Chem最新文献_第9页

Morphological-transition-induced motion

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2025.102454

Xianbao Li , Qi Li , Junbai Li

引用次数: 0

Electrocatalysis enables polyvinyl chloride functionalization

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2025.102435

Yuanbo Liu , Haohong Duan

引用次数: 0

Terahertz-Raman spectroscopy for in situ benchtop monitoring of changes to extended, supramolecular structure in milling mechanochemistry 太赫兹-拉曼光谱法用于原位台式监测研磨机械化学中扩展超分子结构的变化

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.09.018

Tristan H. Borchers , Filip Topić , Mihails Arhangelskis , Michael Ferguson , Cameron B. Lennox , Patrick A. Julien , Tomislav Friščić

{"title":"Terahertz-Raman spectroscopy for in situ benchtop monitoring of changes to extended, supramolecular structure in milling mechanochemistry","authors":"Tristan H. Borchers , Filip Topić , Mihails Arhangelskis , Michael Ferguson , Cameron B. Lennox , Patrick A. Julien , Tomislav Friščić","doi":"10.1016/j.chempr.2024.09.018","DOIUrl":"10.1016/j.chempr.2024.09.018","url":null,"abstract":"<div><div>Low-frequency Raman, also known as terahertz-Raman (THz-Raman), spectroscopy offers a laboratory benchtop-based alternative to synchrotron X-ray diffraction for real-time, <em>in situ</em> monitoring of ball-milling mechanochemical reactions. Although direct monitoring of the long-range structure of materials during mechanochemical reactions is generally challenging by conventional Raman spectroscopy, and typically requires synchrotron X-ray diffraction, here we use THz-Raman spectroscopy to monitor mechanosynthesis of cocrystals, stoichiomorphs, and polymorphs, detect multi-step sequences, and discover solid-state phases in systems difficult to differentiate using fingerprint-region Raman spectroscopy—all through real-time observation of changes in lattice vibrational models. The methodology is augmented by periodic density functional theory (DFT), which enables structural interpretation of spectroscopic changes, notably the identification of THz-Raman bands associated with halogen bond transformations. Simultaneous monitoring of mechanochemical processes in both the fingerprint and low-frequency Raman regions enables real-time observation of changes to extended as well as molecular structure during milling, in a single laboratory benchtop experiment, without synchrotron radiation.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102319"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142489464","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Anisotropy-guided interface molecular engineering for stable blue electroluminescence 各向异性引导的界面分子工程实现稳定的蓝色电致发光

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.08.019

Eunhye Hwang , Unhyeok Jo , Jiyeon Kim , Deok-Ho Roh , Seung Chan Kim , Minseok Kim , Hyun-Chul Ki , Wonyoung Choe , Jun Yeob Lee , Tae-Hyuk Kwon

{"title":"Anisotropy-guided interface molecular engineering for stable blue electroluminescence","authors":"Eunhye Hwang , Unhyeok Jo , Jiyeon Kim , Deok-Ho Roh , Seung Chan Kim , Minseok Kim , Hyun-Chul Ki , Wonyoung Choe , Jun Yeob Lee , Tae-Hyuk Kwon","doi":"10.1016/j.chempr.2024.08.019","DOIUrl":"10.1016/j.chempr.2024.08.019","url":null,"abstract":"<div><div>Despite the emergence of interlayers with high triplet energies (T<sub>1</sub>) to stabilize blue phosphorescent organic light-emitting diodes (PhOLEDs), a limited understanding of their molecular structures poses a challenge in preventing triplet exciton leakage while maintaining charge balance. Here, we report a rational design strategy for interlayers aimed at concurrently controlling T<sub>1</sub> and molecular arrangements conducive to charge transport. Four interlayer materials having high T<sub>1</sub> (∼3.0 eV) are developed as electron-blocking materials (EBMs), utilizing asymmetric orthogonal geometries with varying torsion angles and dipole moments. X-ray crystallographic analyses reveal that the EBM, featuring the most asymmetric charge distributions, exhibits a herringbone packing and a face-on orientation through dipole-induced anisotropic interactions, thereby promoting hole transport. The power efficiency and operational lifetime of the corresponding blue PhOLEDs increase by 24% and 21%, respectively, compared with a conventional EBM. This study offers extensive insights into designing interlayers with versatile applicability in optoelectronics harnessing triplets.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102296"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142246235","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

Non-fluorinated electrolytes with micelle-like solvation for ultra-high-energy-density lithium metal batteries 用于超高能量密度锂金属电池的胶束状溶解的无氟电解质

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2024.09.005

Rui Qiao , Yan Zhao , Shijie Zhou , Huijun Zhang , Fuzhu Liu , Tianhong Zhou , Baoyu Sun , Hao Fan , Chao Li , Yanhua Zhang , Feng Liu , Xiangdong Ding , Jang Wook Choi , Ali Coskun , Jiangxuan Song

{"title":"Non-fluorinated electrolytes with micelle-like solvation for ultra-high-energy-density lithium metal batteries","authors":"Rui Qiao , Yan Zhao , Shijie Zhou , Huijun Zhang , Fuzhu Liu , Tianhong Zhou , Baoyu Sun , Hao Fan , Chao Li , Yanhua Zhang , Feng Liu , Xiangdong Ding , Jang Wook Choi , Ali Coskun , Jiangxuan Song","doi":"10.1016/j.chempr.2024.09.005","DOIUrl":"10.1016/j.chempr.2024.09.005","url":null,"abstract":"<div><div>Electrolyte engineering plays a critical role in enabling lithium (Li) metal batteries. However, the simultaneous realization of anion-rich solvation structure and high ionic conductivity of electrolytes via solvation structure design remains challenging. Here, we report a low-cost, non-fluorinated electrolyte with a micelle-like solvation structure by introducing amphiphilic n-butyl methyl ether (MNBE) into Li bis(fluorosulfonyl)imide (LiFSI)/1,2-dimethoxyethane (DME) for stable Li metal batteries (LMBs). MNBE can effectively promote Li<sup>+</sup>-FSI<sup>−</sup> coordination through steric crowding. Meanwhile, the inert alkyl chains of MNBE can mitigate the reaction between electrolyte and Li metal due to their lithiophobicity. Specifically, the micelle-like, non-fluorinated electrolyte exhibits an ionic conductivity as high as 12.55 mS cm<sup>−1</sup>, and its anion-rich solvation structure promotes the formation of LiF-rich solid-electrolyte interphase. We constructed a 7.3 Ah Li||NMC811 pouch cell employing this electrolyte under harsh conditions, exhibiting ultra-high specific energy of 503.7 Wh kg<sup>−1</sup> with impressive cycling stability of 84.1% capacity retention after 100 cycles.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 2","pages":"Article 102306"},"PeriodicalIF":19.1,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142369578","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Spectral control of photoenzyme through allosteric chromophore tuning 通过变构生色团调谐的光酶光谱控制

IF 19.1 1区化学

Chem Pub Date : 2025-02-13 DOI: 10.1016/j.chempr.2025.102430

Menghan Xu , Yuki Yamanashi , Motomu Kanai

引用次数: 0

para-Selective C–H alkylation of aroyl chlorides through organic photoredox-catalyzed radical tele-substitution

IF 23.5 1区化学

Chem Pub Date : 2025-02-12 DOI: 10.1016/j.chempr.2025.102446

Ryoto Oya, Hinata Sato, Kazunori Nagao, Hirohisa Ohmiya

{"title":"para-Selective C–H alkylation of aroyl chlorides through organic photoredox-catalyzed radical tele-substitution","authors":"Ryoto Oya, Hinata Sato, Kazunori Nagao, Hirohisa Ohmiya","doi":"10.1016/j.chempr.2025.102446","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102446","url":null,"abstract":"The site-selective C(sp<sup>2</sup>)–H alkylation of arenes has provided ubiquitous fragments found in pharmaceutical drugs and agrochemicals. Although <em>ortho</em>- and <em>meta</em>-selective alkylation reactions have been achieved well, <em>para</em>-selective examples are scarce. The currently available methods have been designed on the unique behaviors and characteristics of metals to achieve high <em>para</em>-selectivity. Herein, we demonstrate the <em>para</em>-selective C(sp<sup>2</sup>)–H alkylation of aroyl chlorides with alkyltrifluoroborates and trialkylphosphine through an organic photoredox-catalyzed radical <em>tele</em>-substitution. The reaction proceeds through the <em>para</em>-selective addition of alkyl radicals to <em>in</em>-<em>situ</em>-generated aroyl trialkylphosphonium intermediates followed by a hydrogen shift. Notably, the <em>para</em>-alkylation is associated with the conversion of the carbonyl trialkylphosphonium group to the formyl group, producing <em>para</em>-alkylated benzaldehyde derivatives. This metal-free site-selective C(sp<sup>2</sup>)–C(sp<sup>3</sup>) bond formation allows for streamlined synthesis of siponimod and SR-31747.","PeriodicalId":268,"journal":{"name":"Chem","volume":"20 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143394035","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

Reversible-deactivation radical copolymerization of tetrafluoroethylene via the formation of divergent termini in dormant chains

IF 23.5 1区化学

Chem Pub Date : 2025-02-12 DOI: 10.1016/j.chempr.2025.102434

Kaixuan Chen, Zexi Zhang, Qianhao Ye, Yixuan Liu, Shantao Han, Mengli Xu, Mao Chen

引用次数: 0

Air-stable radical polycyclic aromatic hydrogen-bonded organic frameworks

IF 23.5 1区化学

Chem Pub Date : 2025-02-12 DOI: 10.1016/j.chempr.2025.102445

Bai-Tong Liu, Tao Li, Sheng-Hao Gong, Jia-Chuan Liu, Ze-Yu Ruan, Han Han, Timothy Y.-Z. Li, Yuanning Feng, Rui Wang, Li Gong, Xieming Xu, Rong Cao, Ming-Liang Tong, J. Fraser Stoddart, Tian-Fu Liu

{"title":"Air-stable radical polycyclic aromatic hydrogen-bonded organic frameworks","authors":"Bai-Tong Liu, Tao Li, Sheng-Hao Gong, Jia-Chuan Liu, Ze-Yu Ruan, Han Han, Timothy Y.-Z. Li, Yuanning Feng, Rui Wang, Li Gong, Xieming Xu, Rong Cao, Ming-Liang Tong, J. Fraser Stoddart, Tian-Fu Liu","doi":"10.1016/j.chempr.2025.102445","DOIUrl":"https://doi.org/10.1016/j.chempr.2025.102445","url":null,"abstract":"Air-stable radical materials have emerged as promising candidates for next-generation electronic materials. Traditionally, constructing radical materials has required the intricate design and prolonged synthesis of radical building blocks. Herein, we have discovered a group of polycyclic aromatic monomers, previously considered to be air-unstable radicals, that can be oxidized to air-stable radical materials according to a post-synthetic protocol when they are incorporated into solid porous hydrogen-bonded organic frameworks (HOFs). The inherent porosity and crystallinity of HOFs facilitate extensive interactions with redox agents, such as tetravalent cerium(IV). These radical HOF materials exhibit high radical concentrations with paramagnetic behavior equivalent to two monomers sharing an unpaired electron. The HOFs can maintain their radical nature under ambient conditions on account of spin delocalization along the [π···π] stacked units. The radical formation transforms the HOFs from insulators to typical n-type semiconductors. This discovery opens up avenues for exploring stable radical materials with diverse applications.","PeriodicalId":268,"journal":{"name":"Chem","volume":"7 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143394033","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

Transition-path times of individual molecular shuttles under mechanical equilibrium show symmetry

IF 23.5 1区化学

Chem Pub Date : 2025-02-11 DOI: 10.1016/j.chempr.2024.102410

Tomás Nicolás-García, Natalia Martín Sabanés, Rebeca Bocanegra, R. Dean Astumian, Emilio M. Pérez, Borja Ibarra

引用次数: 0