IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-07-01 DOI: 10.1016/j.cjsc.2025.100620

Qiang Yu , Shuhan Sun , Xianming Jin , Ruiqiang Yan , Bingjing He , Nikolay Sirotkin , Alexander Agafonov , Xianqiang Xiong , Kangle Lv

The modulation of charge transfer pathways within type-I heterojunctions through interfacial electric field (IEF) engineering is of critical importance in promoting photocatalytic hydrogen evolution, effectively facilitating the separation of photogenerated charge carriers. In this study, we performed in-situ growth of two-dimensional ZnIn₂S₄ nanosheets on MnCo₂O_4.5 nanorods to construct an ohmic-like type-I ZnIn₂S₄/MnCo₂O_4.5 heterojunction for efficient photocatalytic hydrogen evolution. This ohmic-like charge transfer mechanism effectively addresses the intrinsic limitations inherent to conventional type-I heterojunctions neglecting IEF effects, particularly through IEF-induced enhancement of charge separation efficiency. Consequently, the optimized ZnIn₂S₄/MnCo₂O_4.5 photocatalyst demonstrates an outstanding photocatalytic hydrogen evolution rate of 20.9 mmol g⁻¹ h⁻¹, 14.9 times that of the bare ZnIn₂S₄. Furthermore, the ohmic-like charge transport behavior has been rigorously validated by integrated advanced experimental characterizations, including in-situ X-ray photoelectron spectroscopy (XPS), Kelvin probe force microscopy (KPFM), and surface photovoltage (SPV) measurements, which collectively provide robust evidence for the proposed mechanism. This work offers valuable insights into the design of high-efficient ohmic-like type-I heterojunction catalysts for photocatalytic H₂ evolution.

通过界面电场（IEF）工程调制i型异质结内的电荷转移途径对于促进光催化析氢，有效地促进光生载流子的分离具有至关重要的意义。在这项研究中，我们在MnCo2O4.5纳米棒上原位生长了二维ZnIn2S4纳米片，构建了一个类似欧姆的i型ZnIn2S4/MnCo2O4.5异质结，用于高效的光催化析氢。这种类欧姆电荷转移机制有效地解决了传统i型异质结忽略IEF效应的固有局限性，特别是通过IEF诱导的电荷分离效率的增强。结果表明，优化后的ZnIn2S4/MnCo2O4.5光催化剂的光催化析氢速率为20.9 mmol g−1 h−1，是裸ZnIn2S4的14.9倍。此外，类欧姆电荷输运行为已经通过集成的先进实验表征得到严格验证，包括原位x射线光电子能谱（XPS），开尔文探针力显微镜（KPFM）和表面光电压（SPV）测量，这些都为所提出的机制提供了有力的证据。这项工作为设计用于光催化氢演化的高效类欧姆i型异质结催化剂提供了有价值的见解。

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引用次数: 0

Four tartaric acid-bridged tetra-europium(III)-containing antimonotungstate with catalytic oxidation of thioethers/alcohols 四酒石酸桥接四铕（III）含反单钨酸盐与硫醚/醇的催化氧化

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-07-01 DOI: 10.1016/j.cjsc.2025.100603

Yuanping Jiang , Haoqi Liu , Jiawei Zhang , Luying Jiao, Xiaoling Lin, Fuhua Zhang, Guoping Yang

A novel tetra-europium(III)-containing antimonotungstate, Na_8.2[H₂N(CH₃)₂]₉[Na_10.8(tar)₄(H₂O)₂₀(Eu₂Sb₂W₂₁O₇₂)₂]·44.5H₂O (EuSbW, H₄tar = dl-tartaric acid), has been synthesized and characterized. The dimeric polyoxoanion of EuSbW consists of two Dawson-like {Eu₂Sb₂W₂₁} units bridged by four dl-tartaric acid ligands. The adjacent carboxyl and hydroxy groups in each tartaric acid simultaneously chelate with W and Eu atoms from different {Eu₂Sb₂W₂₁} units, thereby forming the dimeric structure. EuSbW represents an extremely rare polyoxometalate where four tartaric acid ligands function as connectors to bridge two {Eu₂Sb₂W₂₁} units. Additionally, EuSbW exhibits excellent catalytic activity and reusability in the oxidation of thioethers and alcohols, achieving 100% conversion and > 99% selectivity for various thioethers, and 85–100% conversion with 90–99% selectivity for diverse alcohols under mild conditions.

合成了一种新型的含四铕（III）反单钨酸盐Na8.2[H2N(CH3)2]9[Na10.8(tar)4(H2O)20(Eu2Sb2W21O72)2]·44.5H2O （EuSbW, H4tar = dl-酒石酸）。EuSbW的二聚多氧阴离子由四个dl-酒石酸配体桥接的两个Dawson-like单元组成。每个酒石酸中相邻的羧基和羟基同时与来自不同{Eu2Sb2W21}单元的W和Eu原子螯合，从而形成二聚体结构。EuSbW是一种极其罕见的多金属氧酸盐，其中四个酒石酸配体作为连接两个{Eu2Sb2W21}单元的连接器。此外，EuSbW在硫醚和醇的氧化中表现出优异的催化活性和可重复使用性，达到100%的转化率和>；对各种硫醚的选择性为99%，在温和条件下对各种醇的选择性为90-99%，转化率为85-100%。

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引用次数: 0

Photomechanical movements of a coordination polymer-based composite enable a reversible photocontrollable electrical switch 一种基于配位聚合物的复合材料的光电运动使可逆光可控电气开关成为可能

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-07-01 DOI: 10.1016/j.cjsc.2025.100622

Qian Ren , Shu-Fen Zhang , Dong Liu , Jian-Ping Lang

Flexible circuit switches have been widely used in electronic devices due to their outstanding flexibility and operability. In order to expand the types of flexible circuit switch materials, we develop a unique composite material, which integrates a photoresponsive flexible substrate derived from a photoreactive coordination polymer (CP) with an elastic conductive adhesive tape (CAT) in this work. The photoreactive CP {[Cd(2,6-bpvn)(3,5-DBB)₂]·DMF}_n (1) is prepared through solvothermal reaction of Cd(NO₃)₂·4H₂O with 2,6-bis((E)-2-(pyridin-4-yl)vinyl)naphthalene (2,6-bpvn) and 3,5-dibromobenzoic acid (3,5-HDBB). Upon irradiation with UV light, crystals of 1 can undergo [2 + 2] photocycloaddition reaction and exhibit photomechanical movements. The crystalline powder of 1 can be uniformly distributed in polyvinyl alcohol (PVA) to generate the composite film 1-PVA. After pasting a piece of CAT on the surface of a 1-PVA film, a conductive two-layer film of 1-PVA/CAT can be fabricated. This film bends rapidly upon UV light exposure, connecting the circuit and causing the bulb to light up. When the light source is removed, it reverts to its initial state and the circuit is disconnected and the bulb is extinguished. This process can be cycled at least 100 times, achieving precise turn-on and turn-off performances of the photocontrollable circuit switch.

柔性电路开关以其优异的灵活性和可操作性在电子器件中得到了广泛的应用。为了扩展柔性电路开关材料的类型，我们开发了一种独特的复合材料，该材料将光反应性配位聚合物（CP）衍生的光响应柔性衬底与弹性导电胶带（CAT）集成在一起。通过Cd(NO3)2·4H2O与2,6-双(（E)-2-（吡啶-4-基）乙烯基）萘（2,6-bpvn）和3,5-二溴苯甲酸（3,5- hdbb）溶剂热反应制备光反应物CP {[Cd(2,6-bpvn)(3,5- hdbb)2]·DMF}n(1)。在紫外光照射下，1的晶体可以发生[2 + 2]光环加成反应，并表现出光机械运动。将1的结晶粉末均匀分布在聚乙烯醇（PVA）中，生成1-PVA复合膜。在1-PVA薄膜表面粘贴一块CAT，就可以制成导电的1-PVA/CAT双层薄膜。这种薄膜在紫外线照射下迅速弯曲，连接电路并使灯泡发光。当光源移开时，它恢复到初始状态，电路断开，灯泡熄灭。该过程可循环至少100次，实现光可控电路开关的精确导通和关断性能。

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引用次数: 0

Structural regulation of alkynyl-based covalent organic frameworks for multi-stimulus fluorescence sensing 用于多刺激荧光传感的炔基共价有机框架的结构调控

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-07-01 DOI: 10.1016/j.cjsc.2025.100604

Xinrui Chen, Wenjian Huang, Xiaoyang Zhao, Songyao Zhang, Xinrui Miao

Stimuli-responsive two-dimensional (2D) covalent organic frameworks (COFs) with precise structures and permanent porosity have been employed as platforms for sensors. The slight change of backbones inside frameworks leads to different electronic states by external stimuli, such as solvent, pH, and water. Herein, we introduced an alkynyl-based building block (ETBA) with high planarity to synthesize two imine-based alkynyl-COFs (ETBA-TAPE-COF and ETBA-PYTA-COF) with high yield, good crystallinity, and chemical stability. Due to the presence of acetylene bonds, ETBA-TAPE-COF does not adopt the completely overlapping AA stacking mode. Slight interlayer displacement occurs along the parallel direction relative to the acetylene linkages, which facilitates lower configurational energy. Additionally, the introduction of pyrene group contributes to high π-electron mobility of ETBA-PYTA-COF. The interactions between electron-withdrawing group (ETBA) and electron-donating group (PYTA) during the processes of protonation and intramolecular charge transfer (ICT) endow ETBA-PYTA-COF with excellent acidochromic and solvatochromic properties, respectively. Based on this, a fluorescence sensor is successfully established, which can be used for rapid response to trace amounts of water in organic solvents. In contrast, ETBA-TAPE-COF does not exhibit these photophysical properties due to its higher HOMO–LUMO gap compared to ETBA-PYTA-COF. This work proposes a new strategy for designing and preparing COFs with unique photophysical properties without introducing additional functional groups.

具有精确结构和永久孔隙度的二维（2D）共价有机框架（COFs）已被用作传感器平台。骨架内部骨架的微小变化，在溶剂、pH、水等外界刺激下，会导致不同的电子状态。本文介绍了一种高平面度的炔基构建块（ETBA），用于合成两种产率高、结晶度好、化学稳定性好的亚胺基炔基cofs （ETBA- tape - cof和ETBA- pyta - cof）。由于乙炔键的存在，ETBA-TAPE-COF不采用完全重叠的AA堆叠模式。相对于乙炔键，沿平行方向发生轻微的层间位移，有利于降低构型能。此外，芘基团的引入使得ETBA-PYTA-COF具有较高的π电子迁移率。吸电子基（ETBA）和给电子基（PYTA）在质子化和分子内电荷转移（ICT）过程中的相互作用使ETBA-PYTA- cof分别具有优异的酸致变色和溶剂致变色性能。在此基础上，成功建立了一种荧光传感器，可用于对有机溶剂中微量水的快速响应。相比之下，ETBA-TAPE-COF由于具有比ETBA-PYTA-COF更高的HOMO-LUMO间隙而没有表现出这些光物理性质。本研究提出了一种设计和制备具有独特光物理性质的COFs而不引入额外官能团的新策略。

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引用次数: 0

Strategic metal substitution for enhanced visible-light-driven oxygen evolution in heterometallic MOFs 异质金属MOFs中增强可见光驱动析氧的战略性金属替代

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-07-01 DOI: 10.1016/j.cjsc.2025.100621

Cui Luo , Peng-Hui Li , Wei-Ming Liao , Qia-Chun Lin , Xiao-Xiang Zhou , Jun He

Oxygen evolution reaction (OER), a critical half-reaction in photocatalytic overall water splitting for producing hydrogen, is a key step toward sustainable energy conversion. Conventional photocatalysts often suffer from limited light absorption and rapid charge recombination, hindering their further applications. To address these challenges, we have designed and synthesized a novel series of self-sensitized metal-organic frameworks (MOFs), Fe₂MCDDB (M = Ni, Mn, or Co). By incorporating photosensitive ligands, we have achieved efficient charge separation and promoted the transfer of photogenerated electrons to the active metal sites for water oxidation. Among the series, Fe₂NiCDDB exhibits exceptional OER activity, achieving an oxygen evolution rate of 125.3 μmol g⁻¹ h⁻¹ under visible light irradiation. Experimental and theoretical results reveal that the optimized electronic structure and prolonged excited-state lifetime of Fe₂NiCDDB contribute to its enhanced catalytic performance. This work provides a promising strategy for designing two-in-one MOF photocatalysts for water oxidation.

析氧反应（OER）是光催化全水裂解制氢的关键半反应，是实现可持续能源转化的关键一步。传统的光催化剂往往存在光吸收有限和电荷重组速度快的问题，阻碍了其进一步的应用。为了应对这些挑战，我们设计并合成了一系列新颖的自敏金属有机框架（MOFs）， Fe2MCDDB （M = Ni， Mn或Co）。通过加入光敏配体，我们实现了有效的电荷分离，并促进了光生电子转移到活性金属位进行水氧化。其中Fe2NiCDDB表现出优异的OER活性，在可见光照射下析氧速率达到125.3 μmol g−1 h−1。实验和理论结果表明，优化的电子结构和延长的激发态寿命是Fe2NiCDDB催化性能增强的原因之一。本研究为设计二合一MOF水氧化光催化剂提供了一种有前景的策略。

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引用次数: 0

Nickel phosphide modified TiO2 nanotube arrays for efficient PEC water splitting H2 generation 磷化镍修饰TiO2纳米管阵列用于高效PEC水裂解制氢

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-07-01 DOI: 10.1016/j.cjsc.2025.100623

Yang Yang , Yan-Xin Chen , Ao-Sheng She , Hao-Yan Shi , Wen Chen , Wei Wang , Hai-Long Wang , Ke-Xian Li , Yi-Hu Pu , Wei-Hua Yang , Xiu-Mei Lin , Can-Zhong Lu

Photoelectrochemical (PEC) hydrogen production holds great promise for applications in energy production. A novel strategy characterized by simplicity, stability, and high efficiency is developed to significantly boost the PEC performance of TiO₂ (anatase) nanotube arrays (TNTAs). This strategy entails a series of treatments, including a conventional anodic oxidation (etching) process, a primary annealing treatment, and a secondary annealing treatment via impregnation. As a result, nickel phosphide (Ni₂P) is composited onto well-ordered titanium dioxide (anatase) nanotube array photoanodes (Ni₂P/TNTAs), which exhibit hugely improved PEC H₂ generation performance. A thorough and systematic investigation is conducted to comprehensively analyze the morphology, semiconductor band-gap structure, and PEC H₂ production performance of the Ni₂P/TNTAs composites. The experimental results demonstrate that under identical experimental circumstances, the measured photocurrent density of the Ni₂P/TNTAs photoanode exhibits a 6.63-fold increase relative to that of TNTAs. The H₂ production rate of Ni₂P/TNTAs reaches 182.96 μmol/cm², 6.10 times higher than that of pure TNTAs. The excellent interfacial charge transfer pathway at the Ni₂P/TiO₂ interface promotes photogenerated carrier separation and electron transfer from TiO₂ to Ni₂P. This method offers a valuable reference for designing highly efficient PEC H₂-production catalysts.

光电化学制氢在能源生产中具有广阔的应用前景。本文提出了一种简单、稳定、高效的纳米TiO2（锐钛矿）纳米管阵列（TNTAs）电化学性能的新方法。该策略需要一系列处理，包括传统的阳极氧化（蚀刻）工艺，一次退火处理和浸渍二次退火处理。结果表明，将磷化镍（Ni2P）复合到有序的二氧化钛（锐钛矿）纳米管阵列光阳极（Ni2P/TNTAs）上，大大提高了PEC制氢性能。对Ni2P/TNTAs复合材料的形貌、半导体带隙结构和PEC制氢性能进行了全面、系统的研究。实验结果表明，在相同的实验条件下，Ni2P/TNTAs光阳极的测量光电流密度相对于TNTAs增加了6.63倍。Ni2P/ tnta的H2产率达到182.96 μmol/cm2，是纯tnta的6.10倍。Ni2P/TiO2界面处优良的界面电荷转移途径促进了光生载流子分离和电子从TiO2向Ni2P的转移。该方法为设计高效PEC制h2催化剂提供了有价值的参考。

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引用次数: 0

Functionally graded materials based on porous poly(ionic liquid)s: Design strategies and applications 基于多孔多离子液体的功能梯度材料：设计策略与应用

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-07-01 DOI: 10.1016/j.cjsc.2025.100601

Xiao-Yu Han , Si-Hua Liu , Su-Yun Zhang , Jian-Ke Sun

Functionally graded materials (FGMs) are innovative materials distinguished by gradual variations in composition and structure, offering exceptional properties for diverse applications. Poly(ionic liquid)s (PILs), merging the characteristics of polymers and ionic liquids, have emerged as viable options for the development of FGMs given their tunable skeleton, ionic conductivity, and compatibility with various functional materials. This review highlights the latest advancements in the design strategies of FGMs based on porous PILs, focusing on single and multi-gradient structures. Furthermore, we also highlight their emerging applications in molecular recognition, sensing, adsorption, separation, and catalysis. By exploring the interplay between porosity, ionic functionality, and gradient architecture, this review offers perspectives on the prospects of PIL-based FGMs for tackling global challenges in energy, environment, and healthcare.

功能梯度材料（fgm）是一种创新材料，其特点是成分和结构的逐渐变化，为各种应用提供了卓越的性能。聚离子液体（PILs）融合了聚合物和离子液体的特性，由于其可调节的骨架、离子电导率和与各种功能材料的相容性，已成为发展fgm的可行选择。本文综述了基于多孔PILs的fgm设计策略的最新进展，重点介绍了单梯度和多梯度结构。此外，我们还重点介绍了它们在分子识别、传感、吸附、分离和催化等方面的新兴应用。通过探索孔隙度、离子功能和梯度结构之间的相互作用，本文综述了基于pil的fgm在解决能源、环境和医疗保健方面的全球挑战方面的前景。

引用次数: 0

Neodymium-doped hollow Ir/IrO2 nanospheres with low geometric iridium density enable excellent acidic water oxidation performance 具有低几何铱密度的掺钕空心Ir/IrO2纳米球具有优异的酸性水氧化性能

IF 10.3 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-07-01 DOI: 10.1016/j.cjsc.2025.100600

Xiaoqian Wei , Hanyu Gao , Tiantian Wang , Zijian Li , Yanru Geng , Guiping Zheng , Min Gyu Kim , Haeseong Jang , Xien Liu , Qing Qin

Reducing the Ir loading while preserving catalytic performance and mechanical robustness in anodic catalyst layers remains a critical challenge for the large-scale implementation of proton exchange membrane water electrolysis (PEMWE). Herein, we present a structural engineering strategy involving neodymium-doped Ir/IrO₂ (Nd–Ir/IrO₂) hollow nanospheres with precisely adjustable shell thickness and cavity dimensions. The optimized catalyst demonstrates excellent oxygen evolution reaction (OER) performance in acidic media, achieving a remarkably low overpotential of 259 mV at a benchmark current density of 10 mA cm⁻² while exhibiting substantially enhanced durability compared to commercial IrO₂ and Ir/IrO₂ counterparts. Notably, the Nd–Ir/IrO₂ catalyst delivers a mass activity of 541.6 A g_Ir⁻¹ at 1.50 V vs. RHE, representing a 74.5-fold enhancement over conventional IrO₂. Comprehensive electrochemical analysis and advanced characterization techniques reveal that the hierarchical hollow architecture simultaneously addresses multiple critical requirements: (i) abundant exposed active sites enabled by an enhanced electrochemical surface area, (ii) optimized mass transport pathways through engineered porosity, and (iii) preserved structural integrity via a continuous conductive framework, collectively enabling significant Ir loading reduction without compromising catalytic layer performance. Fundamental mechanistic investigations further disclose that Nd doping induces critical interfacial Nd–O–Ir configurations that stabilize lattice oxygen, together with intensified electron effect among mixed valent Ir that inhibits the overoxidation of Ir active sites during the OER process, synergistically ensuring enhanced catalytic durability. Our work establishes a dual-modulation paradigm integrating nanoscale architectural engineering with atomic-level heteroatom doping, providing a viable pathway toward high-performance PEMWE systems with drastically reduced noble metal requirements.

减少Ir负载，同时保持阳极催化剂层的催化性能和机械稳健性，仍然是大规模实施质子交换膜电解（PEMWE）的关键挑战。在此，我们提出了一种结构工程策略，涉及钕掺杂Ir/IrO2 （Nd-Ir /IrO2）空心纳米球，具有精确可调的壳厚度和腔尺寸。优化后的催化剂在酸性介质中表现出优异的析氧反应（OER）性能，在10 mA cm - 2的基准电流密度下实现了259 mV的过电位，同时与商用IrO2和Ir/IrO2相比，具有显著增强的耐久性。值得注意的是，与RHE相比，Nd-Ir /IrO2催化剂在1.50 V下的质量活性为541.6 a gIr−1，比传统IrO2提高了74.5倍。综合电化学分析和先进的表征技术表明，分层中空结构同时满足多个关键要求：(i)通过增强电化学表面积实现丰富的暴露活性位点，（ii）通过工程孔隙优化质量传输途径，（iii）通过连续导电框架保持结构完整性，共同实现显著的Ir负载减少而不影响催化层性能。基础机理研究进一步揭示，Nd掺杂诱导了稳定晶格氧的关键界面Nd - o - Ir构型，以及混合价Ir之间增强的电子效应，抑制了OER过程中Ir活性位点的过度氧化，协同确保了增强的催化耐久性。我们的工作建立了一种将纳米级结构工程与原子级杂原子掺杂相结合的双调制范式，为大幅降低贵金属需求的高性能PEMWE系统提供了一条可行的途径。

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引用次数: 0

A shape-memory hydrogen-bonded organic framework for flue gas desulfurization 一种用于烟气脱硫的形状记忆氢键有机骨架

IF 5.9 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-06-01 DOI: 10.1016/j.cjsc.2025.100574

Wenlei Yang, Lingyao Wang, Yuanbin Zhang

引用次数: 0

Investigation of water structure and proton transfer within confined graphene by ab initio molecule dynamics and multiscale data analysis 用从头算分子动力学和多尺度数据分析研究石墨烯中水结构和质子转移

IF 5.9 4区化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR

结构化学

Pub Date : 2025-06-01 DOI: 10.1016/j.cjsc.2025.100596

Heng-Su Liu , Xi-Ming Zhang , Ge-Hao Liang , Shisheng Zheng , Jian-Feng Li

The structure of water and proton transfer under nanoscale confinement has garnered significant attention due to its crucial role in elucidating various phenomena across multiple scientific disciplines. However, there remains a lack of consensus on fundamental properties such as diffusion behavior and the nature of hydrogen bonding in confined environments. In this work, we investigated the influence of confinement on proton transfer in water confined within graphene sheets at various spacings by ab initio molecule dynamic and multiscale analysis with time evolution of structural properties, graph theory and persistent homology. We found that reducing the graphene interlayer distance while maintaining water density close to that of bulk water leads to a decrease in proton transfer frequency. In contrast, reducing the interlayer distance without maintaining bulk-like water density results in an increase in proton transfer frequency. This difference is mainly due to the confinement conditions: when density is unchanged, the hydrogen bond network remains similar with significant layering, while compressive stress that increases density leads to a more planar hydrogen bond network, promoting faster proton transfer. Our findings elucidate the complex relationship between confinement and proton transfer dynamics, with implications for understanding proton transport in confined environments, relevant to energy storage and material design.

纳米尺度约束下的水和质子转移结构由于其在解释多个学科的各种现象方面的重要作用而引起了人们的广泛关注。然而，在诸如扩散行为和氢键在密闭环境中的性质等基本性质上，仍然缺乏共识。在这项工作中，我们通过从头算分子动力学和多尺度分析，结合结构性质的时间演化，图论和持续同源性，研究了限制对不同间距的石墨烯片内水中质子转移的影响。我们发现，在减少石墨烯层间距离的同时，保持水的密度接近于水的密度，会导致质子转移频率的降低。相反，在不保持体积水密度的情况下减小层间距离会导致质子转移频率增加。这种差异主要是由约束条件造成的：当密度不变时，氢键网络保持相似，分层明显，而增加密度的压应力导致氢键网络更加平面，促进质子更快转移。我们的研究结果阐明了约束和质子转移动力学之间的复杂关系，对理解约束环境中的质子传输具有重要意义，与能量存储和材料设计有关。

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引用次数: 0

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