Chemistry - A European Journal最新文献_第6页

Metal-organic Framework (MOF)-Based Sensors for Mercury (Hg) Detection: Design Strategies and Recent Progress. 基于金属有机框架 (MOF) 的汞 (Hg) 检测传感器：设计策略与最新进展。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2024-11-20 DOI: 10.1002/chem.202403760

Wei Ma, Qidu Zhang, Dongshan Xiang, Kang Mao, Jiaqi Xue, Zhuo Chen, Zhen Chen, Wei Du, Kun Zhai, Hua Zhang

{"title":"Metal-organic Framework (MOF)-Based Sensors for Mercury (Hg) Detection: Design Strategies and Recent Progress.","authors":"Wei Ma, Qidu Zhang, Dongshan Xiang, Kang Mao, Jiaqi Xue, Zhuo Chen, Zhen Chen, Wei Du, Kun Zhai, Hua Zhang","doi":"10.1002/chem.202403760","DOIUrl":"https://doi.org/10.1002/chem.202403760","url":null,"abstract":"Monitoring mercury (Hg) is critical for environmental and public health. Metal-organic framework (MOF)-based sensors demonstrate the advantage of high sensitivity and rapid response. We summarize the advances of MOF sensors for Hg2+ detection from the perspective of MOF type and role in the sensors. First, we introduce three MOFs used in Hg sensors-UIO, ZIF, and MIL-that have demonstrated superior performance. Then, we discuss the specifics of MOF-based sensors for Hg2+ detection in terms of the recognition and signal elements. Currently, the recognition elements include T-rich aptamers, noble metal nanoparticles, central metal ions, and organic functional groups inherent to MOFs. Sensors with fluorescence and colorimetric signals are the two main types of optical MOF sensors used for Hg detection. Electrochemical sensors have also been fabricated, but these are less frequently reported, potentially due to the limited conductivity and cycling stability of MOFs. Notably, dual-signal sensors mitigate background signals interference and enhance the accuracy of Hg2+ detection. Furthermore, to facilitate portability and user-friendliness, portable devices such as microfluidics, paper-based devices, and smartphones have been developed for Hg2+ detection, showcasing potential applications. We also address the challenges related to MOF-based sensors for Hg2+ and future outlook.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403760"},"PeriodicalIF":3.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142680290","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Basic-functionalized Ionic Porous Organic Polymers: Triple Roles in One for Highly Efficient and Recyclable Carboxylative Cyclization of CO2 under Mild Conditions. 碱性官能化离子多孔有机聚合物：在温和条件下实现 CO2 的高效、可循环羧基环化的三合一作用。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2024-11-20 DOI: 10.1002/chem.202403476

Han Tao, Weiqi Mao, Lili Jiang, Qiaoxin Xiao, Zhenyu Zhao, Kaili Wang, Zhaowei Zhang, Jiayi Bai, Haoran Li, Congmin Wang

{"title":"Basic-functionalized Ionic Porous Organic Polymers: Triple Roles in One for Highly Efficient and Recyclable Carboxylative Cyclization of CO2 under Mild Conditions.","authors":"Han Tao, Weiqi Mao, Lili Jiang, Qiaoxin Xiao, Zhenyu Zhao, Kaili Wang, Zhaowei Zhang, Jiayi Bai, Haoran Li, Congmin Wang","doi":"10.1002/chem.202403476","DOIUrl":"https://doi.org/10.1002/chem.202403476","url":null,"abstract":"The transformation of carbon dioxide (CO2) into high-value chemicals is a significant step towards achieving the goal of \"carbon neutrality\". α-methylene cyclic carbonate, as an intermediate for the synthesis of many important organic compounds, is widely employed in industrial productions. In this work, a series of ionic porous organic polymers (IPOPs) with different basic-functionalized anions were successfully synthesized and adjusted to have certain BET surface areas and high contents of ion sites by post-modification. These basic-functionalized IPOPs could exhibit excellent catalytic performance for carboxylative cyclization of CO2 at 30 oC and 1 bar in presence of silver salts, eliminating the use of extra organic bases. In the whole catalytic reaction, the basic-functionalized anions could play triple roles: enriching CO2 for further transformation, activating the hydroxyl groups of substrates to improve the catalytic performance, while coordinating with Ag atom to stabilize and regenerate catalyst. Notably, the catalytic system of DCX-4-Tet/Ag2O exhibited excellent recyclability, and the yield of α-alkylidene cyclic carbonate was well maintained at 99% after 5 cycles. To the best of our knowledge, the catalytic system was the first example of basic-functionalized IPOPs that played multiple roles for highly efficient CO2 cyclization under mild conditions without any extra organic bases.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403476"},"PeriodicalIF":3.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142674641","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Regulating Room-Temperature Phosphorescence of Organic Luminophores through Stepwise Stabilization by Coordination and In-Situ Precipitation Reaction. 通过配位和原位沉淀反应逐步稳定有机发光体，调节其室温磷光。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2024-11-20 DOI: 10.1002/chem.202403829

Chenglong Ji, Yuncai Gao, Yulu Wang, Ran Li, Yu-E Shi, Zhenguang Wang, Yongqing Zhai

引用次数: 0

Correlation Between NMR Coupling Constants and σ-Donating Properties of N-Heterocyclic Carbenes and Their Derivatives. NMR 耦合常数与 N-Heterocyclic Carbenes 及其衍生物的σ-捐献特性之间的相关性。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2024-11-20 DOI: 10.1002/chem.202403403

Gilles Frison, Radhika Gupta

{"title":"Correlation Between NMR Coupling Constants and σ-Donating Properties of N-Heterocyclic Carbenes and Their Derivatives.","authors":"Gilles Frison, Radhika Gupta","doi":"10.1002/chem.202403403","DOIUrl":"https://doi.org/10.1002/chem.202403403","url":null,"abstract":"Is the 1JC-H coupling constant for protonated carbene a relevant measure of its σ-donation ability? This paper addresses this question by comparing calculated 1JC-H values with various experimental and theoretical approaches across a broad spectrum of carbene compounds. We examined Arduengo-type NHCs based on the 2-imidazolylidene scaffold and many other derivatives with modified frameworks, including carbenes with extended, saturated, or conjugated rings, reduced heteroatom stabilization, alternative heteroatoms, permanently charged carbenes, acyclic carbenes, amidocarbenes, and cyclic amino(alkyl/aryl) carbenes, carbodicarbenes and carbodiphosphoranes. Our findings reveal a nuanced relationship between different parameters associated with σ-interaction, such as 1JC-H, Huynh electronic parameter (HEP), σ-donation from ETS-NOCV, and lone pair energy. Notably, the best correlation was observed between 1JC-H and the ETS-NOCV method, particularly for mono- and diaminocarbenes, highlighting the utility of 1JC-H in comparing σ-donation among structurally similar carbene types. However, the use of 1JC-H as a universal measure across all carbene classes appears limited, especially when considering carbenes with significantly different structural frameworks. While HEP is less effective for carbenes with diverse structural backbones, our study suggests that 1JC-H has potential across a broader range of systems. Additionally, the analysis demonstrates that lone pair energy reflects basicity rather than σ-donor ability.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403403"},"PeriodicalIF":3.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142680280","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Deep-Ultraviolet Transparent Nonlinear Optical Phosphates: A New Alternative to Conventional Borates. 深紫外透明非线性光学磷酸盐：传统硼酸盐的新替代品。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2024-11-20 DOI: 10.1002/chem.202403991

Hua-Jun Zhao, Jia-Xiang Zhang, Hua Lin

{"title":"Deep-Ultraviolet Transparent Nonlinear Optical Phosphates: A New Alternative to Conventional Borates.","authors":"Hua-Jun Zhao, Jia-Xiang Zhang, Hua Lin","doi":"10.1002/chem.202403991","DOIUrl":"https://doi.org/10.1002/chem.202403991","url":null,"abstract":"Deep ultraviolet (DUV) nonlinear optical (NLO) crystals with balanced performance are crucial for extending laser wavelengths into the DUV region, essential for various laser applications. However, developing ideal DUV crystals is challenging due to stringent requirements: strong second-harmonic generation (SHG) response, short cut-off wavelength, and effective phase-matching behavior. DUV NLO borates, which feature π-conjugated groups, have garnered attention for their higher SHG coefficients compared to phosphates. However, phosphates typically show short UV cut-off edges due to the large HOMO-LUMO gap (approximately 9.6 eV) of the [PO₄] units. To enhance the SHG effect while maintaining DUV transparency in phosphates, several strategies have been proposed: 1) using distorted polymerized P-O groups like isolated C₁-[P₃O₁₀]⁵⁻ and [P₂O₇]⁴⁻; 2) aligning isolated [PO₄]³⁻ tetrahedra along the polar screw axis; 3) introducing additional NLO-active units; and 4) exploring new units derived from [PO₄]³⁻, such as [PO₃F]²⁻ tetrahedra. These strategies have led to the successful development of various non-centrosymmetric phosphates, highlighting their potential as DUV NLO candidates. This review explores the relationship between their crystal structures and DUV NLO performance, and proposes future directions for developing ideal DUV NLO materials.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403991"},"PeriodicalIF":3.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142680282","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Intersystem Crossing, Photo-Induced Charge Separation and Regioisomer-Specific Excited State Dynamics in Fully Rigid Spiro Rhodammine-Naphthalene/Anthraquinone Electron Donor-Acceptor Dyads. 完全刚性螺罗-罗丹明-萘/蒽醌电子施主-受主二元体中的系间交叉、光诱导电荷分离和区域异构体特异性激发态动力学。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2024-11-20 DOI: 10.1002/chem.202403758

Kaiyue Ye, Andrey A Sukhanov, Jiayu Li, Lishan Liu, Xi Chen, Jianzhang Zhao, Violeta K Voronkova, MingDe Li

{"title":"Intersystem Crossing, Photo-Induced Charge Separation and Regioisomer-Specific Excited State Dynamics in Fully Rigid Spiro Rhodammine-Naphthalene/Anthraquinone Electron Donor-Acceptor Dyads.","authors":"Kaiyue Ye, Andrey A Sukhanov, Jiayu Li, Lishan Liu, Xi Chen, Jianzhang Zhao, Violeta K Voronkova, MingDe Li","doi":"10.1002/chem.202403758","DOIUrl":"https://doi.org/10.1002/chem.202403758","url":null,"abstract":"We prepared a series fully rigid spiro electron donor-acceptor orthogonal dyads, with closed form of rhodamine (Rho) as electron donor and naphthalene (Np)/anthraquinone (AQ) as electron acceptor, to access the long-lived triplet charge separation (3CS) state, via the electron spin control method. We found strong dependency of the photophysical property of the dyads on the amino substitution positions of the Np chromophores in the dyads 1,8-DaNp-Rho and 2,3-DaNp-Rho. Nanosecond transient absorption (ns-TA) spectra show the population of the 3LE state (lifetime: 47 μs) for 2,3-DaNp-Rho, however, long-lived 3CS state was observed (τCS = 0.62 μs) for AQ-Rho, with a CS quantum yield of ΦCS = 58%. Based on femtosecond transient absorption (fs-TA) spectra, spin orbit charge transfer ISC (SOCT-ISC) is proposed to be responsible for the formation of the triplet states. Time-resolved electron paramagnetic resonance (TREPR) spectra of AQ-Rho indicate the presence of two states, a 3LE state with zero field splitting (ZFS) D parameter of 1400 MHz and E parameter of -410 MHz, formed via radical pair ISC (RP-ISC) and SOCT-ISC mechanism; and a 3CS state with the electron spin-spin interaction in the regime of spin-correlated radical pair (SCRP).","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403758"},"PeriodicalIF":3.9,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142680289","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Parts-per-million Level Loading Cyclometalated Ru(II)-NHC Catalyzed Selective Oxidation of Olefins to Carbonyls. 百万分率级负载环甲基化 Ru(II)-NHC 催化烯烃到羰基的选择性氧化。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2024-11-19 DOI: 10.1002/chem.202403135

Monuranjan Konwar, Tapashi Das, Animesh Das

{"title":"Parts-per-million Level Loading Cyclometalated Ru(II)-NHC Catalyzed Selective Oxidation of Olefins to Carbonyls.","authors":"Monuranjan Konwar, Tapashi Das, Animesh Das","doi":"10.1002/chem.202403135","DOIUrl":"https://doi.org/10.1002/chem.202403135","url":null,"abstract":"Oxidative cleavage of olefins is a useful reaction in organic synthesis. The most well-known catalytic system is the osmium based Lemieux-Johnson catalyst, which generally requires high catalyst loading and tends to suffer from rapid overoxidation to produce the acid predominantly. Hence, the development of a mild, general, and selective method toward the oxidative cleavage of alkenes to carbonyl compounds is highly desired. In this work, a highly efficient ruthenium-based catalyst for olefin oxidation has been demonstrated by employing a fused π-conjugated imidazo[1,5-a]quinoxaline (ImQx) based NHC ligand with bidentate C(carbanion)^CNHC motif. Strong C-donor ligands, paired with a rigid backbone and ruthenium redox activity, provided exceptionally high catalytic activity and a long lifetime for olefin oxidation. Complex showed high catalytic activity and a long lifetime, TONs are several million. The catalyst tolerates numerous functional groups and can be applicable to challenging biomass, natural products, sugar, amino acids, and fatty acid-derived substrates. Based on kinetic studies, thermodynamic activation parameters, and DFT study, the mechanistic finding demonstrated that [3+2] cycloaddition reaction is the key step in the oxidation process. The use of the by-product NaIO3 in the catalytic efficiency has been disclosed for the first time.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202403135"},"PeriodicalIF":3.9,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142674643","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Stepwise Construction of Supramolecular A2B4-type Miktoarm Star Copolymers with a Cobalt Phthalocyanine Core. 逐步构建以酞菁钴为核心的超分子 A2B4 型 Miktoarm 星型共聚物。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2024-11-19 DOI: 10.1002/chem.202403749

Xinhao Zhong, Hsu-Tzu Cheng, Chu-Chen Chueh, Masayuki Takeuchi, Junko Aimi

引用次数: 0

In-situ reduced Cu3N nanocrystals enable high-efficiency ammonia synthesis and zinc-nitrate batteries. 原位还原 Cu3N 纳米晶体实现了高效氨合成和硝酸锌电池。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2024-11-19 DOI: 10.1002/chem.202404129

Shanshan Chen, Zhiwei Wang, Quan Zhang, Shiming Qiu, Yifan Liu, Guangzhi Hu, Jun Luo, Xijun Liu

{"title":"In-situ reduced Cu3N nanocrystals enable high-efficiency ammonia synthesis and zinc-nitrate batteries.","authors":"Shanshan Chen, Zhiwei Wang, Quan Zhang, Shiming Qiu, Yifan Liu, Guangzhi Hu, Jun Luo, Xijun Liu","doi":"10.1002/chem.202404129","DOIUrl":"10.1002/chem.202404129","url":null,"abstract":"Nitrate reduction reaction (NO3RR) involves an 8-electron transfer process and competes with the hydrogen evolution reaction process, resulting in lower yields and Faraday efficiency (FE) in the process of NH3 synthesis. Especially, Cu-based catalysts (Cu0 and Cu+) have been investigated in the field of NO3RR due to the energy levels of d-orbital and the least unoccupied molecular orbital (LUMO) π* of nitrate's orbital. Based on the above, we synthesized a Cu-based compound containing Cu3N (Cu+) through a simple one-step pyrolysis method, applied it to electrocatalytic NO3RR, and tested the performance of the Zn-NO3- battery. Through various characterization analyses, Cu-based catalysts (Cu+) are the key active sites in reduction reactions, making Cu3N a potential catalyst for ammonia synthesis. The research results indicate the application of Cu3N catalyst in NO3RR shows the best NH3 yield of 173.7 μmol h-1 cm-2, with FENH3 reaching 91.0% at -0.3 V vs. RHE, which is much higher than that of Cu catalyst without N. In addition, the Zn-NO3- battery based on Cu3N electrode also exhibits an NH3 yield of 39.8 μmol h-1 cm-2, 63.0% FENH3, and a power density of 2.7 mW cm-2, as well as stable cycling charge-discharge stability for 5 hours.","PeriodicalId":144,"journal":{"name":"Chemistry - A European Journal","volume":" ","pages":"e202404129"},"PeriodicalIF":3.9,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666526","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Site-Selective γ-Trihalomethylation and γ-Dihalomethylidenation of Silyl Dienol Ethers under Organophotoredox Catalysis. 有机醛催化下硅烷二酚醚的γ-三卤甲基化和γ-二卤甲基亚甲基化的位点选择性。

IF 3.9 2区化学

Chemistry - A European Journal Pub Date : 2024-11-19 DOI: 10.1002/chem.202403598

Camille Banoun, Fabien Bourdreux, Emmanuel Magnier, Guillaume Dagousset

引用次数: 0