ChemCatChem最新文献_第3页

Catalytic Reductive Addition of Imine for Chiral Amine Synthesis: Recent Advances and Future Perspectives 用于手性胺合成的亚胺催化还原加成：最新进展与未来展望

IF 4.5 3区化学

ChemCatChem Pub Date : 2024-09-17 DOI: 10.1002/cctc.202401407

Tingting Xia, Zhiying Yu, Xianqing Wu, Jingping Qu, Yifeng Chen

引用次数: 0

Surface Nanojunction Enabled by Vapor‐Assisted π‐Conjugation Modification of Carbon Nitride for Enhanced Photocatalytic Water Splitting 通过气相辅助π共轭修饰氮化碳实现表面纳米结，从而提高光催化水分离效果

IF 4.5 3区化学

ChemCatChem Pub Date : 2024-09-17 DOI: 10.1002/cctc.202401408

Xiaoxue Lin, Xiaoying Peng, Suqin Wu, Chen Ma, Dou Chen, Quanming Peng, Kai Yang, Fan Liu, Shungao Yin, Guiming Peng

{"title":"Surface Nanojunction Enabled by Vapor‐Assisted π‐Conjugation Modification of Carbon Nitride for Enhanced Photocatalytic Water Splitting","authors":"Xiaoxue Lin, Xiaoying Peng, Suqin Wu, Chen Ma, Dou Chen, Quanming Peng, Kai Yang, Fan Liu, Shungao Yin, Guiming Peng","doi":"10.1002/cctc.202401408","DOIUrl":"https://doi.org/10.1002/cctc.202401408","url":null,"abstract":"The unsatisfied visible light harvesting, slow charge separation, and limited practical surface area of carbon nitride (CN) constrain its performance in photocatalytic water splitting and environmental remediation. Herein, the thermal vapor‐assisted π‐conjugation modification of CN by grafting with p‐aminophenoxy groups was developed to tune the photophysical properties of CN to enhance its photocatalytic activity. Besides extending the light absorption, the surface modification constructed a nanojunction across the depth direction, which leads to facilitated charge separation and transfer. In addition, the thermal vapor modification process thermally etches and trims the pristine CN to be highly holey structure, resulting to >10 times increase in specific surface area. Photocatalysis results showed that the obtained modified CN yielded hydrogen from photocatalytic water splitting at a rate of 7.82 mmol/g/h, over 7‐folds as that of pristine CN, with quantum yield of 3.28% at 400 nm. The π‐conjugation modified CN also demonstrated enhanced photocatalytic environmental remediation application, exemplified by much faster photodegradation of tetracycline hydrochloride. This work provides the thermal vapor surface chemical modification of CN as a promising integrated pathway of multiple favorable photophysical properties towards efficient photocatalysis application.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"9 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142253437","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

Avoiding Replicates in Biocatalysis Experiments: Machine Learning for Enzyme Cascade Optimization 避免生物催化实验中的重复：用于酶级联优化的机器学习

IF 4.5 3区化学

ChemCatChem Pub Date : 2024-09-16 DOI: 10.1002/cctc.202400777

Regine Siedentop, Maximilian Siska, Johanna Hermes, Stephan Lütz, Eric von Lieres, Katrin Rosenthal

{"title":"Avoiding Replicates in Biocatalysis Experiments: Machine Learning for Enzyme Cascade Optimization","authors":"Regine Siedentop, Maximilian Siska, Johanna Hermes, Stephan Lütz, Eric von Lieres, Katrin Rosenthal","doi":"10.1002/cctc.202400777","DOIUrl":"https://doi.org/10.1002/cctc.202400777","url":null,"abstract":"The optimization of enzyme cascades is a complex and resource-demanding task due to the multitude of parameters and synergistic effects involved. Machine learning can support the identification of optimal reaction conditions, for example, in the case of Bayesian optimization (BO), by proposing new experiments based on Gaussian process regression (GPR) and expected improvement (EI). Here, we used BO to optimize the concentrations of the reaction components of an enzyme cascade. The productivity-cost-ratio was chosen as the optimization objective in order to achieve the highest possible productivity, which was normalized to the costs of the materials used to prevent convergence to ever-increasing enzyme concentrations. To reduce the experimental effort, contrary to common practice in biological experiments, we did not use replicates but instead relied on the algorithm’s proposed experiments and inherent uncertainty quantification. This approach balances parameter space exploration and exploitation, which is critical for the efficient and effective identification of optimal reaction conditions. At the optimized reaction conditions identified in our study, the productivity-cost ratio was doubled to 38.6 mmol L-1 h-1 €-1 compared to a reference experiment. The parameter optimization required only 52 experiments while being robust to outlying experimental results.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"12 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142253386","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

On the Heterogeneity of Iron-Oxo Species in Zeolites for the Oxidation of Methane to Methanol by Nitrous Oxide: A Theoretical Perspective 氧化亚氮将甲烷氧化成甲醇的沸石中铁-氧化物的异质性：理论视角

IF 4.5 3区化学

ChemCatChem Pub Date : 2024-09-16 DOI: 10.1002/cctc.202401416

Shuo Wang, Chenchen Li, Chong Liu, Wei Zhuang

{"title":"On the Heterogeneity of Iron-Oxo Species in Zeolites for the Oxidation of Methane to Methanol by Nitrous Oxide: A Theoretical Perspective","authors":"Shuo Wang, Chenchen Li, Chong Liu, Wei Zhuang","doi":"10.1002/cctc.202401416","DOIUrl":"https://doi.org/10.1002/cctc.202401416","url":null,"abstract":"The conversion of methane to methanol (MTM) represents a pivotal objective in the C1 chemical industry. Transition metal, such as iron, exchanged zeolites are one category of the most active catalysts for direct conversion of MTM. One important topic in understanding the mechanism of Fe-zeolite catalyzed MTM is how the heterogeneity of catalytic (Fe) sites influences the system stability and reactivity. Employing DFT calculations and machine learning method, we herein studied the stability-reactivity relationship of a MTM catalytic cycle with N2O as the oxidant over Fe-exchanged zeolites. The Fe heterogeneity was introduced by using CHA and FER zeolites and looking at a number of related Fe species (FeII, FeO, and FeOH). A strong correlation was observed between the stability of such Fe species, which is primarily determined by the formation energy of FeII, and such a stability trend remains consistent throughout the MTM catalytic cycle. The reactivity analysis then demonstrated that less stable Fe species can exhibit higher reactivity when situated in specific sites. Further machine learning analysis validated the significant relevance of activation barriers with reaction energies in N2O decomposition step that is not sufficiently captured by the traditional one-dimensional Brønsted–Evans–Polanyi (BEP) relationship.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"66 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142253387","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

Titanium Silicate-1 Coupled with Sn and Er as Effective Catalysts for the Production of Lactic Acid from Saccharides 硅酸钛-1 与 Sn 和 Er 作为从蔗糖生产乳酸的有效催化剂

IF 4.5 3区化学

ChemCatChem Pub Date : 2024-09-15 DOI: 10.1002/cctc.202401303

Wenyu Zhang, Jingying Qin, Shengqi Liao, Guiying Li, Jianmei Li, Changwei Hu

{"title":"Titanium Silicate-1 Coupled with Sn and Er as Effective Catalysts for the Production of Lactic Acid from Saccharides","authors":"Wenyu Zhang, Jingying Qin, Shengqi Liao, Guiying Li, Jianmei Li, Changwei Hu","doi":"10.1002/cctc.202401303","DOIUrl":"https://doi.org/10.1002/cctc.202401303","url":null,"abstract":"Biomass-based saccharide valorization to produce lactic acid (LaA) via chemocatalysis has emerged as a promising approach to meet the substantial demand of global LaA market, whereas the manufacture of prominent heterogeneous catalyst is still challenging. Herein, we fabricate a series of heterogeneous rare earth catalysts, and indicate that Er supported onto titanium silicate-1 (TS-1) exhibits better activity than other rare earth catalysts for glucose transformation towards LaA. Remarkably, coupling Sn with Er onto TS-1 enabled the sharp increment of LaA yield, and 3Sn15Er/TS-1 catalyst outperformed other heterogeneous rare earth catalysts as reported to date, giving as high as 82.2 % and 76.2% yields of LaA from sorbose and glucose, respectively. The catalyst characterization demonstrated the coexistence of Er2O3 and Sn2Er2O7 on 3Sn15Er/TS-1 catalyst, both of which contributed to LaA production. Sn doping favored the formation of active particles in smaller size and increased the Lewis acidic sites when compared to single 15Er/TS-1, thereby promoting the isomerization and retro-aldol reaction of glucose to C3 intermediates. 3Sn15Er/TS-1 catalyst also showed universal activity for diverse biomass-based saccharides. This work might give useful insights to explore heterogeneous rare earth catalysts with superior activity in biomass valorization.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"15 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142253388","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

Research Progress of Catalysts with Atomic-Scale Reactive Sites in Urea Electrosynthesis 尿素电合成中具有原子级反应位点的催化剂的研究进展

IF 4.5 3区化学

ChemCatChem Pub Date : 2024-09-15 DOI: 10.1002/cctc.202401130

Lu Lu, Peng Zhan, Xuehan Chen, Wei Shi, Zhihao Si, Peiyong Qin

{"title":"Research Progress of Catalysts with Atomic-Scale Reactive Sites in Urea Electrosynthesis","authors":"Lu Lu, Peng Zhan, Xuehan Chen, Wei Shi, Zhihao Si, Peiyong Qin","doi":"10.1002/cctc.202401130","DOIUrl":"https://doi.org/10.1002/cctc.202401130","url":null,"abstract":"Urea (CO(NH2)2) is the main component of nitrogen-based fertilizers and is widely used in various industries. Until now, urea production is conducted under high-temperature and high-pressure conditions, which involves a considerable carbon footprint. Urea electrosynthesis, which is powered by renewable-energy-derived electricity, has emerged as a sustainable single-step process for urea production. The development of efficient and stable catalysts is the key to improving the efficiency of urea electrosynthesis. In this review, we summarized the research progress and applications of catalysts with atomic-scale reactive sites in urea electrosynthesis. Firstly, the catalytic mechanisms of urea electrosynthesis from CO2 and various nitrogenous molecules are discussed. Then, typical electrocatalysts such as single atom electrocatalysts, dual atom electrocatalysts, clusters, atomic dopants, and vacancies, etc., are discussed. Furthermore, characterization methods for atomic-scale reactive sites are summarized. Finally, challenges and suggestions for urea electrosynthesis are proposed. We hope this review can provide some inspiration toward the development of catalysts for efficient and sustainable urea electrosynthesis.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"2 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142253390","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

Bimetallic Copper Complexes for Electrocatalytic Bidirectional O2/H2O Conversion in Aqueous Solution 用于水溶液中电催化 O2/H2O 双向转化的双金属铜配合物

IF 4.5 3区化学

ChemCatChem Pub Date : 2024-09-15 DOI: 10.1002/cctc.202401228

Afsar Ali, Divyansh Prakash, Abhishek Saini, Chandan Das, Naseer Ahmed Shah, Arnab Dutta

{"title":"Bimetallic Copper Complexes for Electrocatalytic Bidirectional O2/H2O Conversion in Aqueous Solution","authors":"Afsar Ali, Divyansh Prakash, Abhishek Saini, Chandan Das, Naseer Ahmed Shah, Arnab Dutta","doi":"10.1002/cctc.202401228","DOIUrl":"https://doi.org/10.1002/cctc.202401228","url":null,"abstract":"The distinctive interplay between abundant transition metal-containing active sites and their surrounding outer coordination sphere (OCS) is pivotal in achieving remarkable catalytic responses. In this context, copper complexes continue to garner attention as promising catalysts for the Oxygen Reduction Reaction (ORR) and Oxygen Evolution Reaction (OER). In this article, we report two macrocyclic binuclear Cu complexes having variable peripheral functionalities around a common N2O2 like core. A mononuclear complex bearing the salophen-type ligand design was used as a control. The complex featuring peripheral OH groups, demonstrates highest catalytic activity in ORR (3050 s-1) and OER (6700 s-1), suggesting the crucial role of the alcoholic group during catalysis. In contrast, the mononuclear complex necessitates an additional thermodynamic stimulus to attain catalytic conditions for ORR and OER obverse to the case of binuclear complexes. Hence, this study establishes a template for designing molecular catalysts to mediate energy-relevant multielectron/multiproton reactions in both oxidizing and reducing environments.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"19 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142253391","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

Coupling of the catalytic reactions from formate dehydrogenase and hydrogenase in solution: Insights from computations and in situ IR spectroscopy 溶液中甲酸脱氢酶和氢化酶催化反应的耦合：计算和原位红外光谱的启示

IF 4.5 3区化学

ChemCatChem Pub Date : 2024-09-14 DOI: 10.1002/cctc.202400794

Armel F.T. Waffo, Meritxell Wu Lu, Sagie Katz, Stefan Frielingsdorf, Benjamin R Duffus, Jan Liedtke, Silke Leimkühler, Oliver Lenz, Konstantin Laun, Maria Andrea Mroginski, Ingo Zebger

{"title":"Coupling of the catalytic reactions from formate dehydrogenase and hydrogenase in solution: Insights from computations and in situ IR spectroscopy","authors":"Armel F.T. Waffo, Meritxell Wu Lu, Sagie Katz, Stefan Frielingsdorf, Benjamin R Duffus, Jan Liedtke, Silke Leimkühler, Oliver Lenz, Konstantin Laun, Maria Andrea Mroginski, Ingo Zebger","doi":"10.1002/cctc.202400794","DOIUrl":"https://doi.org/10.1002/cctc.202400794","url":null,"abstract":"Sophisticated enzymatic systems have evolved in nature to efficiently couple distinct biochemical reactions in form of cascades. As such they serve as reference models to understand the indirect interactions of catalytic centers. Herein, we studied, in solution, the coupling of the reactions from membrane‐bound [NiFe] hydrogenase (MBH) from Cupriavidus necator (reversible H2 splitting into H+ and e‐) and the molybdenum‐dependent formate dehydrogenase from Rhodobacter capsulatus (reversible formate to CO2 interconversion). To follow their interplay via the characteristic absorptions from the MBH's active site or the respective substrate and product bands of FDH, we utilized in situ IR spectrocopy and GC(‐MS), in the absence or presence of soluble redox mediators. Coarse grained molecular dynamics (cgMD) computations revealed the lack of productive enzyme complexes for direct electron transfer (ET). Thus, the observed minor amounts of H2 or formate were produced from transient interactions between the two enzymes. On the contrary, the significantly increased product formation in the presence of methylene viologen can be related to the putative multiple interaction sites of the redox mediator with FDH identified by cgMD. Our study represents a proof‐of‐concept approach that can be used in future to develop novel coupled biocatalytic systems by identifying potential ET pathways.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"100 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142253395","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

Metal organic frameworks‐derived NiO/NiCo2O4 heterostructures for effective methanol oxidation reaction 金属有机框架衍生的 NiO/NiCo2O4 异质结构用于有效的甲醇氧化反应

IF 4.5 3区化学

ChemCatChem Pub Date : 2024-09-14 DOI: 10.1002/cctc.202401277

Yuan Xin, Jieyu Ma, Qian Zhang, Zhizhou Wang, Li Jiang, Haidong Bian, Qianli Zhang, Jie Liu

{"title":"Metal organic frameworks‐derived NiO/NiCo2O4 heterostructures for effective methanol oxidation reaction","authors":"Yuan Xin, Jieyu Ma, Qian Zhang, Zhizhou Wang, Li Jiang, Haidong Bian, Qianli Zhang, Jie Liu","doi":"10.1002/cctc.202401277","DOIUrl":"https://doi.org/10.1002/cctc.202401277","url":null,"abstract":"The electrochemical process of methanol oxidation reaction (MOR), which is closely associated with electrochemical production of formate and hydrogen, is considered a highly viable avenue for advancing renewable energy technologies. Nevertheless, the development and creation of affordable, effective, and durable electrocatalysts for MOR continue to present significant obstacles. In this study, a hierarchical porous NiO/NiCo2O4/NF electrode is fabricated through the integration of solvothermal and thermal oxidation treatments of Ni‐MOF‐74 and NiCo‐Asp. After thoroughly assessing the electrochemical performance for MOR, NiO/NiCo2O4/NF demonstrates a significant current density of 140 mA·cm‐2 at 1.6 V (vs. RHE) and a Tafel slop of 45.0 mV·dec‐1 in 1 M KOH and 0.5 M methanol. The excellent performance of MOR can be ascribed to the hierarchical porous nature that enhances mass and electron transport while offering numerous active sites for electrocatalytic reactions. Additionally, the heterointerface between NiO and NiCo2O4 could further enhance electron transfer rate and reaction kinetics for the MOR. The developed NiO/NiCo2O4/NF electrode shows potential as a viable and economical alternative to Pt‐based electrocatalysts for MOR‐based applications.","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"66 1","pages":""},"PeriodicalIF":4.5,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142253502","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

Circular Polyesters Based on Lactones 基于内酯的环状聚酯

IF 4.5 3区化学

ChemCatChem Pub Date : 2024-09-13 DOI: 10.1002/cctc.202401319

Tie-Qi Xu, Run-Hua Dong, Jia-Yin Guo, Hang-Ming Sun

引用次数: 0