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Elucidating oxygen evolution and reduction mechanisms in nitrogen-doped carbon-based photocatalysts 阐明掺氮碳基光催化剂中的氧进化和还原机制
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-10 DOI: 10.1016/j.cclet.2024.110439
Yan Wang , Jiaqi Zhang , Xiaofeng Wu , Sibo Wang , Masakazu Anpo , Yuanxing Fang
Solar-induced water oxidation reaction (WOR) for oxygen evolution is a critical step in the transformation of Earth's atmosphere from a reducing to an oxidation one during its primordial stages. WOR is also associated with important reduction reactions, such as oxygen reduction reaction (ORR), which leads to the production of hydrogen peroxide (H2O2). These transitions are instrumental in the emergence and evolution of life. In this study, transition metals were loaded onto nitrogen-doped carbon (NDC) prepared under the primitive Earth's atmospheric conditions. These metal-loaded NDC samples were found to catalyze both WOR and ORR under light illumination. The chemical pathways initiated by the pristine and metal-loaded NDC were investigated. This study provides valuable insights into potential mechanisms relevant to the early evolution of our planet.
太阳诱导的氧进化水氧化反应(WOR)是地球大气在原始阶段从还原型向氧化型转变的关键步骤。水氧化反应还与重要的还原反应有关,如氧还原反应(ORR),它导致产生过氧化氢(H2O2)。这些转变对生命的出现和进化至关重要。在这项研究中,过渡金属被负载到在原始地球大气条件下制备的掺氮碳 (NDC) 上。研究发现,这些负载金属的 NDC 样品在光照下可催化 WOR 和 ORR。研究了原始 NDC 和金属负载 NDC 引发的化学途径。这项研究为了解与我们星球早期演化相关的潜在机制提供了宝贵的见解。
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引用次数: 0
Fe3+ ion quantification with reusable bioinspired nanopores 利用可重复使用的生物启发纳米孔量化 Fe3+ 离子
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-07 DOI: 10.1016/j.cclet.2024.110428
Yanqiong Wang , Yaqi Hou , Fengwei Huo , Xu Hou
Excessive Fe3+ ion concentrations in wastewater pose a long-standing threat to human health. Achieving low-cost, high-efficiency quantification of Fe3+ ion concentration in unknown solutions can guide environmental management decisions and optimize water treatment processes. In this study, by leveraging the rapid, real-time detection capabilities of nanopores and the specific chemical binding affinity of tannic acid to Fe3+, a linear relationship between the ion current and Fe3+ ion concentration was established. Utilizing this linear relationship, quantification of Fe3+ ion concentration in unknown solutions was achieved. Furthermore, ethylenediaminetetraacetic acid disodium salt was employed to displace Fe3+ from the nanopores, allowing them to be restored to their initial conditions and reused for Fe3+ ion quantification. The reusable bioinspired nanopores remain functional over 330 days of storage. This recycling capability and the long-term stability of the nanopores contribute to a significant reduction in costs. This study provides a strategy for the quantification of unknown Fe3+ concentration using nanopores, with potential applications in environmental assessment, health monitoring, and so forth.
废水中过量的 Fe3+ 离子浓度长期以来一直威胁着人类健康。对未知溶液中的 Fe3+ 离子浓度进行低成本、高效率的定量分析,可以为环境管理决策和优化水处理工艺提供指导。在本研究中,利用纳米孔的快速、实时检测能力以及单宁酸与 Fe3+ 的特异性化学结合亲和力,建立了离子电流与 Fe3+ 离子浓度之间的线性关系。利用这种线性关系,实现了对未知溶液中 Fe3+ 离子浓度的定量。此外,还利用乙二胺四乙酸二钠盐将 Fe3+ 从纳米孔中置换出来,使其恢复到初始状态并重新用于 Fe3+ 离子定量。可重复使用的生物启发纳米孔在储存 330 天后仍能保持功能。这种回收能力和纳米孔的长期稳定性大大降低了成本。这项研究提供了一种利用纳米孔量化未知 Fe3+ 浓度的策略,有望应用于环境评估、健康监测等领域。
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引用次数: 0
Coating colloidal particles with a well-defined polymer layer by surface-initiated photoinduced polymerization-induced self-assembly and the subsequent seeded polymerization 通过表面引发的光诱导聚合自组装和随后的种子聚合,为胶体颗粒涂上一层定义明确的聚合物层
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-07 DOI: 10.1016/j.cclet.2024.110431
Bing Niu , Honggao Huang , Liwei Luo , Li Zhang , Jianbo Tan
Core-shell colloidal particles with a polymer layer have broad applications in different areas. Herein, we developed a two-step method combining aqueous surface-initiated photoinduced polymerization-induced self-assembly and photoinduced seeded reversible addition-fragmentation chain transfer (RAFT) polymerization to prepare a diverse set of core-shell colloidal particles with a well-defined polymer layer. Chemical compositions, structures, and thicknesses of polymer layers could be conveniently regulated by using different types of monomers and feed [monomer]/[chain transfer agent] ratios during seeded RAFT polymerization.
带有聚合物层的核壳胶体粒子在不同领域有着广泛的应用。在此,我们开发了一种两步法,结合水表面诱导的光诱导聚合自组装和光诱导的种子可逆加成-碎片链转移(RAFT)聚合,制备出多种具有明确聚合物层的核壳胶体粒子。在种子可逆加成-链转移聚合过程中,通过使用不同类型的单体和进料[单体]/[链转移剂]比例,可以方便地调节聚合物层的化学成分、结构和厚度。
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引用次数: 0
Understanding excitonic behavior and electroluminescence light emitting diode application of carbon dots 了解碳点的激子行为和电致发光发光二极管的应用
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-07 DOI: 10.1016/j.cclet.2024.110426
Yuan Liu , Boyang Wang , Yaxin Li , Weidong Li , Siyu Lu
Carbon dots (CDs), due to their low cost, high stability, and high luminous efficiency, have emerged as an excellent material for the emissive layer in next-generation electroluminescent light-emitting diodes (ELEDs). However, improving the efficiency of fluorescent CDs-based ELEDs remains challenging, primarily because it is difficult to utilize triplet excitons in the electroluminescence process. Therefore, enhancing the exciton utilization efficiency of CDs during electroluminescence is crucial. Based on this, we exploited the characteristic large exciton binding energy commonly found in CDs to develop exciton-emitting CDs. These CDs facilitate the radiative recombination of excitons during electroluminescence, thereby improving the electroluminescent efficiency. By rationally selecting precursors, we developed high quantum efficiency CDs and subsequently constructed CDs-based ELEDs. The blue-light device exhibited an external quantum efficiency of over 4 %. This study introduces a novel design concept for CDs, providing a new strategy for developing high-performance blue ELEDs based on CDs.
碳点(CD)因其低成本、高稳定性和高发光效率,已成为下一代电致发光二极管(ELED)发光层的绝佳材料。然而,提高基于荧光光盘的电致发光二极管的效率仍然具有挑战性,这主要是因为在电致发光过程中很难利用三重激子。因此,提高 CD 在电致发光过程中的激子利用效率至关重要。在此基础上,我们利用光盘中常见的大激子结合能特性,开发出了激子发光光盘。这些光盘有助于激子在电致发光过程中进行辐射重组,从而提高电致发光效率。通过合理选择前驱体,我们开发出了高量子效率的光盘,并随后构建了基于光盘的电致发光器件。该蓝光器件的外部量子效率超过 4%。这项研究引入了一种新颖的光盘设计理念,为开发基于光盘的高性能蓝光发光二极管提供了一种新策略。
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引用次数: 0
Constriction-susceptible lithium support for fast cycling of solid-state lithium metal battery 用于固态锂金属电池快速循环的易收缩锂支持物
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-06 DOI: 10.1016/j.cclet.2024.110417
Dong Sui, Jiayi Liu
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引用次数: 0
Corrigendum to “Morphology controllable conjugated network polymers based on AIE-active building block for TNP detection” 基于 AIE 活性结构单元的形态可控共轭网络聚合物用于 TNP 检测 "的更正
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-05 DOI: 10.1016/j.cclet.2023.108998
Shan Jiang , Lingchen Meng , Wenyue Ma , Qingkai Qi , Wei Zhang , Bin Xu , Leijing Liu , Wenjing Tian
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引用次数: 0
Tuning the ion-dipole interactions between fluoro and carbonyl (EC) by electrolyte design for stable lithium metal batteries 通过电解质设计调谐氟和羰基(EC)之间的离子-偶极子相互作用,制造稳定的锂金属电池
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-03 DOI: 10.1016/j.cclet.2024.110385
Guihuang Fang , Ying Liu , Yangyang Feng , Ying Pan , Hongwei Yang , Yongchuan Liu , Maoxiang Wu
Ethylene carbonate (EC) is the conventional and promising solvent to achieve high energy lithium metal battery. However, the innate low energy level of lowest unoccupied molecular orbital (LUMO) in EC makes it incompatible with lithium metal, causing uncontrolled lithium growth and low Coulombic efficiency (CE). Herein, we introduced bis(2,2,2-trifluoroethyl) carbonate (TFEC), a carbonate with a strong electron-withdrawing effect (-CF3), which enhances the stability of EC at electrode interface by reducing ion-dipole interactions between Li+ and EC. As the interaction between Li and EC weakens, TFEC and more PF6 anions coordinate with Li⁺, promoting the formation of contact ion pairs (CIPs) and aggregates (AGGs), thereby increasing the inorganic composition within the solid electrolyte interphase. Additionally, the distinct solvated sheath structure favors the decomposition of fluorinated solvents and PF6− anions, forming inorganic-rich electrode-electrolyte interfaces (SEI and CEI), thereby ensuring high stability for both the Li anode and high-voltage cathode. Hence, when applied in the full-cell Li||LiMn0.8Fe0.2PO4, it displays consistent cycling performance, exhibiting minimal capacity decay with a retention rate of 62.5% after 800 cycles, substantially surpassing that of cells using base electrolytes (29.8%).
碳酸乙烯酯(EC)是实现高能锂金属电池的传统且前景广阔的溶剂。然而,碳酸乙烯酯中最低未占分子轨道(LUMO)的先天低能级使其与金属锂不相容,导致锂生长失控和库仑效率(CE)低下。在此,我们引入了双(2,2,2-三氟乙基)碳酸酯(TFEC),这是一种具有强电子抽离效应(-CF3)的碳酸酯,可通过减少 Li+ 与 EC 之间的离子-偶极子相互作用来增强 EC 在电极界面上的稳定性。随着 Li 和 EC 之间相互作用的减弱,TFEC 和更多的 PF6- 阴离子与 Li⁺配位,促进了接触离子对(CIP)和聚集体(AGG)的形成,从而增加了固体电解质间相中的无机成分。此外,独特的溶解鞘结构有利于氟化溶剂和 PF6- 阴离子的分解,形成富含无机物的电极-电解质界面(SEI 和 CEI),从而确保锂阳极和高压阴极的高稳定性。因此,当应用于全电池 Li||LiMn0.8Fe0.2PO4 时,它显示出稳定的循环性能,在 800 次循环后容量衰减极小,保持率为 62.5%,大大超过使用碱电解质的电池(29.8%)。
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引用次数: 0
Aqueous indium metal batteries 含水金属铟电池
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-03 DOI: 10.1016/j.cclet.2024.110407
Jingjing Zhang , Lan Ding , Vadim Popkov , Kezhen Qi
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引用次数: 0
Cucurbituril and cyclodextrin co-confinement-based multilevel assembly for single-molecule phosphorescence resonance energy transfer behavior 基于葫芦素和环糊精共聚的多级组装,实现单分子磷光共振能量转移行为
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-31 DOI: 10.1016/j.cclet.2024.110261
Siwei Wang , Wei-Lei Zhou , Yong Chen
{"title":"Cucurbituril and cyclodextrin co-confinement-based multilevel assembly for single-molecule phosphorescence resonance energy transfer behavior","authors":"Siwei Wang ,&nbsp;Wei-Lei Zhou ,&nbsp;Yong Chen","doi":"10.1016/j.cclet.2024.110261","DOIUrl":"10.1016/j.cclet.2024.110261","url":null,"abstract":"","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"35 12","pages":"Article 110261"},"PeriodicalIF":9.4,"publicationDate":"2024-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142097424","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
Detecting dynamic structural evolution based on in-situ high-energy X-ray diffraction technology for sodium layered oxide cathodes 基于原位高能 X 射线衍射技术检测钠层状氧化物阴极的动态结构演变
IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-31 DOI: 10.1016/j.cclet.2024.110389
Yan-Jiang Li, Shu-Lei Chou, Yao Xiao
The detrimental phase transformations of sodium layered transition metal oxides (NaxTMO2) during desodiation/sodiation seriously suppress their practical applications for sodium ion batteries (SIBs). Undoubtedly, comprehensively investigating of the dynamic crystal structure evolutions of NaxTMO2 associating with Na ions extraction/intercalation and then deeply understanding of the relationships between electrochemical performances and phase structures drawing support from advanced characterization techniques are indispensable. In-situ high-energy X-ray diffraction (HEXRD), a powerful technology to distinguish the crystal structure of electrode materials, has been widely used to identify the phase evolutions of NaxTMO2 and then profoundly revealed the electrochemical reaction processes. In this review, we begin with the descriptions of synchrotron characterization techniques and then present the advantages of synchrotron X-ray diffraction (XRD) over conventional XRD in detail. The optimizations of structural stability and electrochemical properties for P2-, O3-, and P2/O3-type NaxTMO2 cathodes through single/dual-site substitution, high-entropy design, phase composition regulation, and surface engineering are summarized. The dynamic crystal structure evolutions of NaxTMO2 polytypes during Na ion extraction/intercalation as well as corresponding structural enhancement mechanisms characterizing by means of HEXRD are concluded. The interior relationships between structure/component of NaxTMO2 polytypes and their electrochemical properties are discussed. Finally, we look forward the research directions and issues in the route to improve the electrochemical properties of NaxTMO2 cathodes for SIBs in the future and the combined utilizations of multiple characterization techniques. This review will provide significant guidelines for rational designs of high-performance NaxTMO2 cathodes.
钠层状过渡金属氧化物(NaxTMO2)在去阳极化/阳极化过程中的有害相变严重阻碍了其在钠离子电池(SIB)中的实际应用。毋庸置疑,全面研究 NaxTMO2 与 Na 离子萃取/插层相关的动态晶体结构演变,并在先进表征技术的支持下深入理解电化学性能与相结构之间的关系是必不可少的。原位高能 X 射线衍射(HEXRD)是一种区分电极材料晶体结构的强大技术,已被广泛用于识别 NaxTMO2 的相变,进而深刻揭示其电化学反应过程。在这篇综述中,我们首先介绍了同步辐射表征技术,然后详细介绍了同步辐射 X 射线衍射 (XRD) 相对于传统 XRD 的优势。总结了通过单/双位点置换、高熵设计、相组成调节和表面工程优化 P2-、O3- 和 P2/O3 型 NaxTMO2 阴极的结构稳定性和电化学性能。总结了 Na 离子萃取/插层过程中 NaxTMO2 多类型晶体结构的动态演变,以及通过 HEXRD 表征的相应结构增强机制。我们还讨论了 NaxTMO2 聚合物的结构/组分与其电化学特性之间的内部关系。最后,我们展望了未来改善用于 SIB 的 NaxTMO2 阴极电化学性能的研究方向和问题,以及多种表征技术的综合利用。本综述将为高性能 NaxTMO2 阴极的合理设计提供重要指导。
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Chinese Chemical Letters
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