Chinese Chemical Letters最新文献

英文中文

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

Chinese Chemical Letters

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 PF_6⁻ 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||LiMn_0.8Fe_0.2PO₄, 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

Chinese Chemical Letters

Pub Date : 2024-09-03 DOI: 10.1016/j.cclet.2024.110407

Jingjing Zhang , Lan Ding , Vadim Popkov , Kezhen Qi

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

Chinese Chemical Letters

Pub Date : 2024-08-31 DOI: 10.1016/j.cclet.2024.110261

Siwei Wang , Wei-Lei Zhou , Yong Chen

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

Chinese Chemical Letters

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 (Na_xTMO₂) during desodiation/sodiation seriously suppress their practical applications for sodium ion batteries (SIBs). Undoubtedly, comprehensively investigating of the dynamic crystal structure evolutions of Na_xTMO₂ 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 Na_xTMO₂ 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 Na_xTMO₂ cathodes through single/dual-site substitution, high-entropy design, phase composition regulation, and surface engineering are summarized. The dynamic crystal structure evolutions of Na_xTMO₂ 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 Na_xTMO₂ 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 Na_xTMO₂ 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 Na_xTMO₂ 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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引用次数: 0

Interface engineering of Pt/CeO2-{100} catalysts for enhancing catalytic activity in auto-exhaust carbon particles oxidation 铂/CeO2-{100}催化剂的界面工程以提高汽车尾气碳颗粒氧化的催化活性

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-08-31 DOI: 10.1016/j.cclet.2024.110396

Peng Zhang , Yitao Yang , Tian Qin , Xueqiu Wu , Yuechang Wei , Jing Xiong , Xi Liu , Yu Wang , Zhen Zhao , Jinqing Jiao , Liwei Chen

Herein, we fabricate an embedding structure at the interface between Pt nanoparticles (NPs) and CeO₂-{100} nanocubes with surface defect sites (CeO₂-SDS) through quenching and gas bubbling-assisted membrane reduction methods. The in-situ substitution of Pt NPs for atomic-layer Ce lattice significantly increases the amount of reactive oxygen species from 133.68 µmol/g to 199.44 µmol/g. As a result, the distinctive geometric structure of Pt/CeO₂-SDS catalyst substantially improves the catalytic activity and stability for soot oxidation compared with the catalyst with no quenching process, i.e., its T₅₀ and TOF values are 332 °C and 2.915 h^-1, respectively. Combined with the results of experimental investigations and density functional theory calculations, it is unveiled that the unique embedding structure of Pt/CeO₂-SDS catalyst can facilitate significantly electron transfer from Pt to the CeO₂-{100} support, and induce the formation of interfacial [Ce-O_x-Pt₂] bond chains, which plays a crucial role in enhancing the key step of soot oxidation through the dual activation of surface lattice oxygen and molecular O₂. Such a fundamental revelation of the interfacial electronic transmission and corresponding modification strategy contributes a novel opportunity to develop high-efficient and stable noble metal catalysts at the atomic level.

在此，我们通过淬火法和气泡辅助膜还原法在铂纳米粒子（NPs）和具有表面缺陷位点的 CeO2-{100} 纳米立方体（CeO2-SDS）之间的界面上制造了一种嵌入结构。原子层 Ce 晶格原位取代铂 NPs 后，活性氧的含量从 133.68 µmol/g 显著增加到 199.44 µmol/g。因此，与没有淬火过程的催化剂相比，Pt/CeO2-SDS 催化剂独特的几何结构大大提高了烟尘氧化的催化活性和稳定性，即其 T50 值和 TOF 值分别为 332 °C 和 2.915 h-1。结合实验研究和密度泛函理论计算的结果，揭示了 Pt/CeO2-SDS 催化剂独特的嵌入结构能显著促进电子从 Pt 向 CeO2-{100} 载体转移，并诱导形成界面 [Ce-Ox-Pt2] 键链，通过表面晶格氧和分子 O2 的双重活化，在增强烟尘氧化的关键步骤中发挥了至关重要的作用。从根本上揭示了界面电子传输和相应的改性策略，为在原子水平上开发高效稳定的贵金属催化剂提供了新的机遇。

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引用次数: 0

Design and fabrication of triangle-pattern superwettability hybrid surface with high-efficiency condensation heat transfer performance

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-08-31 DOI: 10.1016/j.cclet.2024.110395

Rui Wang , Yuan Tian , Xuefeng Gao , Lei Jiang

Utilizing superwettability micro/nanostructures to enhance the condensation heat transfer (CHT) performance of engineering materials has attracted great interest due to its values in basic research and technological innovations. Currently, exploring facile micro/nanofabrication approaches to create high-efficiency CHT surfaces has been one of research hotspots. In this work, we propose and demonstrate a type of new superwettability hybrid surface for high-efficiency CHT, which consists of superhydrophobic nanoneedle arrays and triangularly-patterned superhydrophilic microdots (SMDs). Such hybrid surface can be fabricated by the facile growth of densely-packed ZnO nanoneedles on the Zn-electroplated copper surface followed by fluorosilane modification and mask-assisted photodegradation. Through regulating the diameters and interspaces of SMDs, we obtain the optimized triangularly-patterned hybrid surface, which shows 42.7 % higher CHT coefficient than the squarely-patterned hybrid surface and 58.5 % higher CHT coefficient than the superhydrophobic surface. The key of such hybrid surface design is to considerably increase CHT coefficient brought about by SMD-triggered drop sweeping at the cost of slightly reducing heat transfer area of superhydrophobic functional zone for drop jumping. Such new strategy helps develop advanced CHT surfaces for high-efficiency electronic cooling and energy utilization.

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引用次数: 0

MOF-derived NiCo bimetallic cocatalyst for enhanced photocatalytic overall water splitting

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-08-31 DOI: 10.1016/j.cclet.2024.110397

Liang Dong, Jingkuo Qu, Tuo Zhang, Guanghui Zhu, Ningning Ma, Chang Zhao, Yi Yuan, Xiangjiu Guan, Liejin Guo

The development of stable and efficient non-noble metal cocatalysts has arisen as a promising yet challenging endeavor in the context of photocatalytic overall water splitting. In this study, NiCo alloy cocatalysts were synthesized with nickel/cobalt metal organic framework (NiCo-MOF) as source of nickel and cobalt. Systematic characterization results demonstrate the successful deposition of alloy cocatalysts onto the surface of SrTiO₃. The prepared SrTiO₃ loaded NiCo-alloy can generate hydrogen and oxygen in a stoichiometric ratio for photocatalytic overall water splitting, achieving an apparent quantum yield of 11.9% at 350 ± 10 nm. Theoretical calculations indicate that the introduction of cobalt has a beneficial regulatory effect on the hydrogen evolution sites of Ni, reducing the free energy of H adsorption. The synergistic catalytic effect of bimetallic catalysts contributes to enhancing photocatalytic activity and stability. This study offers constructive insights for the development of high-efficiency and cost-effective cocatalyst systems.

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引用次数: 0

Preparing sub-monolayer metals with continuous coverage spread for high-throughput growth of metal-organic frameworks

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-08-31 DOI: 10.1016/j.cclet.2024.110394

Jiayi Lu, Yizhang Li, Hao Jiang, Zhiwen Zhu, Fengru Zheng, Qiang Sun

Surface-confined metal-organic frameworks have emerged as versatile structures with a broad spectrum of applications such as nanoelectronics, catalysis, sensing, and molecular storage, owing to their unique structural and electronic properties. However, the exploration and optimization of molecular networks typically involve resource-intensive trial-and-error experiments. The complexity comes from factors like metal nodes, organic ligands, substrates, and the preparation conditions. To address this challenge, high-throughput methodologies have been used in materials exploration. In this work, we explored a high-throughput method for preparing sub-monolayer metals with continuous coverage spread on metal surfaces. By employing a physical mask during metal deposition under ultra-high vacuum conditions, we achieved sample libraries with copper (Cu) and silver (Ag) adatoms on the metal substrates, and constructed surface-supported metal-organic frameworks with varying metal-to-molecule stoichiometric ratios. This approach facilitates the exploration of surface-confined metal-organic frameworks, particularly in terms of varying metal-to-ligand stoichiometric ratios, offering an efficient pathway to unlock the potential of these intricate two-dimensional networks.

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Targeting novel sites represents an effective strategy for combating drug resistance 靶向新位点是对抗耐药性的有效策略

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-08-30 DOI: 10.1016/j.cclet.2024.110378

Shaoqing Du , Xinyong Liu , Xueping Hu , Peng Zhan

引用次数: 0

Topologically close-packed intermetallic alloy electrocatalysts for CO2 reduction towards high value-added multi-carbon chemicals 拓扑紧密堆积金属间合金电催化剂，用于还原二氧化碳，生产高附加值多碳化学品

IF 9.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters

Pub Date : 2024-08-30 DOI: 10.1016/j.cclet.2024.110384

Qiyan Wu, Qing Li

引用次数: 0

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