Chem最新文献_第8页

From low-res measurements to high-res insights: Revolutionizing COF structural determination

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2025.102452

Elad Harel

引用次数: 0

One-pot catalytic conversion of polyethylene wastes to gasoline through a dual-catalyst system 通过双催化剂系统将聚乙烯废料一锅催化转化为汽油

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.10.007

Wanying Han , Longfei Lin , Ziyu Cen , Yubin Ke , Qian Xu , Junfa Zhu , Xuelei Mei , Zhanghui Xia , Xinrui Zheng , Yaqin Wang , Yani Liu , Mingyuan He , Haihong Wu , Buxing Han

{"title":"One-pot catalytic conversion of polyethylene wastes to gasoline through a dual-catalyst system","authors":"Wanying Han , Longfei Lin , Ziyu Cen , Yubin Ke , Qian Xu , Junfa Zhu , Xuelei Mei , Zhanghui Xia , Xinrui Zheng , Yaqin Wang , Yani Liu , Mingyuan He , Haihong Wu , Buxing Han","doi":"10.1016/j.chempr.2024.10.007","DOIUrl":"10.1016/j.chempr.2024.10.007","url":null,"abstract":"<div><div>Chemical upcycling of polyethylene (PE) waste presents a viable and promising approach to address the issues of plastic waste accumulation. However, developing cost-effective and efficient routes for converting PE waste into value-added products remains a challenging task. Here, we report a one-pot, dual-catalyst system for efficient conversion of PE into gasoline without the need for noble-metal catalysts, external hydrogen, or solvents. A gasoline yield of up to 87% is achieved over a dual-catalyst system comprising WZr-KIT-6 and HZSM-5 at 240°C. The WZr-KIT-6 catalyst facilitated the activation and pre-cracking of PE chains into unsaturated oligomers over Si-O-Zr and W-O(H)-Zr sites. These unsaturated oligomers, characterized by increased mobility and reactivity, were subsequently converted into C<sub>4</sub>–C<sub>12</sub> gasoline-range compounds through β-scission, isomerization, and hydride transfer over HZSM-5. The synergistic reaction mechanism over mesoporous and microporous materials was crucial for enhancing the efficiency and selectivity of PE conversion.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102340"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589051","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

The sustainability potential of single-atom catalysts in chemical process

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2025.102412

Zirui Gao , Shixiang Yu , Zeyan Cen , Ding Ma

引用次数: 0

Ion-dipole interaction manipulated bilateral interface chemistry for deep rechargeability and high redox activity of Zn-organic batteries

IF 23.5 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2025.102411

Yanyan Chen, Bowen Yin, Yinxiang Zeng, Hongfei Wang, Bin-Bin Xie, Deyan Luan, Yong Hu, Xiong Wen (David) Lou

{"title":"Ion-dipole interaction manipulated bilateral interface chemistry for deep rechargeability and high redox activity of Zn-organic batteries","authors":"Yanyan Chen, Bowen Yin, Yinxiang Zeng, Hongfei Wang, Bin-Bin Xie, Deyan Luan, Yong Hu, Xiong Wen (David) Lou","doi":"10.1016/j.chempr.2025.102411","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102411","url":null,"abstract":"The practical application of Zn-based batteries is compromised by rampant dendrite growth, unfavorable side reactions, and serious capacity decay. We report a trifunctional glutarimide (Glu) electrolyte additive to stabilize the electrochemical reaction of the Zn anode and facilitate redox activity of the cathode. Theoretical calculations and spectroscopic characterizations reveal that Glu with the electron-withdrawing/donating capability can substitute partially coordinated water and manipulate the solvation structure by reinforced ion-dipole interactions. Meanwhile, Glu can form a solid electrolyte interphase layer and alleviate parasitic reactions. Consequently, Glu renders excellent Zn plating/stripping cycling of 2,000 h at 1 mA cm<sup>−2</sup>/1 mAh cm<sup>−2</sup>. Even at an ultra-high depth of discharge of 85.2%, a stable cycling of 138 h is obtained. The formulated additive serves as the charge redistributor and decouples the cation-anion interaction to stabilize the interaction of ClO<sub>4</sub><sup>−</sup> with the half-oxidized protonated polyaniline, enabling the Zn-organic battery with enhanced energy storage performance.","PeriodicalId":268,"journal":{"name":"Chem","volume":"50 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401696","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

Globally aromatic odd-electron π-magnetic macrocycle 全芳香奇电子π-磁性大环

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.09.015

Federico Villalobos , Jan Berger , Adam Matěj , Reed Nieman , Ana Sánchez-Grande , Diego Soler , Andrés Pinar Solé , Hans Lischka , Mikuláš Matoušek , Jiri Brabec , Libor Veis , Alba Millan , Carlos Sánchez-Sánchez , Araceli G. Campaña , Juan M. Cuerva , Pavel Jelínek

引用次数: 0

Sequence-defined main-chain photoswitching macromolecules with odd-even-effect-controlled properties 具有奇偶效应控制特性的序列定义主链光开关大分子

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.10.008

Linh Duy Thai , Jochen A. Kammerer , Dmitri Golberg , Hatice Mutlu , Christopher Barner-Kowollik

{"title":"Sequence-defined main-chain photoswitching macromolecules with odd-even-effect-controlled properties","authors":"Linh Duy Thai , Jochen A. Kammerer , Dmitri Golberg , Hatice Mutlu , Christopher Barner-Kowollik","doi":"10.1016/j.chempr.2024.10.008","DOIUrl":"10.1016/j.chempr.2024.10.008","url":null,"abstract":"<div><div>The installation of stimuli-responsive moieties into their main chain maximizes the stimuli response of polymers. Yet, facile and orthogonal synthesis of such complex macromolecules is a daunting challenge, especially for achieving absolute chain-end-group fidelity, monodispersity, and the formation of block copolymers (BCPs). We harness metal-free hydroxyl-yne click and deprotection chemistry to realize monodisperse, sequence-defined oligomers and BCPs featuring α-bisimines as main-chain photoswitches and orthogonally incorporate functional terminal groups (olefins, acrylates, and non-activated alkynes). We reveal the significant influence of the sequence on solution and solid-state material properties, which manifests as a strong odd-even effect on the hydrodynamic volume, glass transition temperature, and BCP domain spacing. The odd-even effect originates from the distinct symmetries of the sequences resulting from our precise synthetic strategy. Thus, our sequence-defined, orthogonal synthesis strategy with near absolute chain-end-group fidelity and wide functional group compatibility paves the way toward complex polymeric materials with precise properties, topology, composition, and main-chain functionalities.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102341"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574648","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

Ordered [2]catenanes in covalent organic frameworks: From molecules to materials 共价有机框架中的有序[2]链烷：从分子到材料

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.10.024

Ruozhou Huang , Yuping Wang

引用次数: 0

2D covalent organic framework via catenation 通过催化反应实现二维共价有机框架

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.09.006

Thirumurugan Prakasam , Sudhir Kumar Sharma , Florent Ravaux , Farah Benyettou , Matteo Lusi , Varghese Sabu , Philippe Bazin , Thomas Delclos , Ramesh Jagannathan , Jamie Whelan , Mohamad El-Roz , Mark A. Olson , Mahmoud Abdellatief , Obieda S. Mudraj , Felipe Gándara , Ali Trabolsi

{"title":"2D covalent organic framework via catenation","authors":"Thirumurugan Prakasam , Sudhir Kumar Sharma , Florent Ravaux , Farah Benyettou , Matteo Lusi , Varghese Sabu , Philippe Bazin , Thomas Delclos , Ramesh Jagannathan , Jamie Whelan , Mohamad El-Roz , Mark A. Olson , Mahmoud Abdellatief , Obieda S. Mudraj , Felipe Gándara , Ali Trabolsi","doi":"10.1016/j.chempr.2024.09.006","DOIUrl":"10.1016/j.chempr.2024.09.006","url":null,"abstract":"<div><div>Molecular-level structural modification is a well-established approach to impart advanced functionality to materials that continues to be the focus of research and development in both academic and industrial laboratories. Here, we report the synthesis of an ordered two-dimensional (2D) poly[2]catenate from the simultaneous self-assembly of two organic ligands and a metal salt by the formation of catenate links using metal coordination and imine condensation reactions. Subsequent chemical reduction of the imine bonds generated the corresponding demetallized poly[2]catenane, which was found to have greater non-rigid-body-like character than the poly[2]catenate as a result of the increased internal dynamics of the mechanical bonds and resulted in an 8-fold increase in elasticity. This synthetic approach allowed for the efficient incorporation of mechanically interlocked molecules (MIMs) within a 2D ordered structure and demonstrated their importance in improving the physical properties of materials by accessing molecular degrees of freedom that cannot be achieved by other means.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102307"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142384025","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

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 19.1 1区化学

Chem Pub Date : 2025-02-13 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":"10.1016/j.chempr.2024.11.009","url":null,"abstract":"<div><div>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.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102371"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","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

Single-site nanozyme with exposed unsaturated Cu-O2 sites for tumor therapy by coordinating innate immunity and vasculature normalization 带有暴露的不饱和 Cu-O2 位点的单位点纳米酶，通过协调先天免疫和血管正常化治疗肿瘤

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.08.020

Yang Liu , Huan Zhao , Rui Niu , Bin Zhang , Boon Teck Garrick Lim , Shuyan Song , Yinghui Wang , Hongjie Zhang , Yanli Zhao

{"title":"Single-site nanozyme with exposed unsaturated Cu-O2 sites for tumor therapy by coordinating innate immunity and vasculature normalization","authors":"Yang Liu , Huan Zhao , Rui Niu , Bin Zhang , Boon Teck Garrick Lim , Shuyan Song , Yinghui Wang , Hongjie Zhang , Yanli Zhao","doi":"10.1016/j.chempr.2024.08.020","DOIUrl":"10.1016/j.chempr.2024.08.020","url":null,"abstract":"<div><div>The low immunogenicity of tumors, coupled with abnormal and dysfunctional tumor vasculature, hinders the infiltration and function of effector T cells and suppresses the efficacy of immunotherapy. Herein, we developed a defective-copper-based metal-organic framework single-site nanozyme (F@D-CHTP SN) with co-loaded MSA-2 (stimulator of interferon genes [STING] agonist) and fruquintinib (vascular endothelial growth factor receptor [VEGFR] inhibitor). The conjugated organic ligands and highly exposed unsaturated Cu-O<sub>2</sub> single-atom sites endow F@D-CHTP SN with excellent reactive oxygen species generation activity, which can disrupt the cellular redox balance, impair mitochondrial function, and ultimately induce cuproptosis and ferroptosis, enhancing tumor immunogenicity. Meanwhile, intratumoral STING activation and VEGFR blockade synergistically promote tumor vasculature normalization, further reshaping the immunosuppressive microenvironment and enhancing T cell infiltration to achieve effective tumor suppression. Our work demonstrates the feasibility and significant synergistic effects of initiating cascade-enhancing immunity by combining cuproptosis and ferroptosis with STING activation and tumor vasculature normalization.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102297"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142246236","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