Carbon最新文献_第4页

Autonomous adhesion enhancement of two-dimensional materials driven by interfacial evolution 界面演化驱动的二维材料自主粘附增强

IF 11.6 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2026-03-05 Epub Date: 2026-02-06 DOI: 10.1016/j.carbon.2026.121355

Haojie Lang , Peipei Xu , Nannan Xia , Cong Li , Haoyang Su , Ruling Chen , Yao Huang , Kun Zou , Yitian Peng

Adhesion is a fundamental property of two-dimensional (2D) materials due to their intrinsic ultrahigh surface-to-volume ratio, making adhesion very strong in many processes related to fabrication, integration, and performance of devices incorporating 2D materials. Here, time-dependent adhesion between 2D materials, including graphene, molybdenum disulfide, and hexagonal boron nitride, and silicon dioxide is investigated. The logarithmic increase in adhesion with contact time is attributed to the out-of-plane deformation of the topmost layer of 2D materials, which surpasses interlayer interactions, as revealed by van der Waals force calculations and density functional theory calculations of interfacial binding energy. Over time, the topmost layer spontaneously conforms to the contact surface, resulting in enhanced adhesion. Additionally, adhesion enhancement accelerates in high relative humidity environments, as the hydrogen bonding of water molecules strengthens the interfacial interaction. These studies based on experimental characterizations and computational analysis reveal that the adhesion of 2D materials is dynamic and can autonomously increase over time, driven by van der Waals force-induced interfacial evolution. This dynamic adhesion behavior is critical for the design and performance of 2D material-based electronic devices, lubricating coatings, sensors, and related applications.

附着力是二维（2D）材料的基本特性，由于其固有的超高表面体积比，使得附着力在许多与制造、集成和包含2D材料的器件性能相关的过程中非常强。本文研究了石墨烯、二硫化钼和六方氮化硼等二维材料与二氧化硅之间的时间依赖性粘附。根据范德华力计算和界面结合能的密度泛函理论计算，黏附力随接触时间的对数增长归因于二维材料最上层的面外变形，这种变形超过了层间的相互作用。随着时间的推移，最上层会自发地与接触面保持一致，从而增强附着力。此外，在相对湿度较高的环境中，由于水分子的氢键加强了界面相互作用，附着力增强的速度加快。这些基于实验表征和计算分析的研究表明，在范德华力诱导的界面演化的驱动下，二维材料的粘附是动态的，可以随时间自主增加。这种动态粘附行为对于基于二维材料的电子器件、润滑涂层、传感器和相关应用的设计和性能至关重要。

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引用次数: 0

High-yield inner-outer wall separation of double-wall carbon nanotubes via Nafion-temperature synergistic modulation 纳米温度协同调制双壁碳纳米管的高产率内外壁分离

IF 11.6 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2026-03-05 Epub Date: 2026-01-31 DOI: 10.1016/j.carbon.2026.121323

Dehua Yang , Xiaofei Yang , Donghui Zhang , Xuan Chang , Jiayi Xing , Qing Gao , Xuning Zhang , Xueliang Yang , Jianxin Guo , Wei Xi , Huaping Liu , Jianhui Chen

Double-wall carbon nanotubes (DWCNTs) offer promising properties for electronics and photovoltaics, and exhibit unique physical properties distinct from single-wall carbon nanotubes (SWCNTs). However, both fundamental and applied research on DWCNTs have been limited by the lack of scalable methods for producing high-purity DWCNTs with uniform electronic type. Here, we report a high-yield separation method based on Nafion-assisted, temperature-controlled selective adsorption chromatography. Using this strategy, S@S, M@S, S@M, and M@M DWCNTs were obtained with a total yield of 58 mg per batch from mixed SWCNT/DWCNT samples. We further evaluated the separation purity of inner and outer walls. The outer-wall purities exceeded 95% for S@S and 98% for the other three types, with inner-wall purities of 90% (S@S), 88% (M@S), 81% (S@M), and 92% (M@M). In this method, Nafion-induced selective protonation creates electronic-type-dependent differences in surface charge and surfactant coverage, and elevated temperature further enhances this Nafion-induced effect, thus amplifying the differences in surfactant coverage of various DWCNTs and enabling precise control of their selective adsorption onto gel. This work marks a major advance towards scalable preparation of high-purity DWCNTs with identical electronic type and demonstrates the advantage of selective adsorption chromatography for their separation. It lays the groundwork for inner/outer wall chirality resolution and future studies on DWCNT properties and device applications.

双壁碳纳米管（DWCNTs）具有不同于单壁碳纳米管（SWCNTs）的独特物理特性，在电子和光伏领域具有广阔的应用前景。然而，由于缺乏可扩展的方法来制备具有均匀电子型的高纯度DWCNTs，对DWCNTs的基础研究和应用研究都受到了限制。在这里，我们报告了一种基于nafion辅助、温度控制的选择性吸附色谱的高产率分离方法。使用该策略，从SWCNT/DWCNT混合样品中获得了S@S、M@S、S@M和M@M DWCNTs，每批总收率为58 mg。我们进一步评价了内外壁的分离纯度。其中，S@S的外壁纯度超过95%，其余三种均超过98%，内壁纯度分别为90% （S@S）、88% （M@S）、81% （S@M）、92% （M@M）。在该方法中，nafion诱导的选择性质子化产生了电子类型依赖的表面电荷和表面活性剂覆盖的差异，升高的温度进一步增强了nafion诱导的这种效应，从而放大了各种DWCNTs表面活性剂覆盖的差异，并能够精确控制它们在凝胶上的选择性吸附。这项工作标志着在可扩展制备具有相同电子类型的高纯度DWCNTs方面取得了重大进展，并证明了选择性吸附色谱法对其分离的优势。它为小碳纳米管的内/外壁手性分辨率和未来小碳纳米管性质和器件应用的研究奠定了基础。

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引用次数: 0

Advances on multi-heteroatom doped carbon catalysts: Synthesis, mechanistic insight, synergies, and application in microbial electrochemical energy, fuel and chemical production 多杂原子掺杂碳催化剂的合成、机理、协同作用及其在微生物电化学能源、燃料和化工生产中的应用研究进展

IF 11.6 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2026-03-05 Epub Date: 2026-02-03 DOI: 10.1016/j.carbon.2026.121315

Seyed Masoud Parsa , Seyed Mohammad Reza Miraboutalebi , Shahin Shoeibi , Xinbo Zhang , Jixiang Li , Huu Hao Ngo , Wenshan Guo , Bing-Jie Ni

Multi-heteroatom doping strategy emerged as a promising approach to overcome the limitations of carbon electrocatalysts through providing synergistic effects to tune electronic structures, increase/optimize active sites, improve stability, enhance biocompatibility and conductivity. This review provides a comprehensive analysis on progress in multi-heteroatom doped carbon electrocatalysts in microbial electrochemical technologies (METs) for wastewater treatment toward power generation, biohydrogen production, and CO₂ valorization through microbial fuel cells (MFCs), microbial electrolysis cells (MECs), and microbial electrosynthesis (MESs) respectively. Initially, the synthesis strategies from template-free pyrolysis and templating methods to advance MOF-derived and self-sacrificial routes were briefly summarized. Following, mechanistic insights by focusing on integration of advanced theoretical calculations and operando characterizations to understand how multi-doping tailor adsorption energies, charge redistribution, and intermediate stabilization in key electrocatalytic reactions such as the oxygen reduction reaction (ORR), hydrogen evolution reaction (HER), and CO₂ reduction reaction (CO₂RR) were thoroughly elucidated. Importantly, the structure–function relationships that link dopant type, coordination environment, and defect engineering with catalytic activity, durability, and selectivity were further elaborated. Finally, the current challenges and future research directions for designing advanced high-performance electrocatalysts toward sustainable practical METs were suggested.

多杂原子掺杂策略通过提供协同效应来调整电子结构，增加/优化活性位点，提高稳定性，增强生物相容性和导电性，是克服碳电催化剂局限性的一种很有前途的方法。本文综述了多杂原子掺杂碳电催化剂在微生物电化学技术（METs）中的研究进展，这些技术分别用于微生物燃料电池（mfc）、微生物电解电池（MECs）和微生物电合成（MESs）的废水发电、生物制氢和二氧化碳气化处理。首先，简要总结了从无模板热解和模板法到推进mof衍生和自我牺牲路线的合成策略。随后，通过将先进的理论计算和operando表征相结合，深入了解了多掺杂如何在氧还原反应（ORR）、析氢反应（HER）和CO2还原反应（CO2RR）等关键电催化反应中调整吸附能、电荷重分配和中间稳定的机理。重要的是，进一步阐述了掺杂类型、配位环境和缺陷工程与催化活性、耐久性和选择性之间的结构-功能关系。最后，提出了面向可持续实用METs的高性能电催化剂设计面临的挑战和未来的研究方向。

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引用次数: 0

Selective homoepitaxial growth of buried diamond films with NV centers 具有NV中心的埋藏金刚石薄膜的选择性同外延生长

IF 11.6 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2026-03-05 Epub Date: 2026-01-29 DOI: 10.1016/j.carbon.2026.121307

K. Hayashi , Y. Nakamura , M. Katayama , K. Shimamura , R. Yoshida , K. Kobayashi , K. Ichikawa , T. Yoshikawa , T. Matsumoto , T. Inokuma , S. Yamasaki , C.E. Nebel , N. Tokuda

We develop a buried-growth process for NV centers based on microwave plasma chemical vapor deposition that integrates selective etching and growth in a single process. Au/Ti metal masks patterned on (100) and (111) diamond substrates define micrometer-scale regions where the diamond is selectively etched by an H₂+N₂ plasma, followed by local CVD growth of NV-doped diamond within the etched regions, thereby enabling selective buried formation of NV centers. Confocal fluorescence imaging shows that NV centers are selectively buried in patterned regions on both (100) and (111) diamonds. Optically detected magnetic resonance under a static field applied from the backside of the substrates reveals that highly aligned NV centers are formed in the buried regions of the (111) diamond. X-ray diffraction measurements indicate the formation of Ti₂N at the Au/Ti/diamond during H₂+N₂ plasma processing, which we identify as the origin of the improved hydrogen resistance. The CVD diamond-layer buried-growth process demonstrated here provides a robust and versatile route to selectively buried NV centers and is readily extendable to buried doped layers for future diamond-based electronic and quantum devices.

我们开发了一种基于微波等离子体化学气相沉积的NV中心埋地生长工艺，该工艺将选择性蚀刻和生长集成在一个过程中。（100）和（111）金刚石衬底上的Au/Ti金属掩模定义了微米尺度的区域，其中金刚石被H2+N2等离子体选择性蚀刻，然后在蚀刻区域内局部CVD生长掺杂NV的金刚石，从而实现选择性埋藏形成NV中心。共聚焦荧光成像显示NV中心选择性地埋藏在（100）和（111）钻石的图案区域中。从衬底背面施加静态场下的光学检测磁共振显示，在（111）金刚石的埋藏区域形成了高度排列的NV中心。x射线衍射测量表明，在H2+N2等离子体处理过程中，在Au/Ti/金刚石处形成了Ti2N，我们认为这是提高抗氢性能的原因。本文所展示的CVD金刚石层埋地生长工艺为选择性埋地NV中心提供了一种稳健和通用的途径，并且很容易扩展到未来基于金刚石的电子和量子器件的埋地掺杂层。

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引用次数: 0

Film-type carbon nanotube thermal interface materials for advanced thermal management: A study on interfacial resistance 用于高级热管理的薄膜型碳纳米管热界面材料：界面阻力研究

IF 11.6 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2026-02-20 Epub Date: 2026-01-17 DOI: 10.1016/j.carbon.2026.121288

Tomoki Okumura , Takayuki Nakano , Yoku Inoue

Carbon nanotubes (CNTs) possess high thermal conductivity and mechanical flexibility, making them promising candidates for thermal interface materials (TIMs) for high-density heat-generating components requiring heat dissipation solutions. In this study, we fabricated a film-type CNT-TIM by sandwiching a thin polyphenylene sulfide (PPS) film between two opposing CNT forests. The transient thermal response, analyzed using the thermal structure function, revealed a low thermal resistance of 0.7 cm²K/W at a contact pressure of 100 kPa, including the interfacial contact thermal resistance with the heat source and heat sink. This performance is comparable to TIMs with CNTs grown directly on both sides of Cu or Al foils, and to conventional thermal grease. These results indicate that the thermal resistance of the contact interface is the dominant factor over the bulk material. The CNT-TIM with the PPS interlayer demonstrated a stable and robust solid-state TIM as a substitute for thermal grease. This research offers an effective manufacturing process to advance the practical application of CNT-based TIMs.

碳纳米管（CNTs）具有高导热性和机械灵活性，使其成为需要散热解决方案的高密度发热部件的热界面材料（TIMs）的有希望的候选者。在这项研究中，我们通过将一层薄薄的聚苯硫醚（PPS）薄膜夹在两个相对的碳纳米管林中来制备薄膜型碳纳米管tim。利用热结构函数分析瞬态热响应，发现在接触压力为100 kPa时，热阻较低，为0.7 cm2K/W，包括与热源和散热器的界面接触热阻。这种性能与直接在Cu或Al箔两侧生长碳纳米管的TIMs以及传统的导热润滑脂相当。这些结果表明，接触界面的热阻是块体材料的主要因素。具有PPS中间层的CNT-TIM证明了一种稳定而坚固的固态TIM作为导热脂的替代品。本研究为推进碳纳米管基TIMs的实际应用提供了一种有效的制造工艺。

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引用次数: 0

Design and synthesis of core-shell Fe4N@C nanowires for efficient electromagnetic wave absorption and corrosion resistance 高效电磁波吸收和耐腐蚀的核壳纳米线Fe4N@C的设计与合成

IF 11.6 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2026-02-20 Epub Date: 2026-01-23 DOI: 10.1016/j.carbon.2026.121306

Shuting Zhang , Chengguo Wang , Meijie Yu

To further enhance electromagnetic wave absorption capability and the marine corrosion resistance of ferromagnetic metallic materials, a dual-strategy approach combining the construction of the one-dimensional core-shell structure with Fe₄N phase transition was proposed. Through in-situ phenolic resin polymerization on Fe nanowire followed by carbonization-nitridation, core-shell Fe₄N@C nanowires were synthesized, where Fe₄N particles were successfully confined within high-aspect-ratio carbon shells. Distinctive structural and composition design optimized impedance matching and endowed the material with multiple loss mechanisms, including significant conductive loss, interfacial polarization, defect-induced dipole polarization and magnetic loss. Owing to a more balanced dielectric-magnetic synergistic loss relationship, the thicker-shell sample FWCN-2 achieved an impressive minimum reflection loss of −60.51 dB and a maximum effective absorption bandwidth of 7.28 GHz (2.65 mm, 10.72–18.00 GHz) at low filler loading, demonstrating outstanding electromagnetic wave absorption performance. Moreover, by Fe₄N phase transformation, FWCN-2 exhibited enhanced corrosion resistance in marine environments (E_corr = −0.13V, I_corr = 2.63 μA/cm²). This work offered a scalable and structure-guided route to lightweight, broadband, and corrosion-resistant electromagnetic wave absorbers.

为了进一步提高铁磁性金属材料的电磁波吸收能力和耐海洋腐蚀能力，提出了一种将一维核壳结构的构建与Fe4N相变相结合的双策略方法。通过酚醛树脂原位聚合Fe纳米线，然后碳化-氮化，合成了核壳Fe4N@C纳米线，其中Fe4N颗粒成功地限制在高纵横比的碳壳中。独特的结构和组成设计优化了阻抗匹配，并赋予材料多种损耗机制，包括显著的导电损耗、界面极化、缺陷诱导偶极子极化和磁损耗。由于更平衡的介质-磁协同损耗关系，厚壳样品fwn -2在低填料负载下的最小反射损耗为- 60.51 dB，最大有效吸收带宽为7.28 GHz (2.65 mm, 10.72-18.00 GHz)，表现出出色的电磁波吸收性能。通过Fe4N相变，FWCN-2在海洋环境中的耐蚀性增强（Ecorr = - 0.13V, Icorr = 2.63 μA/cm2）。这项工作为轻型、宽带和耐腐蚀电磁波吸收器提供了一种可扩展和结构导向的途径。

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引用次数: 0

Direct laser writing carbon lines on polyimide film tailored for highly sensitive strain sensors with low temperature coefficient 直接激光书写碳线的聚酰亚胺薄膜定制的高灵敏度应变传感器与低温系数

IF 11.6 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2026-02-20 Epub Date: 2026-01-21 DOI: 10.1016/j.carbon.2026.121275

Chenxin Sa , Dini Qing , Yanbo Yao , Tao Liu

Direct laser writing carbonization (DLWc) has been proved to be a highly promising technique for fabricating low-cost piezoresistive sensors. Nevertheless, there remains a great challenge to develop the highly sensitive DLWc enabled strain sensor with low temperature coefficient to impart the sensor with self-temperature-compensation ability. In the present study, we comprehensively investigate the effect of laser processing conditions, carbon line design pattern and testing temperature on the electrical transport characteristics for the carbon lines fabricated by DLWc. Upon mapping the large experimental space to achieve the DLWc carbon lines with a nominal sheet resistance ranging from 1 Ω/sq to 10⁷ Ω/sq, we discovered that the synergistic effect of the laser processing conditions and the carbon line design parameter can make the dotted carbon line convert from an NTC (negative temperature coefficient of resistance) behaviour to that of PTC (positive temperature coefficient of resistance). On the basis of this discovery and along with the combined treatment of strain engineering straining and infusion of PDMS elastomer, we fabricated the DLWc enabled dotted line strain sensor with high piezoresistive sensitivity (gauge factor >1000) and low temperature coefficient and successfully demonstrated its use for sensing small mechanical deformation and high-frequency vibration, as well as for wearable sensor in registering the wrist and finger gesture status, monitoring the heartbeats, and measuring the blood pressure. This study paves the way for developing the DLWc enabled high-performance and low-cost strain sensors with high sensitivity and self-temperature compensation ability.

直接激光写入碳化（DLWc）已被证明是一种极有前途的低成本压阻传感器制造技术。然而，如何开发高灵敏度的低温度系数DLWc应变传感器，使其具有自温度补偿能力，仍然是一个很大的挑战。在本研究中，我们全面研究了激光加工条件、碳线设计模式和测试温度对DLWc制备的碳线电输运特性的影响。通过绘制大的实验空间来实现标称片电阻为1 Ω/sq ~ 107 Ω/sq的DLWc碳线，我们发现激光加工条件和碳线设计参数的协同作用可以使点碳线从NTC（负电阻温度系数）行为转变为PTC（正电阻温度系数）行为。在这一发现的基础上，结合应变工程应变和PDMS弹性体注入的综合处理，我们制造了具有高压阻灵敏度（测量因子>；1000）和低温系数的DLWc启用虚线应变传感器，并成功地演示了其用于感应小机械变形和高频振动，以及用于记录手腕和手指手势状态的可穿戴传感器。监测心跳，测量血压。该研究为开发具有高灵敏度和自温度补偿能力的高性能低成本DLWc应变传感器铺平了道路。

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引用次数: 0

Enhancement of stability and durability in MXene/TaOx bilayer memristor through hetero-interface engineering for neuromorphic computing 基于异质界面工程增强MXene/TaOx双层记忆电阻器的稳定性和耐用性

IF 11.6 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2026-02-20 Epub Date: 2026-01-16 DOI: 10.1016/j.carbon.2026.121273

Mingmin Zhu , Hui Ouyang , Liangyu Chen , Yu Du , Guangxiao Song , Wenjing Dong , Jiawei Wang , Yang Qiu , Guoliang Yu , Wei Wang , Xufeng Jing , Haibin Zhu , Hao-Miao Zhou

Two-dimensional (2D) MXene nanomaterials exhibit considerable potential for electronic devices owing to their metal-like conductivity and abundant surface functional groups. However, utilizing the intrinsic properties of MXene in memristors remains challenging as MXene exhibits free-electron conduction behavior rather than semiconductor characteristics. In this work, a Cu/MXene/TaO_x/ITO memristor was fabricated via heterostructure engineering, and its resistive switching (RS) performances were systematically compared with those of the monolayer Cu/MXene/ITO and Cu/TaO_x/ITO memristors. Compared with the monolayer ones, the MXene/TaO_x memristor exhibits a narrower switching voltage range, a higher on/off ratio exceeding 240, and extended resistance retention exceeding 10⁴ s. Even after 15 months of storage, it maintains stable RS behavior with over 10⁴ cycles of endurance. The enhanced device performance is attributed to the interaction between MXene's surface functional groups and Cu²⁺ ions, coupled with the optimized interface Schottky barrier at the MXene/TaO_x heterojunction. Furthermore, typical biological synaptic plasticity characteristics, such as long-term potentiation/depression (LTP/LTD), paired-pulse facilitation (PPF), and spike time-dependent plasticity (STDP) were simulated with the proposed memristors. The MXene/TaO_x memristor achieves excellent LTP/LTD behavior with the best nonlinearity of 0.39/3.15 and symmetricity of 6.57. By its enhanced conductance symmetry and linearity, an accuracy of up to 94.57 % can be achieved in handwritten digit recognition within a constructed neuromorphic network. These results provide a feasible and effective strategy of integrating 2D materials with metal oxides to enhance memristor performance, highlighting their immense application potential in bio-inspired neuromorphic systems.

二维（2D） MXene纳米材料由于其类似金属的导电性和丰富的表面官能团，在电子器件中表现出相当大的潜力。然而，在记忆电阻器中利用MXene的固有特性仍然具有挑战性，因为MXene表现出自由电子传导行为而不是半导体特性。本文采用异质结构工程方法制备了Cu/MXene/TaOx/ITO忆阻器，并与单层Cu/MXene/ITO和Cu/TaOx/ITO忆阻器的电阻开关性能进行了系统比较。与单层记忆电阻器相比，MXene/TaOx记忆电阻器具有更窄的开关电压范围、更高的通断比（超过240）和延长的电阻保持时间（超过104 s）。即使在15个月的储存后，它仍保持稳定的RS行为，超过104次的续航时间。器件性能的增强是由于MXene表面官能团与Cu2+离子之间的相互作用，以及MXene/TaOx异质结处优化的界面肖特基势垒。此外，还模拟了典型的生物突触可塑性特征，如长时程增强/抑制（LTP/LTD）、对脉冲促进（PPF）和脉冲时间依赖性可塑性（STDP）。MXene/TaOx忆阻器具有优异的LTP/LTD性能，其最佳非线性为0.39/3.15，对称性为6.57。由于其增强的电导对称性和线性性，在构建的神经形态网络中，手写数字识别的准确率高达94.57%。这些结果为将二维材料与金属氧化物集成以提高忆阻器性能提供了一种可行而有效的策略，突出了其在仿生神经形态系统中的巨大应用潜力。

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引用次数: 0

Oxidation-locking of hydrogen-substituted γ-graphdiyne via a two-step hydrothermal route: from enhanced catalyst to bifunctional quantum dots 氢取代γ-石墨炔的两步水热氧化锁：从增强催化剂到双功能量子点

IF 11.6 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2026-02-20 Epub Date: 2026-01-17 DOI: 10.1016/j.carbon.2026.121294

Wenjun Zhang , Youhai Huang , Sifan Zhang , Sanqiang Zhang , Zhaohua Fang , Meng Chen

As a rising new member of carbon allotropes, graphdiyne has shown great potential in various fields due to its fascinating properties. Herein, a controlled two-step hydrothermal route was employed to convert hydrogen-substituted γ-graphdiyne into two functional derivatives: graphdiyne oxides (OGDY) and graphdiyne oxide quantum dots (OGDYQD). Systematic characterization revealed distinct differences in morphology, chemical structure, and optical properties between precursors and derivatives. Especially, the existence of alkyne bonds was demonstrated through evidence from Fourier transform infrared spectroscopy (FTIR), photoluminescence spectroscopy (PL), and selective oxidation experiments, which provides new insights for the characterization of graphdiyne materials. Moreover, we identified an oxidation-locking phenomenon governing selective alkyne oxidation at specific sites during synthesis. The oxidation-locking feature endowed significant application potential upon both derivatives: OGDY exhibited excellent photocatalytic ability in the degradation of cationic dyes, achieving efficiency ∼5–200 higher than those of other carbon-based materials; while OGDYQD could achieve ultrasensitive electrochemical detection of methyl orange with a limit of detection (LOD) as low as 0.032 μM, as well as serve as an excellent catalyst, which was comparable to metal catalysts, for the hydrogenation of 4-nitrophenol. This work provides fundamental insights into sp-carbon reactivity while delivering practical platforms for multiple applications.

石墨炔作为碳同素异形体中一个新兴的成员，以其独特的性能在各个领域显示出巨大的潜力。本文采用可控的两步法将氢取代的γ-石墨炔转化为两种功能衍生物：石墨炔氧化物（OGDY）和石墨炔氧化物量子点（OGDYQD）。系统表征表明前体和衍生物在形态、化学结构和光学性质上存在明显差异。特别是，通过傅里叶变换红外光谱（FTIR）、光致发光光谱（PL）和选择性氧化实验证明了炔键的存在，为石墨炔材料的表征提供了新的见解。此外，我们还发现了一种氧化锁定现象，这种现象控制着合成过程中特定位点的选择性炔氧化。氧化锁定特性为这两种衍生物提供了巨大的应用潜力：OGDY在降解阳离子染料方面表现出优异的光催化能力，效率比其他碳基材料高出约5-200；OGDYQD可实现甲基橙的超灵敏电化学检测，检出限（LOD）低至0.032 μM，是4-硝基苯酚加氢反应的优良催化剂，可媲美金属催化剂。这项工作提供了sp-碳反应性的基本见解，同时为多种应用提供了实用的平台。

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引用次数: 0

High-electronegativity O-triggered vacancy defects and ionic channels in N-doped carbon-confined amorphous Mo–O clusters for high-performance potassium-ion hybrid capacitors 高性能钾离子杂化电容器中n掺杂碳约束非晶Mo-O团簇的高电负性o触发空位缺陷和离子通道

IF 11.6 2区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon

Pub Date : 2026-02-20 Epub Date: 2026-01-27 DOI: 10.1016/j.carbon.2026.121314

Taiyang Wang , Fanyan Zeng , Wenxiu He , Jiaqi Li , Hongbo Huang , Dui Ma , Yang Pan

The performance of potassium-ion hybrid capacitors (PIHCs) is hindered by insufficient electroactive sites and sluggish charge transfer in anodes. Herein, this work proposes a high-electronegativity O-mediated amorphization strategy to construct N-doped carbon-confined amorphous Mo–O clusters (Mo–O@NC). Compared with N- or C-coordinated analogues (Mo–N@NC and Mo–C@NC), the strongly bonded O (χ = 3.44) markedly modulates the local environment of Mo, inducing pronounced electron redistribution. This process generates abundant unsaturated vacancy defects and isotropic ion transport channels in the clusters and at their interfaces. Theoretical calculations reveal that high-electronegativity O optimizes K⁺ adsorption energy, broadens available adsorption sites, and upshifts the d-band center of Mo. These effects collectively promote charge transfer and establish a highly active “electron reservoir.” Electrochemically, the Mo–O@NC anode delivers a high reversible capacity of 529.5 mAh g⁻¹ at 0.1 A g⁻¹ and retains 231.3 mAh g⁻¹ after 3000 cycles at 5.0 A g⁻¹, accompanied by a high capacitive contribution and low charge-transfer resistance, significantly outperforming its counterparts. The assembled PIHCs achieve remarkable energy/power densities (211.2 Wh kg⁻¹/10015 W kg⁻¹), with a capacity decay of only 0.0022 % per cycle. This study offers a novel design strategy for high-performance electrodes for metal ion storage via high-electronegativity O-triggered amorphization.

钾离子混合电容器（pihc）的性能受到电活性位点不足和阳极电荷转移缓慢的阻碍。在此，本研究提出了一种高电负性o介导的非晶化策略来构建n掺杂碳约束的非晶Mo - o簇（Mo - O@NC）。与N-或c -配位类似物（Mo - N@NC和Mo - C@NC）相比，强键O （χ = 3.44）显著调节Mo的局部环境，诱导明显的电子重分布。这一过程在团簇及其界面处产生了丰富的不饱和空位缺陷和各向同性离子输运通道。理论计算表明，高电负性的O优化了K+的吸附能，拓宽了可用的吸附位点，并提升了Mo的d带中心。这些效应共同促进了电荷转移，并建立了一个高活性的“电子库”。在电化学上，Mo - O@NC阳极在0.1 a g - 1下提供529.5 mAh g - 1的高可逆容量，在5.0 a g - 1下循环3000次后保持231.3 mAh g - 1，同时具有高电容贡献和低电荷转移电阻，显著优于同类阳极。组装的pihc实现了显著的能量/功率密度（211.2 Wh kg−1/10015 W kg−1），每周期容量衰减仅为0.0022%。本研究通过高电负性o触发非晶化为高性能金属离子存储电极提供了一种新的设计策略。

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