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Gold nanorod gradient surfaces 金纳米棒梯度表面
IF 6.9 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-05-30 Epub Date: 2026-01-27 DOI: 10.1016/j.apsusc.2026.166104
Maja Lidström Uusitalo , Michal Strach , Mats Hulander , Martin Andersson
Materials based on solid-supported nanoparticles are used in a range of applications, spanning from catalysis to sensing. Controlling the inter-nanoparticle distance is essential in property optimization of these materials. To achieve such control, nanoparticle gradient surfaces, where nanoparticles are attached in a number density gradient on the support, show great promise. This study presents a tunable method for the preparation of gold nanorod gradient surfaces, exploiting nanoparticle adsorption kinetics to control the surface coverage. The method involves immersing a mercapto silane-functionalized substrate in a gold nanorod suspension, which is then withdrawn at a fixed rate. We show that the gradient dynamics can be tuned by changing the withdrawal rate, and that the gradients exhibit a linear increase in surface coverage along the distance of the support. The changes in optical properties and influence of plasmon coupling with the surface coverage of gold nanorods were evaluated using extinction spectroscopy. Additionally, by assessing the photothermal properties of the gradients upon irradiation with a near-infrared laser, through thermal imaging and in situ X-ray diffraction, we show that a temperature gradient is achieved, correlating with the increased surface coverage of gold nanorods.
基于固体支撑纳米颗粒的材料被用于从催化到传感的一系列应用中。控制纳米粒子间的距离是优化这些材料性能的关键。为了实现这样的控制,纳米颗粒梯度表面,即纳米颗粒以一定数量的密度梯度附着在载体上,显示出很大的希望。本研究提出了一种制备金纳米棒梯度表面的可调方法,利用纳米颗粒吸附动力学来控制表面覆盖。该方法包括将巯基硅烷功能化的底物浸入金纳米棒悬浮液中,然后以固定速率撤出。我们表明,梯度动态可以通过改变退出率来调整,并且梯度沿支架的距离呈现线性增加的表面覆盖率。利用消光光谱研究了等离激元耦合对金纳米棒表面覆盖度的影响。此外,通过评估近红外激光照射后梯度的光热特性,通过热成像和原位x射线衍射,我们表明实现了温度梯度,与金纳米棒表面覆盖率的增加相关。
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引用次数: 0
Nitrogen-rich porous carbon for long-lived sodium-ion batteries: An efficient strategy based on interpenetrating polymers 用于长寿命钠离子电池的富氮多孔碳:基于互穿聚合物的有效策略
IF 6.9 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-05-30 Epub Date: 2026-02-05 DOI: 10.1016/j.apsusc.2026.166209
Fei-Yu Hu , Zu-Tao Pan , Ling-Bin Kong
Carbon materials have garnered significant attention due to their low cost and structural tunability. This study developed an amorphous carbon (A-C) material suitable for sodium-ion batteries (SIBs) using industrially producible dicyandiamide-formaldehyde resin (DFR) as a precursor. To address challenges such as low carbon yield, severe high-temperature pyrolysis, and insufficient sodium storage sites, a three-dimensional cross-linked network was constructed by introducing polyacrylate. Combined with a metal ion etching strategy, this approach effectively expanded the carbon interlayer spacing, enriched active sites, and formed a high-specific-surface-area, hierarchical porous structure. Benefiting from these structural advantages, the A-C anode exhibits outstanding sodium storage performance: The initial coulombic efficiency was 90.11% and the reversible specific capacity remained at 348.9 mAhg−1 after 500 cycles at 2 Ag−1. The symmetric full cell assembled with this anode retains a capacity of 246 Whkg−1 after 1500 cycles, achieving a capacity retention rate of 85.3%. This study provides a simple, scalable synthetic pathway for developing high-performance carbon anodes, significantly advancing the practical application of SIBs.
碳材料因其低成本和结构的可调性而受到广泛关注。本研究以工业生产的双氰胺甲醛树脂(DFR)为前驱体,开发了一种适用于钠离子电池(sib)的无定形碳(a - c)材料。为了解决碳收率低、高温热解严重、钠储存位点不足等问题,引入聚丙烯酸酯构建了三维交联网络。结合金属离子蚀刻策略,该方法有效地扩大了碳层间距,丰富了活性位点,形成了高比表面积、层次化的多孔结构。得益于这些结构优势,A-C阳极表现出优异的储钠性能:在2ag−1下循环500次后,初始库仑效率为90.11%,可逆比容量保持在348.9 mAhg−1。使用该阳极组装的对称全电池在1500次循环后保持了246 Whkg−1的容量,实现了85.3%的容量保持率。该研究为开发高性能碳阳极提供了一种简单、可扩展的合成途径,显著推进了sib的实际应用。
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引用次数: 0
p-d orbital hybridization induced by carbon-doped of nickel sulfides for enhanced hydrogen evolution reaction 碳掺杂硫化镍诱导P-d轨道杂化增强析氢反应
IF 6.9 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-05-30 Epub Date: 2026-02-04 DOI: 10.1016/j.apsusc.2026.166206
Xiaobing Xu , Haoyuan Wei , Qing Luo , Haifeng Chu , Xueming Liu , Yanru Jiang , Yulan Zhu , Lei Zhang , Min Zhang , Shiming Yan , Zhigang Zhang , Peng Zhan , Xinglong Wu
Since the modulation of electron distribution in metal active sites plays a vital role to boost the catalytic activity, it is essential to optimize hydrogen adsorption by p-d orbital coupling for efficient hydrogen evolution catalysis. Herein, we employ a hydrothermal approach and carburization treatments to prepare the C-doped Ni3S2 nanoarrays on the Nickel Foam substrate (C-Ni3S2/NF). Density functional theoretical (DFT) analysis reveals optimal carbon doped could induce p-d orbital coupling between Ni 3d and S 2p orbital in C-Ni3S2, which can optimize the electrons states density of the dominated Ni atoms and lower the Gibbs free energy of hydrogen adsorption (ΔGH*) simultaneously. As a result, an overpotential of 38 mV at 10 mA cm−2 and Tafel slope down to 47 mV dec−1 suggest the C-Ni3S2/NF with 6% C doped owns an enhanced alkaline hydrogen evolution reaction. This study would offer a perception into the logical design of nonprecious-metal catalysis with high electrocatalytic activities for practical applications via p-d orbital coupling.
由于金属活性位点的电子分布调节对提高催化活性起着至关重要的作用,因此优化p-d轨道耦合对氢的吸附是实现高效析氢催化的必要条件。本文采用水热法和渗碳处理在泡沫镍衬底上制备了掺杂c的Ni3S2纳米阵列(C-Ni3S2/NF)。密度泛函数理论(DFT)分析表明,最佳碳掺杂可以诱导C-Ni3S2中Ni 3d和s2p轨道之间的p-d轨道耦合,从而优化Ni主导原子的电子态密度,同时降低氢吸附的吉布斯自由能(ΔGH*)。结果表明,C- ni3s2 /NF在10 mA cm−2时的过电位为38 mV, Tafel斜率降至47 mV dec−1,表明掺6% C的C- ni3s2 /NF具有增强的碱性析氢反应。该研究将为通过p-d轨道耦合实现具有高电催化活性的非贵金属催化剂的逻辑设计提供一种思路
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引用次数: 0
Self-regenerating passivation of redox-responsive polyaniline in elastomer-modified perfluorocyclobutyl polymer coatings 弹性体改性全氟环丁基聚合物涂料中氧化还原反应聚苯胺的自再生钝化
IF 6.9 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-05-30 Epub Date: 2026-02-04 DOI: 10.1016/j.apsusc.2026.166207
Mark Rigel R. Ali , Reymark D. Maalihan , Rebekah C. Wilson , Eugene B. Caldona
The development of corrosion-protective coatings combining barrier durability with active interfacial control remains a challenge in achieving long-term sustainability for metallic infrastructure. This study introduces an elastomer-modified perfluorocyclobutyl (EPFCB) fluoropolymer composite incorporating redox-active polyaniline (PANI) as a multifunctional filler to achieve both barrier and self-passivating protection. At moderate loading (∼0.5 wt%), PANI optimizes mechanical compliance and adhesion while maintaining the low surface energy and dielectric stability of the EPFCB matrix, providing a robust foundation for active corrosion control. Macroscopic performance, evaluated by electrochemical impedance spectroscopy, potentiodynamic polarization, cyclic corrosion, and UV weathering, was correlated with interfacial chemistry and morphology through complementary spectroscopic and microscopic analyses. The results show that well-dispersed PANI domains establish localized redox equilibria (emeraldine salt ⇄ emeraldine base) that regulate Fe oxidation and promote a uniform, continuous Fe(III)-rich passive layer at early corrosion sites, as verified by surface spectroscopy and potential mapping. The optimal formulation exhibited sustained impedance above 108 Ω·cm2 after 30 d in 3.5 wt% NaCl solution, minimal rust creep, and improved UV stability, outperforming both neat EPFCB and higher PANI loadings. These findings demonstrate that sub-percolation PANI incorporation transforms an inert fluoropolymer barrier into a hybrid, self-regulating coating system, bridging passive protection and dynamic interfacial passivation.
结合屏障耐久性和主动界面控制的防腐涂层的开发仍然是金属基础设施实现长期可持续性的挑战。本研究介绍了一种弹性体改性的全氟环丁基(EPFCB)含氟聚合物复合材料,其中含有氧化还原活性聚苯胺(PANI)作为多功能填料,以实现屏障和自钝化保护。在中等负载(~ 0.5 wt%)下,PANI优化了EPFCB基体的机械适应性和粘附性,同时保持了EPFCB基体的低表面能和介电稳定性,为主动腐蚀控制提供了坚实的基础。宏观性能通过电化学阻抗谱、动电位极化、循环腐蚀和紫外线风化来评估,并通过互补的光谱和微观分析将界面化学和形貌联系起来。结果表明,分散良好的聚苯胺域建立了局部氧化还原平衡(祖母绿盐  祖母绿碱),调节了铁的氧化,并在早期腐蚀部位促进了均匀、连续的富铁(III)钝化层,这得到了表面光谱和电位映射的证实。最佳配方在3.5% NaCl环境下处理30 天后阻抗维持在108 Ω·cm2以上,锈蠕变最小,紫外线稳定性提高,优于纯EPFCB和高PANI负载。这些发现表明,聚苯胺的亚渗透掺入将惰性含氟聚合物屏障转变为一种混合的、自调节的涂层体系,架起了被动保护和动态界面钝化的桥梁。
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引用次数: 0
Synergistic modification of g-C3N4-based photocatalysts with MnCo2O4 and carbon dots for optimizing multiple processes in photocatalytic H2 production MnCo2O4与碳点协同改性g- c3n4基光催化剂以优化光催化制氢的多个工艺
IF 6.9 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-05-30 Epub Date: 2026-02-05 DOI: 10.1016/j.apsusc.2026.166215
Jialin Lu , Jiazheng Zhang , Daokui Yang , Zhanlong Song , Wenlong Wang , Yibo Gao , Yanpeng Mao
Faced with global energy and environmental crises, developing novel and efficient photocatalysts to enhance the efficiency of photocatalytic water splitting for hydrogen production represents a crucial solution to future energy challenges. However, photocatalytic reactions involve multiple steps, and a slow rate in any one step can limit the overall rate of the photocatalytic reaction system. In this study, a novel MnCo2O4 and carbon dot (CDs) co-modified nanoflake g-C3N4 (MnCo2O4/NCN-CDs) composite photocatalyst was synthesized via a simple method, achieving synergistic optimization of multiple steps. The as-prepared MnCo2O4/NCN-CDs catalyst exhibits a higher photocatalytic water splitting H2 production rate than pristine nanoflake g-C3N4 (NCN), and tests under complex conditions further confirm its potential for practical application. Targeted characterization analyses verify two key mechanisms: the S-scheme charge transfer mechanism in the MnCo2O4/NCN system and the optimization of surface properties by CDs. Additionally, variable-controlled experiments clarify the positive role of MnCo2O4′s photothermal effect in broadening the spectral utilization range and enhancing catalytic activity. This study, for the first time, proposes a synergistic modification strategy that simultaneously optimizes three critical processes in photocatalysis (light utilization, carrier separation and transfer, and surface redox reactions), providing a paradigm for the design of high-performance photocatalysts.
面对全球性的能源和环境危机,开发新型高效的光催化剂来提高光催化水裂解制氢的效率是解决未来能源挑战的关键。然而,光催化反应涉及多个步骤,任何一个步骤的慢速都会限制光催化反应体系的总体速度。本研究通过简单的方法合成了一种新型的MnCo2O4和碳点(CDs)共改性纳米片g-C3N4 (MnCo2O4/NCN-CDs)复合光催化剂,实现了多步骤协同优化。制备的MnCo2O4/NCN- cds催化剂比原始纳米片g-C3N4 (NCN)具有更高的光催化水裂解H2产率,在复杂条件下的测试进一步证实了其实际应用潜力。有针对性的表征分析验证了两个关键机制:MnCo2O4/NCN体系中的S-scheme电荷转移机制和CDs对表面性能的优化。此外,变量控制实验还阐明了MnCo2O4光热效应在拓宽光谱利用范围和提高催化活性方面的积极作用。本研究首次提出了一种协同改性策略,同时优化光催化中的三个关键过程(光利用、载流子分离和转移以及表面氧化还原反应),为高性能光催化剂的设计提供了范例。
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引用次数: 0
Dual anion induced amorphous-crystalline CoNi-P-B heterojunctions for bifunctional water splitting electrocatalyst 双阴离子诱导的非晶CoNi-P-B异质结双功能水分解电催化剂
IF 6.9 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-05-30 Epub Date: 2026-02-06 DOI: 10.1016/j.apsusc.2026.166152
Jiale Wu, Kaizhao Wang, Zhaowei Sun, Kaijun Wang, Jian Wang, Junkai Li, Yafei Wang, Jin Hu, Shizhao Xiong
Amorphous structures and heterojunctions are regarded as effective strategies for significantly enhancing the electrocatalytic activity, owing to their unique electronic modulation capabilities. Herein, by controllable phosphatization and boronation of coral-like CoNi microparticles, bifunctional CoNi-P-B electrocatalysts with crystalline CoNiP/amorphous CoNiP-B heterogeneous interface were successfully constructed. Combined experimental and theoretical analyses reveal that P/B co-doping, amorphous structure introduction, and heterogeneous interface construction jointly endow the materials with optimized charge distribution states, a large number of available active sites, and accelerated interfacial electronic coupling and charge transfer, resulting in a significantly optimized d-band center and reduced intermediate adsorption/desorption energy barriers. During the oxygen evolution reaction (OER), the catalyst pre-generated numerous γ-Ni/CoOOH as the actual active phase through surface reconstruction to potentially enhance its reaction kinetics and intrinsic activity. It exhibits outstanding oxygen and hydrogen evolution reaction (HER) activities, requiring low overpotentials of only 235 mV and 109 mV overpotentials at 10 mA cm−2 current density, respectively, along with excellent long-term durability. This work offers valuable insights into developing efficient and stable water splitting electrocatalysts through the integration of amorphous structures and heterointerface engineering.
由于其独特的电子调制能力,非晶结构和异质结被认为是显著提高电催化活性的有效策略。在此基础上,通过可控磷化和硼化,成功构建了具有晶态CoNiP/非晶态CoNiP- b非均相界面的双功能CoNiP- p - b电催化剂。实验和理论分析表明,P/B共掺杂、非晶结构的引入和非均相界面的构建共同使材料具有优化的电荷分布状态、大量的可用活性位点、加速的界面电子耦合和电荷转移,从而显著优化了d带中心,降低了中间吸附/解吸能垒。在析氧反应(OER)过程中,催化剂通过表面重构预先生成大量γ-Ni/CoOOH作为实际活性相,有可能提高其反应动力学和本禀活性。它具有出色的析氧反应和析氢反应(HER)活性,在10 mA cm - 2电流密度下,过电位仅为235 mV和109 mV,并且具有优异的长期耐用性。这项工作为通过非晶结构和异质界面工程的结合开发高效稳定的水分解电催化剂提供了有价值的见解。
{"title":"Dual anion induced amorphous-crystalline CoNi-P-B heterojunctions for bifunctional water splitting electrocatalyst","authors":"Jiale Wu,&nbsp;Kaizhao Wang,&nbsp;Zhaowei Sun,&nbsp;Kaijun Wang,&nbsp;Jian Wang,&nbsp;Junkai Li,&nbsp;Yafei Wang,&nbsp;Jin Hu,&nbsp;Shizhao Xiong","doi":"10.1016/j.apsusc.2026.166152","DOIUrl":"10.1016/j.apsusc.2026.166152","url":null,"abstract":"<div><div>Amorphous structures and heterojunctions are regarded as effective strategies for significantly enhancing the electrocatalytic activity, owing to their unique electronic modulation capabilities. Herein, by controllable phosphatization and boronation of coral-like CoNi microparticles, bifunctional CoNi-P-B electrocatalysts with crystalline CoNiP/amorphous CoNiP-B heterogeneous interface were successfully constructed. Combined experimental and theoretical analyses reveal that P/B co-doping, amorphous structure introduction, and heterogeneous interface construction jointly endow the materials with optimized charge distribution states, a large number of available active sites, and accelerated interfacial electronic coupling and charge transfer, resulting in a significantly optimized d-band center and reduced intermediate adsorption/desorption energy barriers. During the oxygen evolution reaction (OER), the catalyst pre-generated numerous γ-Ni/CoOOH as the actual active phase through surface reconstruction to potentially enhance its reaction kinetics and intrinsic activity. It exhibits outstanding oxygen and hydrogen evolution reaction (HER) activities, requiring low overpotentials of only 235 mV and 109 mV overpotentials at 10 mA cm<sup>−2</sup> current density, respectively, along with excellent long-term durability. This work offers valuable insights into developing efficient and stable water splitting electrocatalysts through the integration of amorphous structures and heterointerface engineering.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"729 ","pages":"Article 166152"},"PeriodicalIF":6.9,"publicationDate":"2026-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146134600","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High-throughput DFT screening of single-atom catalysts: unraveling the effects of transition metals and coordination environments for electrocatalytic nitrate-to-ammonia conversion 单原子催化剂的高通量DFT筛选:揭示过渡金属和配位环境对电催化硝酸盐转化为氨的影响
IF 6.9 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-05-30 Epub Date: 2026-02-08 DOI: 10.1016/j.apsusc.2026.166226
Beibei Yan , Dandan Xu , Tiecheng Liu , Kang Tang , Jinglan Wang , Guanyi Chen , Zhanjun Cheng
Electrocatalytic nitrate reduction reaction (NO3RR) to ammonia (NH3) represents a promising “waste-to-wealth” strategy, addressing both nitrate wastewater treatment and sustainable NH3 synthesis. The key challenge lies in developing electrocatalysts with high NO3RR performance to enhance the yield and selectivity of NH3. Herein, density functional theory calculations were performed to comprehensively evaluate the synergistic effects between transition metal centers (Fe, Co, Ni, Cu, Ru, Rh) supported on five different coordination environments of defective carbon nitride (CNx) substrate, aiming to rationally design high-performance single-atom catalysts (SACs) for NO3RR. The calculation results revealed that the Co center in a specific coordination environment (Co-CN3) exhibited notable comprehensive performance. The limiting potential of the potential-determining step was as low as −0.13 V. It showed high selectivity for the target product NH3, effectively suppressing the hydrogen evolution reaction and the formation pathways of other nitrogen-containing by-products. Its stability in molecular dynamics simulations suggests potential for experimental realization. This work predicted a highly promising catalyst candidate, Co-CN3 SAC. It revealed the microscopic mechanism of “metal-coordination” combination in regulating catalytic performance, providing a new theoretical perspective and clear design principles for subsequent experimental synthesis and broader electrocatalyst design.
电催化硝酸还原反应(NO3RR)制氨(NH3)是一种有前途的“废物转化财富”策略,既解决了硝酸盐废水处理问题,又解决了可持续的NH3合成问题。关键的挑战在于开发高NO3RR性能的电催化剂,以提高NH3的收率和选择性。本文通过密度泛函理论计算,综合评价了在缺陷氮化碳(CNx)衬底5种不同配位环境下过渡金属中心(Fe, Co, Ni, Cu, Ru, Rh)之间的协同效应,旨在合理设计高性能NO3RR单原子催化剂。计算结果表明,Co中心在特定配位环境(Co- cn3)中表现出显著的综合性能。测定电位步骤的极限电位低至−0.13 V。对目标产物NH3具有较高的选择性,有效抑制了析氢反应和其他含氮副产物的生成途径。它在分子动力学模拟中的稳定性表明了实验实现的潜力。这项工作预测了一个非常有前途的催化剂候选物,Co-CN3 SAC。揭示了“金属-配位”组合调控催化性能的微观机制,为后续的实验合成和更广泛的电催化剂设计提供了新的理论视角和明确的设计原则。
{"title":"High-throughput DFT screening of single-atom catalysts: unraveling the effects of transition metals and coordination environments for electrocatalytic nitrate-to-ammonia conversion","authors":"Beibei Yan ,&nbsp;Dandan Xu ,&nbsp;Tiecheng Liu ,&nbsp;Kang Tang ,&nbsp;Jinglan Wang ,&nbsp;Guanyi Chen ,&nbsp;Zhanjun Cheng","doi":"10.1016/j.apsusc.2026.166226","DOIUrl":"10.1016/j.apsusc.2026.166226","url":null,"abstract":"<div><div>Electrocatalytic nitrate reduction reaction (NO<sub>3</sub>RR) to ammonia (NH<sub>3</sub>) represents a promising “waste-to-wealth” strategy, addressing both nitrate wastewater treatment and sustainable NH<sub>3</sub> synthesis. The key challenge lies in developing electrocatalysts with high NO<sub>3</sub>RR performance to enhance the yield and selectivity of NH<sub>3</sub>. Herein, density functional theory calculations were performed to comprehensively evaluate the synergistic effects between transition metal centers (Fe, Co, Ni, Cu, Ru, Rh) supported on five different coordination environments of defective carbon nitride (CN<sub>x</sub>) substrate, aiming to rationally design high-performance single-atom catalysts (SACs) for NO<sub>3</sub>RR. The calculation results revealed that the Co center in a specific coordination environment (Co-CN<sub>3</sub>) exhibited notable comprehensive performance. The limiting potential of the potential-determining step was as low as −0.13 V. It showed high selectivity for the target product NH<sub>3</sub>, effectively suppressing the hydrogen evolution reaction and the formation pathways of other nitrogen-containing by-products. Its stability in molecular dynamics simulations suggests potential for experimental realization. This work predicted a highly promising catalyst candidate, Co-CN<sub>3</sub> SAC. It revealed the microscopic mechanism of “metal-coordination” combination in regulating catalytic performance, providing a new theoretical perspective and clear design principles for subsequent experimental synthesis and broader electrocatalyst design.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"729 ","pages":"Article 166226"},"PeriodicalIF":6.9,"publicationDate":"2026-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146134584","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A first-principles study of two-dimensional V2N as a cathode material for sodium-sulfur batteries 二维V2N作为钠硫电池正极材料的第一性原理研究
IF 6.9 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-05-30 Epub Date: 2026-02-03 DOI: 10.1016/j.apsusc.2026.166198
Yusheng Wang , Juanjuan Wang , Yaolong Jia , Nahong Song , Xiaoyan Song , Haiyan Gao , Qiaoli Zhang , Bin Xu , Yaru Peng , Fei Wang
The practical implementation of room-temperature sodium-sulfur (Na-S) batteries is hindered by polysulfide shuttling and sluggish reaction kinetics. To tackle these issues, we systematically investigated surface-functionalized two-dimensional (2D) vanadium nitride (V2N) MXene as sulfur cathode hosts using first-principles calculations. The results indicate that the functionalized V2N-Tx (where T = O, F, S, OH) can effectively anchor polysulfides, thereby suppressing the shuttle effect. Among these functionalized materials, V2N-S exhibits excellent metallic characteristics, a moderate polysulfide anchoring ability, and remarkable dynamic performance. It features a low energy barrier of 0.40 eV for the sulfur reduction reaction (SRR) and only a 0.10 eV diffusion barrier for Na ions. Additionally, the asymmetric surface of V2N-F facilitates rapid Na ion migration (with an energy barrier of 0.15 eV) and efficient Na2S decomposition (0.26 eV), thus overcoming key kinetic bottlenecks. This work highlights functionalized V2N as an outstanding cathode host for high-performance Na-S batteries. It also provides perspectives on design of advanced MXene electrocatalysts via surface chemistry engineering.
室温钠硫(Na-S)电池的实际实施受到多硫化物穿梭和反应动力学缓慢的阻碍。为了解决这些问题,我们使用第一性原理计算系统地研究了表面功能化二维(2D)氮化钒(V2N) MXene作为硫阴极宿主。结果表明,功能化的V2N-Tx (T = O, F, S, OH)可以有效地锚定多硫化物,从而抑制穿梭效应。在这些功能化材料中,V2N-S具有优异的金属特性、适度的多硫化物锚定能力和显著的动态性能。硫还原反应(SRR)具有0.40 eV的低能垒,而Na离子的扩散势垒仅为0.10 eV。此外,V2N-F的不对称表面有利于Na离子的快速迁移(能垒为0.15 eV)和Na2S的高效分解(0.26 eV),从而克服了关键的动力学瓶颈。这项工作突出了功能化V2N作为高性能Na-S电池的优秀阴极宿主。并从表面化学工程的角度对新型MXene电催化剂的设计提出了展望。
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引用次数: 0
Hydrophilic surface modification of polytetrafluoroethylene by ultraviolet induced grafting polymerization 紫外光诱导接枝聚合对聚四氟乙烯的亲水性表面改性
IF 6.9 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-05-30 Epub Date: 2026-02-01 DOI: 10.1016/j.apsusc.2026.166167
Chuan Li , Wangfeng Du , Guan Wang , Changwen Zhao , Wantai Yang
Polytetrafluoroethylene (PTFE) exhibits outstanding chemical and thermal stability, but its strong hydrophobicity and poor adhesion property limit its potential applications. To address these limitations, we developed a facile two-step photografting method for effectively modifying the surface of polytetrafluoroethylene (PTFE). The PTFE surface was firstly activated under UV irradiation in the presence of an amide compound. Then, UV-induced graft polymerization of acrylic acid was performed on the activated PTFE substrate using benzophenone as photosensitizer. Under optimal conditions (1 wt% BP, 30 wt% AA, 10 min of UV irradiation), the modified PTFE surface exhibited high hydrophilicity, with a water contact angle of 15° and a graft density of 407.8 nmol/cm2. Patterned modification of the PTFE was achieved by using a photomask to enable the controlled immobilization of proteins. Furthermore, the peel strength between the modified PTFE and stainless steel increased to 10.3 N/cm.
聚四氟乙烯(PTFE)具有良好的化学稳定性和热稳定性,但其较强的疏水性和较差的粘接性能限制了其潜在的应用前景。为了解决这些限制,我们开发了一种简单的两步光接枝方法来有效地修饰聚四氟乙烯(PTFE)的表面。聚四氟乙烯表面首先在酰胺化合物存在下的紫外线照射下活化。然后,以二苯甲酮为光敏剂,在活化的聚四氟乙烯基上进行了紫外诱导丙烯酸接枝聚合。在最佳条件下(1 wt% BP, 30 wt% AA, 10 min UV照射),改性聚四氟乙烯表面具有较高的亲水性,水接触角为15°,接枝密度为407.8 nmol/cm2。聚四氟乙烯的图案修饰是通过使用光掩膜实现的,以控制蛋白质的固定。改性PTFE与不锈钢之间的剥离强度提高到10.3 N/cm。
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引用次数: 0
High-performance filter supercapacitors utilizing graphene aerogel composite thin-film electrodes 采用石墨烯气凝胶复合薄膜电极的高性能滤波超级电容器
IF 6.9 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-05-30 Epub Date: 2026-02-07 DOI: 10.1016/j.apsusc.2026.166210
Qingsong Zhao , Guanglei Zhang , Shuai Yang , Zunbin Duan , Gang Yu
Filter supercapacitors (FSCs) have emerged as ideal candidates to replace traditional aluminum electrolytic capacitors due to their superior power characteristics and rapid charge–discharge capabilities, offering a critical solution for the miniaturization and integration of electronic devices. However, their further development has been hindered by the inherent trade-off between the charge–discharge rate and charge storage capacity of electrode materials. This study proposes an innovative composite electrode design strategy, successfully constructing a three-dimensional reduced graphene oxide aerogel film skeleton with high electronic conductivity through a mild thermochemical reduction method. The oxygen-containing functional groups retained on its surface enhance the ion charge transport rate, ultimately achieving a coordinated optimization of electronic and ionic conductivity. Meanwhile, the surface-loaded, highly electrochemically active CuxO nanoparticles synergistically boost the capacitance density of this integrated composite electrode. The FSC based on these electrodes demonstrates outstanding frequency response at a high frequency of 120 Hz: a phase angle of −80.04°, and a remarkable areal capacitance of 3.24 mF cm−2. This study not only significantly advances the performance boundaries of FSCs in balancing frequency response and capacitance density but also provides innovative theoretical guidance and technical solutions for the electrode structure design of next-generation miniaturized FSCs.
滤波超级电容器(FSCs)由于其优越的功率特性和快速充放电能力,已成为取代传统铝电解电容器的理想候选者,为电子设备的小型化和集成化提供了关键解决方案。然而,电极材料的充放电速率和电荷存储能力之间的内在权衡阻碍了它们的进一步发展。本研究提出了一种创新的复合电极设计策略,通过温和的热化学还原方法,成功构建了具有高电子导电性的三维还原氧化石墨烯气凝胶膜骨架。保留在其表面的含氧官能团提高了离子电荷传输速率,最终实现了电子和离子电导率的协调优化。同时,表面负载的高电化学活性CuxO纳米颗粒协同提高了该集成复合电极的电容密度。基于这些电极的FSC在120 Hz的高频下表现出出色的频率响应,相角为- 80.04°,面电容为3.24 mF cm−2。本研究不仅突破了FSCs在平衡频率响应和电容密度方面的性能界限,也为下一代小型化FSCs的电极结构设计提供了创新的理论指导和技术解决方案。
{"title":"High-performance filter supercapacitors utilizing graphene aerogel composite thin-film electrodes","authors":"Qingsong Zhao ,&nbsp;Guanglei Zhang ,&nbsp;Shuai Yang ,&nbsp;Zunbin Duan ,&nbsp;Gang Yu","doi":"10.1016/j.apsusc.2026.166210","DOIUrl":"10.1016/j.apsusc.2026.166210","url":null,"abstract":"<div><div>Filter supercapacitors (FSCs) have emerged as ideal candidates to replace traditional aluminum electrolytic capacitors due to their superior power characteristics and rapid charge–discharge capabilities, offering a critical solution for the miniaturization and integration of electronic devices. However, their further development has been hindered by the inherent trade-off between the charge–discharge rate and charge storage capacity of electrode materials. This study proposes an innovative composite electrode design strategy, successfully constructing a three-dimensional reduced graphene oxide aerogel film skeleton with high electronic conductivity through a mild thermochemical reduction method. The oxygen-containing functional groups retained on its surface enhance the ion charge transport rate, ultimately achieving a coordinated optimization of electronic and ionic conductivity. Meanwhile, the surface-loaded, highly electrochemically active Cu<em><sub>x</sub></em>O nanoparticles synergistically boost the capacitance density of this integrated composite electrode. The FSC based on these electrodes demonstrates outstanding frequency response at a high frequency of 120 Hz: a phase angle of −80.04°, and a remarkable areal capacitance of 3.24 mF cm<sup>−2</sup>. This study not only significantly advances the performance boundaries of FSCs in balancing frequency response and capacitance density but also provides innovative theoretical guidance and technical solutions for the electrode structure design of next-generation miniaturized FSCs.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"729 ","pages":"Article 166210"},"PeriodicalIF":6.9,"publicationDate":"2026-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146129542","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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