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Anion-coordination- and π-π-stacking-interaction-driven assembly of a complex Frank-Kasper structure 阴离子配位和π-π堆积相互作用驱动的复杂弗兰克-卡斯帕结构组装
IF 23.5 1区 化学
Chem Pub Date : 2024-12-17 DOI: 10.1016/j.chempr.2024.11.009
Zhu Zhuo, Zi-Ang Nan, Wen-Zheng Fu, Wei Wang, Guo-Ling Li, Ming-Yan Wu, Maochun Hong, You-Gui Huang
{"title":"Anion-coordination- and π-π-stacking-interaction-driven assembly of a complex Frank-Kasper structure","authors":"Zhu Zhuo, Zi-Ang Nan, Wen-Zheng Fu, Wei Wang, Guo-Ling Li, Ming-Yan Wu, Maochun Hong, You-Gui Huang","doi":"10.1016/j.chempr.2024.11.009","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.11.009","url":null,"abstract":"Constructing artificial sophisticated architectures from simple small-molecular subunits by cooperative interactions remains one of the most formidable challenges. Herein, we report a complex supramolecular structure, {{[CoL(SCN)]<sub>20</sub>}{[CoL(SCN)]<sub>24</sub>}<sub>3</sub>(SO<sub>4</sub>)<sub>23</sub>(HSO<sub>4</sub>)<sub>46</sub>}·246(CH<sub>3</sub>CN) (<strong>1</strong>), that arises from the assembly of [CoL(SCN)]<sup>+</sup> with SO<sub>4</sub><sup>2−</sup> and HSO<sub>4</sub><sup>−</sup> (L = tris(2-benzimidazolylmethyl)amine) under solvothermal condition. The crystallization of compound <strong>1</strong> is driven by the cooperation of the <em>π-π</em> stacking interactions between [CoL(SCN)]<sup>+</sup> cations and the hydrogen bonds between [CoL(SCN)]<sup>+</sup> and SO<sub>4</sub><sup>2−</sup> and HSO<sub>4</sub><sup>−</sup>. [CoL(SCN)]<sup>+</sup> cations self-associate through intermolecular <em>π-π</em> stacking interactions to create two <em>π</em>-stacked polyhedral 5<sup>12</sup>-{[CoL(SCN)]<sub>20</sub>} dodecahedra and 5<sup>12</sup>6<sup>2</sup>-{[CoL(SCN)]<sub>24</sub>} tetrakaidekahedra. These two <em>π</em>-stacked polyhedral subunits coexist in the same lattice in a 1:3 ratio and coordinate with SO<sub>4</sub><sup>2−</sup> and HSO<sub>4</sub><sup>−</sup>, resulting in a complex Frank-Kasper (FK) A15 structure. This research demonstrates that small-molecular scaffolds can assemble into sophisticated architectures and creates exciting perspectives for constructing sophisticated clathrate structures from simple small molecules.","PeriodicalId":268,"journal":{"name":"Chem","volume":"30 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832715","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Hydrogen-bond catalysis in biomass valorization
IF 23.5 1区 化学
Chem Pub Date : 2024-12-16 DOI: 10.1016/j.chempr.2024.11.002
Yingchuan Zhang, George W. Huber, Zhengxiao Guo
{"title":"Hydrogen-bond catalysis in biomass valorization","authors":"Yingchuan Zhang, George W. Huber, Zhengxiao Guo","doi":"10.1016/j.chempr.2024.11.002","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.11.002","url":null,"abstract":"As a biomimetic concept of enzymatic catalysis, hydrogen-bond catalysis (HBC) leverages H-bond-inducing atomic sites or functional groups in catalysts to regulate substrate binding and transition states so as to enable highly efficient and (stereo)selective organic reactions. However, it has rarely been employed in catalytic biomass valorization toward renewable fuels and value-added chemicals until recently. This perspective aims to highlight the opportunities offered by HBC to promote effective transformations of biomass-derived oxygenates. The concept and characterization approaches of HBC strategies are first introduced, followed by a critical overview of HBC-involved reactions, catalyst structures, and dynamic interfaces between biomass substrates and catalysts. Particular attention is paid to binding configurations and adsorption energetics for which engineered H-bonds can tune bond cleavage/formation and promote desirable reaction pathways in association with intrinsic catalytic sites (e.g., Lewis/Brønsted acid sites, metal active sites, and photogenerated charges) and therefore enable biomass valorization in more efficient and sustainable manners.","PeriodicalId":268,"journal":{"name":"Chem","volume":"106 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825653","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Switchable diversification of quaternary ammonium salts using photocatalysis
IF 23.5 1区 化学
Chem Pub Date : 2024-12-13 DOI: 10.1016/j.chempr.2024.11.004
Takumi Kinoshita, Yota Sakakibara, Tomoko Hirano, Kei Murakami
{"title":"Switchable diversification of quaternary ammonium salts using photocatalysis","authors":"Takumi Kinoshita, Yota Sakakibara, Tomoko Hirano, Kei Murakami","doi":"10.1016/j.chempr.2024.11.004","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.11.004","url":null,"abstract":"Over the past few decades, significant advances have been made in the radical chemistry of amine molecules. However, the radical reactions of related quaternary ammonium salts remain comparatively underexplored. If radicals could be generated from ammonium salts in a controlled manner, this could lead to a method for producing distonic radical cations, offering valuable synthetic applications for quaternary ammonium salts and their tertiary amine derivatives. In this study, we developed a photoredox-catalyzed method for derivatizing quaternary ammonium salts by reacting α-haloalkylammonium salts with olefins. The key to success is the photocatalytic generation of distonic α-ammonio radicals under both oxidative and reductive quenching conditions. This chemistry enables selective and switchable alkylations and alkenylations, affording structurally new quaternary ammonium salts. The utility of this procedure is showcased in the divergent synthesis and derivatization of bioactive quaternary ammonium salts, a deuterated tertiary amine, and the identification of salinity-tolerance-conferring molecules.","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816436","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Quantity effect of heteroatom incorporation on the oxygen evolution mechanism in ruthenium oxide
IF 23.5 1区 化学
Chem Pub Date : 2024-12-13 DOI: 10.1016/j.chempr.2024.11.005
Hyunwoo Jun, Eunseo Kang, Jinuk Moon, Hoyoung Kim, Sunghoon Han, Seokhyun Choung, Seongbeen Kim, Seung Yeop Yi, Eunae Kang, Chang Hyuck Choi, Jeong Woo Han, Jinwoo Lee
{"title":"Quantity effect of heteroatom incorporation on the oxygen evolution mechanism in ruthenium oxide","authors":"Hyunwoo Jun, Eunseo Kang, Jinuk Moon, Hoyoung Kim, Sunghoon Han, Seokhyun Choung, Seongbeen Kim, Seung Yeop Yi, Eunae Kang, Chang Hyuck Choi, Jeong Woo Han, Jinwoo Lee","doi":"10.1016/j.chempr.2024.11.005","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.11.005","url":null,"abstract":"Research on ruthenium oxide (RuO<sub>2</sub>) catalysts as alternatives to Ir-based catalysts for the acidic oxygen evolution reaction (OER) has focused on enhancing activity and stability by incorporating heteroatoms. However, the relationship between the amount of incorporated heteroatom and the OER mechanism remains unclear. Herein, we synthesized rutile manganese-ruthenium solid-solution oxides (Mn<sub>x</sub>Ru<sub>1-x</sub>O<sub>2</sub>) with varying Mn/Ru ratios to identify factors affecting activity and stability with Mn content. Both experimental and computational results show that increasing Mn content raises the oxidation state of Ru and shifts the OER mechanism from the adsorbate evolution mechanism (AEM) to the lattice oxygen mechanism (LOM). Increased Mn concentration enhances Ru–O bond covalency, leading to lattice oxygen involvement in the OER. The Mn<sub>0.2</sub>Ru<sub>0.8</sub>O<sub>2</sub> catalyst, with an optimal Mn/Ru ratio, operated stably in a proton exchange membrane water electrolyzer (PEMWE) for 100 h and achieved 3.15 A cm<sup>−2</sup> at 1.8 V<sub>cell</sub>, surpassing the 2026 Department of Energy activity goal.","PeriodicalId":268,"journal":{"name":"Chem","volume":"29 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816437","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Controlled carbon nanotube growth with hydrocarbon nanobelt templates
IF 23.5 1区 化学
Chem Pub Date : 2024-12-12 DOI: 10.1016/j.chempr.2024.11.011
Shengnan Gao, Andrew C.-H. Sue
{"title":"Controlled carbon nanotube growth with hydrocarbon nanobelt templates","authors":"Shengnan Gao, Andrew C.-H. Sue","doi":"10.1016/j.chempr.2024.11.011","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.11.011","url":null,"abstract":"The attainment of structurally uniform single-walled carbon nanotubes (SWCNTs) remains a significant challenge in carbon materials science. Recently in <em>Journal of the American Chemical Society</em>, Huang, Guo, Hu, and co-workers reported the synthesis of a series of [2<em>n</em>]collarene macrocycles and demonstrated their utility as rigid templates for the controlled growth of SWCNTs with predefined diameters via a chemical vapor deposition method.","PeriodicalId":268,"journal":{"name":"Chem","volume":"4 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142809956","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Reshaping quinolines by single-electron-transfer-triggered dearomatization
IF 23.5 1区 化学
Chem Pub Date : 2024-12-12 DOI: 10.1016/j.chempr.2024.11.007
Yun-Peng Chu, Jiajia Ma
{"title":"Reshaping quinolines by single-electron-transfer-triggered dearomatization","authors":"Yun-Peng Chu, Jiajia Ma","doi":"10.1016/j.chempr.2024.11.007","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.11.007","url":null,"abstract":"In this issue of <em>Chem</em>, Prof. Shunsuke Chiba, Prof. Derek Pratt, and their colleagues report a groundbreaking study on the dearomative dimerization and skeletal rearrangement of quinolines under polysulfide anion photocatalysis. This work demonstrates a unique method for transforming quinolines into complex sp<sup>3</sup>-rich polyheterocycles and 4-(3-indolylmethyl)quinolines through a sequence of reactions initiated by single-electron transfer (SET).","PeriodicalId":268,"journal":{"name":"Chem","volume":"20 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142809955","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Transformative ligand effects in iron photocatalysis
IF 23.5 1区 化学
Chem Pub Date : 2024-12-12 DOI: 10.1016/j.chempr.2024.11.008
Luisa Zach, Jola Pospech
{"title":"Transformative ligand effects in iron photocatalysis","authors":"Luisa Zach, Jola Pospech","doi":"10.1016/j.chempr.2024.11.008","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.11.008","url":null,"abstract":"Iron photocatalysis has been constrained by a lack of tunable ligands for diverse substrate scopes. Ackerman-Biegasiewicz et al. demonstrate diethylenetriamine (DETA) as a transformative ligand in Fe-catalyzed Giese-type additions recently in <em>Chem Catalysis</em>. This platform enables effective coupling of substrates with free amines, alcohols, and boronic esters, highlighting iron’s potential as a sustainable alternative to precious metals in photoredox catalysis.","PeriodicalId":268,"journal":{"name":"Chem","volume":"1 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142810049","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Chemical education in digital chemistry
IF 23.5 1区 化学
Chem Pub Date : 2024-12-12 DOI: 10.1016/j.chempr.2024.10.010
Fun Man Fung, Magdalena Lederbauer, Yvonne S.L. Choo, Timo Gehring, Kevin Maik Jablonka, Kjell Jorner, Philippe Schwaller, Michael B. Sullivan, Andrea Volkamer, Matthew S. Sigman, Kuangbiao Liao, Charles Windle
{"title":"Chemical education in digital chemistry","authors":"Fun Man Fung, Magdalena Lederbauer, Yvonne S.L. Choo, Timo Gehring, Kevin Maik Jablonka, Kjell Jorner, Philippe Schwaller, Michael B. Sullivan, Andrea Volkamer, Matthew S. Sigman, Kuangbiao Liao, Charles Windle","doi":"10.1016/j.chempr.2024.10.010","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.010","url":null,"abstract":"In this digital age where machine learning has won the Nobel Prizes in both Physics and Chemistry, it is ever more important to give chemistry students an educational advantage that will enable them to use the tools of artificial intelligence and machine learning to enhance both their study experience and their future research. In this Voices article, chemistry education and research experts gather to share their implementation and utilization of these data-driven tools in classes and in labs.","PeriodicalId":268,"journal":{"name":"Chem","volume":"62 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142810048","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
BINOLates as potent reducing photocatalysts for inert bond activation and reduction of unsaturated systems 作为惰性键活化和还原不饱和体系的强效还原光催化剂的双乙醇酸盐
IF 23.5 1区 化学
Chem Pub Date : 2024-12-11 DOI: 10.1016/j.chempr.2024.10.026
Can Liu, Yan Zhang, Rui Shang
{"title":"BINOLates as potent reducing photocatalysts for inert bond activation and reduction of unsaturated systems","authors":"Can Liu, Yan Zhang, Rui Shang","doi":"10.1016/j.chempr.2024.10.026","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.10.026","url":null,"abstract":"Phenolates are increasingly studied as photocatalysts because of their abundance and easy accessibility. However, their potential as potent and broadly applicable reducing photoredox catalysts is hindered by the high electronegativity of oxygen and the reactivity of phenoxy radicals. Herein, we discovered that renowned 1,1′-Bi-2-naphtholate derivatives (BINOLates) are potent reducing photocatalysts. These catalysts are effective for the activation of inert bonds and the reduction of unsaturated bonds, including selective CF activation of activated –CF<sub>3</sub>,–CF<sub>2</sub>H, –C<sub>2</sub>F<sub>5</sub>, and aryl fluoride, activation of alkyl and aryl chlorides, detosylation, Birch reduction, and alkene reduction, demonstrating potent reducing ability and catalytic versatility. Defluoroalkylation using PhCF<sub>3</sub> as a limiting reagent, a challenging substrate for reported catalysts, proceeded smoothly. BINOLates were applicable as photoredox catalysts even under green light. This work introduces a new catalytic application for the renowned BINOLates, suggesting the potential for future expansion of their applications in the realm of photocatalysis.","PeriodicalId":268,"journal":{"name":"Chem","volume":"20 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805258","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Hybrid photoanodes based on surface-bound host-guest molecular assemblies
IF 23.5 1区 化学
Chem Pub Date : 2024-12-09 DOI: 10.1016/j.chempr.2024.11.003
Jiaxuan Wang, Daokuan Li, Xiaona Li, Guoquan Liu, Yong Zhu, Licheng Sun, Fei Li
{"title":"Hybrid photoanodes based on surface-bound host-guest molecular assemblies","authors":"Jiaxuan Wang, Daokuan Li, Xiaona Li, Guoquan Liu, Yong Zhu, Licheng Sun, Fei Li","doi":"10.1016/j.chempr.2024.11.003","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.11.003","url":null,"abstract":"In artificial photosynthesis, molecule/semiconductor hybrids combine the merits of the high activity of molecular catalysts and the high stability of semiconductor light absorbers. We report here a host-guest strategy for hybrid photoanode fabrication, where phosphonate-derivatized cyclodextrins (p-CDs) as hosts were anchored on the surface of a tungsten oxide (WO<sub>3</sub>) film, and molecular catalysts as guests were self-encapsulated into the cavities of p-CDs in either aqueous or organic media. By choosing an admantanyl cobaloxime complex (<strong>Co1</strong>) as a molecular water oxidation catalyst, the resulting WO<sub>3</sub>|p-CD|<strong>Co1</strong> photoanode exhibited high photoelectrochemical (PEC) activity and stability for water oxidation due to the unexpected efficient charge separation and the strong affinity between p-CD and catalyst. In addition, the WO<sub>3</sub>|p-CD was identified to be a versatile platform for catalyst loading, when a 4-hydroxy-2,2,6,6-tetramethylpiperidine 1-oxyl (TEMPO) derivative was employed as the guest molecule, the conversion yield of PEC alcohol oxidation to aldehyde was dramatically increased.","PeriodicalId":268,"journal":{"name":"Chem","volume":"35 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793789","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
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