Takayoshi Ishimoto, Shigeo Satokawa
The Front Cover illustrates liquid hydrocarbon formation by CO2 hydrogenation through reverse water gas shift and the Fischer–Tropsch synthesis reactions over a supported cobalt catalyst. In their Research Article, Keigo Tashiro, Shigeo Satokawa, and co-workers reveal that lanthanum-doped ceria provides the oxygen vacancies which promote CO2 reduction to CO, and the supported cobalt metals produce long-chain hydrocarbons via Fischer–Tropsch synthesis. As reported by the authors, the CO2 direct Fischer–Tropsch reaction technology will contribute to reaching a bright carbon-neutral future. For more details, see the Research Article by K. Tashiro, S. Satokawa, and co-workers (DOI: 10.1002/cctc.202400261).
封面展示了通过反向水气变换进行二氧化碳加氢形成液态碳氢化合物的过程，以及在支撑钴催化剂上进行的费托合成反应。Keigo Tashiro、Shigeo Satokawa 和合作者在他们的研究文章中揭示，掺镧铈提供的氧空位可促进 CO2 还原成 CO，而支撑钴金属则可通过费托合成生产长链碳氢化合物。正如作者所报告的，二氧化碳直接费托合成反应技术将有助于实现碳中和的美好未来。更多详情，请参阅 K. Tashiro、S. Satokawa 及合作者的研究文章（DOI: 10.1002/cctc.202400261）。
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