Chem Catalysis最新文献_第5页

Ketones as ideal photocatalysts for decarboxylative fluorination and a competition with C(sp3)-H fluorination 酮类作为理想的光催化剂用于脱羧氟化以及与 C（sp3）-H 氟化的竞争

IF 9.4

Chem Catalysis Pub Date : 2024-10-24 DOI: 10.1016/j.checat.2024.101162

Yu Zhang, Jiahui Qian, Miao Wang, Yahao Huang, Hansjörg Grützmacher, Peng Hu

引用次数: 0

Photoreduction of CO2 to complete CO catalyzed by charge-density-regulating metal-organic frameworks 在电荷密度调节金属有机框架催化下将 CO2 光还原为完全 CO

IF 9.4

Chem Catalysis Pub Date : 2024-10-24 DOI: 10.1016/j.checat.2024.101154

Luyao Wang, Yifan Gu, Fengting Li

{"title":"Photoreduction of CO2 to complete CO catalyzed by charge-density-regulating metal-organic frameworks","authors":"Luyao Wang, Yifan Gu, Fengting Li","doi":"10.1016/j.checat.2024.101154","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101154","url":null,"abstract":"Photoreduction of CO2 to a single gas product requires catalysts with remarkable product selectivity because CO and CH4 are usually produced simultaneously. We propose that the charge-density regulation within metal-organic frameworks (MOFs) could effectively manage the binding energy required for reduction intermediates, thereby controlling the ultimate product formation to obtain CO with 100% selectivity. Herein, two iso-structured Fe-based MOFs bearing linkers with different electronic properties were prepared and exhibited favorable CO2 photoreduction performance without any cocatalyst or photosensitizer. In particular, the linker was altered to reduce the transfer of charges from Fe to the surrounding ligands, regulating the charge-density distribution. The binding affinity with the key COH∗ was remarkably weakened and behaved thermodynamically unfavorably compared with CO desorption, resulting in 100% CO generation. These insights provide a catalyst design strategy for controlling reduction species and improving product selectivity, which could encourage the development of intriguing MOF material customization for photocatalysis.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"1 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142489082","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Fine-tuning catalytic selectivity by modulating catalyst-environment interactions: CO2 hydrogenation over Pd-based catalysts 通过调节催化剂与环境的相互作用微调催化选择性：钯基催化剂的二氧化碳加氢反应

IF 9.4

Chem Catalysis Pub Date : 2024-10-22 DOI: 10.1016/j.checat.2024.101156

Hong Zhang, Ping Liu

{"title":"Fine-tuning catalytic selectivity by modulating catalyst-environment interactions: CO2 hydrogenation over Pd-based catalysts","authors":"Hong Zhang, Ping Liu","doi":"10.1016/j.checat.2024.101156","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101156","url":null,"abstract":"Capturing catalytic behaviors under operational conditions is pivotal to gaining a mechanistic understanding and promoting the design of robust catalysts. The challenge lies in the difficulty of monitoring real-time surface dynamics driven by catalyst-environment interactions. Here, we introduce a framework based on density functional calculations and kinetic modeling. This framework significantly improves the accuracy of theoretical models’ descriptions of experimental observations by quantifying environmental impacts on surface phases and active sites. CO2 hydrogenation over Pd-based catalysts is taken as a showcase. The observed selectivity variations of Pd and Pd-M bimetallic catalysts strongly correlate with hydrogen coverage maintained under typical CO2 hydrogenation conditions. By reducing the amount of surface hydrogen, the selectivity tuned effectively from formic acid toward CO and methanol. This study not only deepens the comprehension of dynamics of active sites under active chemical conditions but also introduces an alternative opportunity for catalytic tuning by modulating catalyst-environment interactions.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"75 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486571","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Electrochemical CO2 fixation with amines to synthesize α-amino acids 用胺进行电化学二氧化碳固定以合成α-氨基酸

IF 9.4

Chem Catalysis Pub Date : 2024-10-22 DOI: 10.1016/j.checat.2024.101158

Yimeng Cao, Jun Chen, Chunmei Ding, Ying Zhang, Haibo Chi, Yan Liu, Can Li

引用次数: 0

Transformative ligand effects in Fe-photocatalyzed Giese-type additions 铁光催化盖斯型加成中的配体转换效应

IF 9.4

Chem Catalysis Pub Date : 2024-10-22 DOI: 10.1016/j.checat.2024.101131

Michael S. Crocker, Jung-Ying Lin, Reem Nsouli, Nathan D. McLaughlin, Djamaladdin G. Musaev, Aliyeh Mehranfar, Ernesto R. Lopez, Laura K.G. Ackerman-Biegasiewicz

{"title":"Transformative ligand effects in Fe-photocatalyzed Giese-type additions","authors":"Michael S. Crocker, Jung-Ying Lin, Reem Nsouli, Nathan D. McLaughlin, Djamaladdin G. Musaev, Aliyeh Mehranfar, Ernesto R. Lopez, Laura K.G. Ackerman-Biegasiewicz","doi":"10.1016/j.checat.2024.101131","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101131","url":null,"abstract":"Visible-light-promoted Fe photocatalysis is a sustainable strategy for synthetic chemistry. Yet, the adoption of Fe photocatalytic reactions proceeding through a ligand-to-metal charge transfer event has been limited to simple substrates in many transformations. An outstanding challenge in the field is the selection of tunable ligand scaffolds providing general reactivity. In this work, we describe the use of aliphatic amines as ligands in Fe-promoted decarboxylative Giese-type additions. Unlike prior photoredox reports, this method enables the coupling of substrates with free amines, alcohols, and a boronic ester. To gain insight into the role of diethylenetriamine (L1), ligated Fe salts were investigated using ultraviolet-visible spectroscopy, thermal gravimetric analysis, and density functional theory. These studies support the formation of a photoactive octahedral carboxylate (L1)Fe(OCOR)3. As an increasing number of photocatalytic reactions proceed using earth-abundant metals, the use of these ligands expands the possibility of applying Fe to a broad array of transformations.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"85 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486559","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Copper-catalyzed 1,4-aminohydroxylation and aminothiolation of 1,3-dienes by carbonyl-assisted migration 铜催化 1,3-二烯的 1,4-氨基羟化反应和羰基辅助迁移的氨基硫代反应

IF 9.4

Chem Catalysis Pub Date : 2024-10-21 DOI: 10.1016/j.checat.2024.101147

Noah H. Watkins, Yungeun Kwon, Qiu Wang

引用次数: 0

Modulator engineering of bifunctional metal-organic framework for synergistic catalysis 用于协同催化的双功能金属有机框架调制器工程

IF 9.4

Chem Catalysis Pub Date : 2024-10-21 DOI: 10.1016/j.checat.2024.101155

Jing Ouyang, Hongyi Tao, Zhiyi Yang, Yim Kwan Wong, Wei Shen Aik, Herman Ho-Yung Sung, Ian Williams, Yangjian Quan

{"title":"Modulator engineering of bifunctional metal-organic framework for synergistic catalysis","authors":"Jing Ouyang, Hongyi Tao, Zhiyi Yang, Yim Kwan Wong, Wei Shen Aik, Herman Ho-Yung Sung, Ian Williams, Yangjian Quan","doi":"10.1016/j.checat.2024.101155","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101155","url":null,"abstract":"Pursuing both structural uniformity/crystallinity and functional complexity is a long-term goal in functional materials engineering. Often, efforts to enhance one attribute may compromise the other. Herein, we report an elaborate strategy of integrating a catalytic center into a modulator, which enables the one-pot synthesis of a bifunctional metal-organic framework (MOF), Zr-TBAPy-TSA (TBAPy = 1,3,6,8-tetrakis(p-benzoic acid)pyrene; TSA = o-thiosalicylic acid). TSA serves as both a modulator for metal-organic framework (MOF) preparation and a catalytic center. Zr-TBAPy-TSA is distinguished by its highly uniform and crystalline structure, as evidenced by detailed characterizations including single-crystal X-ray diffraction. Additionally, Zr-TBAPy-TSA incorporating both photosensitizer and thiol active centers showcases superior catalytic performance in the activation of element–H bonds (elements include C, B, Si, and P). Due to its less defective structure, extra high turnover numbers of up to 14,200 and good catalyst recyclability are obtained.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"12 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452301","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Electron-acceptor-controlled polyimides for photoredox-neutral trifluoromethylation 用于光氧化中性三氟甲基化反应的电子受体控制聚酰亚胺

IF 9.4

Chem Catalysis Pub Date : 2024-10-17 DOI: 10.1016/j.checat.2024.101151

Lin Zuo, Gonghong Qiu, Yan Liu, Xiaolan Chen, Kai Sun, Igor B. Krylov, Lingbo Qu, Alexander O. Terent’ev, Bing Yu

{"title":"Electron-acceptor-controlled polyimides for photoredox-neutral trifluoromethylation","authors":"Lin Zuo, Gonghong Qiu, Yan Liu, Xiaolan Chen, Kai Sun, Igor B. Krylov, Lingbo Qu, Alexander O. Terent’ev, Bing Yu","doi":"10.1016/j.checat.2024.101151","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101151","url":null,"abstract":"Heterogeneous photocatalysts present notable benefits over homogeneous systems. However, their application is often hindered by spontaneous electron-hole recombination, undermining photoconversion efficiency. Addressing this, our study introduces a diversity-oriented synthesis of electron-donor-acceptor (D-A)-type polyimides via N-amidation of aromatic dianhydrides with anilines. These polyimides exhibit segregated D-A alignments that facilitate enhanced charge separation, rapid electron transfer, and long-lived photogenerated electron-hole pairs, attributed to superior electron-donating and -accepting capabilities alongside predictable π-π stacking. Their efficacy is demonstrated in catalyzing visible-light-driven redox-neutral C–H trifluoromethylation, transforming pharmaceuticals and bioactive molecules into trifluoromethyl-functionalized products with high yield and selectivity. A continuous-flow fixed-bed photoreactor supports gram-scale synthesis, and the photocatalyst maintains activity through at least four recycling rounds. Time-dependent density functional theory (TD-DFT) and non-covalent interaction (NCI) analyses suggest that the observed performance enhancement is due to controlled photoinduced electron transfer within the D-A system and intrachain π-π stacking.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"231 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444437","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

NHC-catalyzed remote site-selective arene C–H acylations NHC 催化的远程位点选择性炔烃 C-H 丙烯酸化反应

IF 9.4

Chem Catalysis Pub Date : 2024-10-17 DOI: 10.1016/j.checat.2024.101125

Jiamiao Jin, Shi-Chao Ren

引用次数: 0

A new functional surfactant enables direct C−H arylation in water under mild conditions 一种新型功能表面活性剂可在温和条件下实现水中直接 C-H 芳基化

IF 9.4

Chem Catalysis Pub Date : 2024-10-17 DOI: 10.1016/j.checat.2024.101161

Francesca Pallini, Luca Beverina

引用次数: 0