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Electron-rich and electron-poor active centers induced by interface coupling to enhance the degradation of fluorinated antibiotic via peroxymonosulfate activation. 界面耦合诱导富电子和贫电子活性中心通过过氧单硫酸盐活化增强氟化抗生素的降解。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-01 Epub Date: 2025-08-20 DOI: 10.1016/j.jcis.2025.138781
Ruya Chen, Dongchen Lv, Jiayi Gao, Xinyun Li, Shengran Yu, Yudi Wang, Tong Wei, Yanqing Cong, Shi-Wen Lv

The water pollution issue triggered by antibiotic was a great challenge facing humanity, and it was necessary to develop an effective remediation technique. In this work, Fe2O3/Co3O4 composite with internal electric field was fabricated by a simple method. The presence of internal electric field reduced the interfacial resistance and facilitated the charge transfer, so stimulating the electron transport during reaction process. With the inducement of electrostatic force based on internal electric field, two active areas (namely electron-rich region and electron-deficient region) were formed at Fe2O3/Co3O4 composite. The electron-deficient active area (namely Co3O4 component) can oxidize peroxymonosulfate (PMS) to produce SO5•-, further turning into 1O2. In the meantime, the Fe2O3 component as electron-rich active area provided electrons to achieve the Fe-O-O heterolysis, then generating high-valent metal complexes. As predicted, the Fe2O3/Co3O4-driven PMS system displayed excellent ability to remove ofloxacin. Furthermore, the micro reactor loaded with Fe2O3/Co3O4 composite exhibited satisfactory performance in treating the wastewater containing ofloxacin. All in all, the effects of internal electric field on PMS activation are investigated in depth, which provided a valuable reference for future research.

抗生素引发的水污染问题是人类面临的巨大挑战,有必要开发一种有效的修复技术。本文采用一种简单的方法制备了具有内电场的Fe2O3/Co3O4复合材料。内部电场的存在降低了界面电阻,促进了电荷的传递,从而刺激了反应过程中的电子传递。在基于内部电场的静电力的诱导下,Fe2O3/Co3O4复合材料形成了富电子区和缺电子区两个活性区。缺电子活性区(即Co3O4组分)可氧化过氧单硫酸根(PMS)生成SO5•-,进而转化为1O2。同时,Fe2O3组分作为富电子活性区提供电子,实现Fe-O-O杂解,生成高价金属配合物。正如预测的那样,Fe2O3/ co3o4驱动的PMS体系表现出优异的去除氧氟沙星的能力。此外,负载Fe2O3/Co3O4复合材料的微反应器在处理含氧氟沙星废水中表现出满意的性能。总之,深入研究了内部电场对PMS活化的影响,为今后的研究提供了有价值的参考。
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引用次数: 0
Iron-cobalt dual atomic sites in N, P-codoped carbon nanobelts as a multifunctional catalyst for Zn-air/iodide hybrid batteries. N, p共掺杂碳纳米带中铁钴双原子位作为锌-空气/碘化物混合电池的多功能催化剂。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-01 Epub Date: 2025-08-06 DOI: 10.1016/j.jcis.2025.138640
Hanwen He, Depeng Zhang, Xinshuang Lin, Hongrui Yang, Jiabei Yu, Hangyuan Xing, Rong Gao, Yukun Liu, Sen Zhang, Chao Deng

The exploration of high-performance and multifunctional catalysts is a key issue in Zinc-air/iodide hybrid battery (ZAIHB). In this study, iron‑cobalt dual atomic sites (DAS) embedded in a biomass-derived (N, P) heteroatom-codoped carbon nanobelt (NPCB) framework were designed as a multifunctional catalyst for ZAIHB. Theoretical analysis reveals that the structure matching on both dual-atomic-centers and local electronic engineering contribute to the promoted catalytic activities for oxygen and iodide redox reactions. In addition, the nitrogen (N)-, and phosphorus (P)-codoped carbon nanobelts contributed to the highly porous and freestanding substrate, which endowed rapid kinetics. Benefiting from the above advantageous features, FeCo DAS@NPCB exhibits the excellent multifunctional catalytic properties for oxygen/iodide redox reactions. The full ZAIHB battery with the FeCo DAS@NPCB cathode exhibited high energy efficiency (77.4 %) and a long cycle life (over 300 h). Moreover, the solid-state ZAIHB with a hydrogel electrolyte showed good flexibility and stability during charge/discharge cycling. More impressively, the cell shows high reliability during the transition from exposure to air to an oxygen free environment with the replacement of oxygen reduction reaction (ORR) by iodide reduction reaction (IRR). This unique mechanism results in the high adaptability of the fabricated ZAIHB to serve multifarious working environments. Therefore, this study introduces a novel strategy for the design and construction of multifunctional catalysts, and promotes the rapid development of highly efficient ZAIHB for diverse electronics.

探索高性能、多功能催化剂是锌-空气/碘混合电池(ZAIHB)的关键问题。在这项研究中,铁钴双原子位(DAS)嵌入在生物质衍生的(N, P)杂原子共掺杂碳纳米带(NPCB)框架中,被设计为ZAIHB的多功能催化剂。理论分析表明,双原子中心的结构匹配和局部电子工程都有助于提高氧和碘化物氧化还原反应的催化活性。此外,氮(N)-和磷(P)-共掺杂的碳纳米带有助于形成高度多孔和独立的底物,这赋予了快速的动力学。得益于以上优点,FeCo DAS@NPCB在氧/碘氧化还原反应中表现出优异的多功能催化性能。采用FeCo DAS@NPCB阴极的全ZAIHB电池具有高能量效率(77.4%)和长循环寿命(超过300小时)。此外,水凝胶电解质的固态ZAIHB在充放电循环中表现出良好的柔韧性和稳定性。更令人印象深刻的是,电池在从暴露于空气到无氧环境的过渡过程中表现出高可靠性,其中氧还原反应(ORR)被碘还原反应(IRR)取代。这种独特的机制导致制造的ZAIHB具有很高的适应性,可以服务于各种工作环境。因此,本研究为多功能催化剂的设计和构建提供了一种新的策略,并促进了高效ZAIHB在各种电子领域的快速发展。
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引用次数: 0
Mo2TiC2Tx loaded core-shell structural MIL-88 derived iron-based cathode with in-situ Zn adulteration for high-performance aqueous zinc-ion batteries. Mo2TiC2Tx负载核壳结构MIL-88衍生铁基阴极的原位锌掺杂高性能水性锌离子电池。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-01 Epub Date: 2025-08-20 DOI: 10.1016/j.jcis.2025.138778
Liu Yang, Ruotong Li, Jiqing Zhang, Tao Zou, Xuekun Sui, Hongfan Huang, Yuhui Du, Enze Zhu, Xiaohui Guan, Haihui Yu, Penggang Yin, Guangsheng Wang

New-type and high-quality cathodes are of immense importance for the development of aqueous zinc-ion batteries (AZIBs). Herein, a core-shell structural iron-based metal organic framework (MIL-88) derived cathode (ZnFe2O4/Fe3O4/C@NC/Mo2TiC2Tx) with admirable specific capacity, rate performance, and cycling stability has been firstly designed and prepared. The in-situ adulterated Zn and loaded Mo2TiC2Tx MXene could effectively modulate the electron distribution, facilitating the electron transfer from Fe and Zn to O atoms, which dramatically decrease the adsorption Gibbs energy for charge carriers and improve the electrical conductivity, leading to fast electrochemical kinetics. Moreover, the structural and chemical stability of the composites could be greatly improved by integrating MIL-88 derived doped carbon, polydopamine derived N-doped carbon coating, and MXene substrate. In addition, the unique core-shell and two dimensional/three dimensional hierarchical structure could provide plentiful active sites and optimize the charge storage kinetics. The synthesized electrode exhibits more excellent specific capacity of 467.9 mAh·g-1 than that of Fe3O4/C (143.5 mAh·g-1), Fe3O4/C@NC (166.4 mAh·g-1), and ZnFe2O4/Fe3O4/C@NC (225.6 mAh·g-1), as well as eminent rate performance and cycling stability. Additionally, the improved electrochemical performance and charge storage mechanisms of the cathode are revealed by characterizations, theoretical calculations, and simulations. The high-quality cathode and its designed strategy proposed in this study would promote the development and commercialization of AZIBs.

新型高质量阴极对于水锌离子电池的发展具有十分重要的意义。本文首次设计并制备了具有良好比容量、倍率性能和循环稳定性的核壳结构铁基金属有机骨架(MIL-88)衍生阴极(ZnFe2O4/Fe3O4/C@NC/Mo2TiC2Tx)。原位掺杂Zn和负载Mo2TiC2Tx MXene可以有效地调节电子分布,促进电子从Fe和Zn向O原子转移,从而显著降低电荷载体的吸附吉布斯能,提高电导率,从而实现快速的电化学动力学。此外,MIL-88衍生掺杂碳、聚多巴胺衍生n掺杂碳涂层和MXene衬底可以大大提高复合材料的结构和化学稳定性。此外,独特的核壳结构和二维/三维层次结构可以提供丰富的活性位点,优化电荷存储动力学。该电极的比容量为467.9 mAh·g-1,优于Fe3O4/C (143.5 mAh·g-1)、Fe3O4/C@NC (166.4 mAh·g-1)和ZnFe2O4/Fe3O4/C@NC (225.6 mAh·g-1),具有优异的倍率性能和循环稳定性。此外,通过表征、理论计算和模拟,揭示了阴极的电化学性能和电荷存储机制的改进。本研究提出的高质量阴极及其设计策略将促进azib的发展和商业化。
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引用次数: 0
Multifunctional nanofiber-based electronic skin with moisture-wicking, piezoelectric motion sensing and thermochromic temperature response. 具有吸湿、压电运动传感和热致变色温度响应的多功能纳米纤维电子皮肤。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-01 Epub Date: 2025-08-18 DOI: 10.1016/j.jcis.2025.138773
Jun Zhang, Jinke Guo, Kainan Guo, Qianyue Li, Shouzhi Yan, Tingxiao Li, Binjie Xin

Electronic skin (e-skin) faces challenges in achieving long-term signal stability and wearability due to the poor breathability, sweat accumulation, and limited sensitivity. This paper reports a multifunctional nanofibrous e-skin (PTZ-PPPB-PPT) fabricated via layer-by-layer electrospinning, integrating a hydrophobic layer (PVDF-TrFE/ZnO), a piezoelectric enhancement layer (PAN/PVP/PDA@BTO), and a thermochromic layer (PAN/PVP/TCM). Benefited from the asymmetric wettability and hierarchical fiber structure, the device enables unidirectional sweat transport (contact angle reduces from 132.8° to 0° within 5.72 s) while blocking reverse osmosis (hydrostatic resistance of 40 mmH₂O). When the piezoelectric sensor operates under excessive sweating conditions, the unidirectional sweat transport maintains skin surface dryness, thereby ensuring stable piezoelectric output during movement. Notably, the E-skin achieves a high output voltage (40 V at 30 N with a sensitivity of 0.825 V/N), exhibits rapid response/recovery (100/80 ms). It also demonstrates reversible thermochromism (25-40 °C) for real-time temperature visualization. Additionally, the device ensures superior comfort during prolonged wear by maintaining exceptional air permeability (8.05 mm/s) and outstanding mechanical flexibility (187.75 % elongation at break). This multifunctional integrated E-skin synergizes sweat management with temperature visualization, holding promising potential for applications in wearable healthcare, human-computer interaction, and dynamic environmental monitoring.

电子皮肤(e-skin)由于透气性差、积汗和灵敏度有限,在实现长期信号稳定性和可穿戴性方面面临挑战。本文报道了一种由疏水性层(PVDF-TrFE/ZnO)、压电增强层(PAN/PVP/PDA@BTO)和热致变色层(PAN/PVP/TCM)组成的多层纳米纤维电子皮肤(PTZ-PPPB-PPT)。得益于非对称润湿性和分层纤维结构,该设备可以实现单向汗水传输(接触角在5.72秒内从132.8°降至0°),同时阻止反渗透(流体静力阻力为40 mmH₂O)。当压电传感器在过度出汗的条件下工作时,单向的汗液输送保持皮肤表面干燥,从而保证运动过程中稳定的压电输出。值得注意的是,E-skin实现了高输出电压(30 N时40 V,灵敏度为0.825 V/N),具有快速响应/恢复(100/80 ms)。它还具有可逆的热变色性(25-40°C),用于实时温度可视化。此外,该装置通过保持出色的透气性(8.05毫米/秒)和出色的机械灵活性(断裂伸长率187.75%),确保了长时间磨损时的卓越舒适性。这款多功能集成电子皮肤将汗液管理与温度可视化相结合,在可穿戴医疗保健、人机交互和动态环境监测方面具有广阔的应用前景。
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引用次数: 0
Li3PO4-enriched solid electrolyte interphase on Si-based anode for enhanced Li+ transport and interfacial stability in lithium batteries. 硅基阳极上富li3po4固体电解质界面相增强锂离子在锂电池中的输运和界面稳定性。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-01 Epub Date: 2025-08-16 DOI: 10.1016/j.jcis.2025.138710
Guang Ma, Chong Xu, Sai Che, Dongyuan Zhang, Shuang Liu, Junjie Fu, Gong Cheng, Ye Wang, Yang Sun, Chao Dong, Wenyue Gao, Yongfeng Li

The structure and composition of the solid electrolyte interphase (SEI) exerts a significant influence on the fast-charging capability and stability of lithium-ion batteries (LIBs). However, elucidating the design principles governing anode interfacial structures and revealing the kinetics and mechanisms of Li+ transport remain challenging. SEI layer. Herein, we present an efficient synthesis strategy for fabricating LIBs anodes consisting of silicon nanoparticles coated with a Li3PO4-modified carbon shell (Si@C@LPO). Through a combination of comprehensive experimental investigations and density functional theory (DFT) calculations, we elucidate the influence of SEI layer enriched with various inorganic components on Li+ transport. The high adsorption energy of the LiPO4-enriched SEI enhances its affinity for Li+ during the cycling process and suppresses solvent decomposition at the anode interface, thereby improving both fast-charging performance and electrode stability. Consequently, the Si@C@LPO anode exhibit a specific capacity of 605.67 mAh g-1 at 8 A g-1 and significantly enhanced cycling durability with a higher capacity retention of 73.3 % after 100 cycles at 1 A g-1. This strategy establishes a clear correlation among SEI components, Li+ transport kinetics, and the design of interfacial structures in high performance LIBs anode materials.

固体电解质界面相(SEI)的结构和组成对锂离子电池的快速充电能力和稳定性有重要影响。然而,阐明控制阳极界面结构的设计原则和揭示Li+输运的动力学和机制仍然具有挑战性。SEI层。在此,我们提出了一种高效的合成策略,用于制造由涂有li3po4修饰碳壳的硅纳米颗粒组成的lib阳极(Si@C@LPO)。通过综合实验研究和密度泛函理论(DFT)计算相结合,我们阐明了富含各种无机组分的SEI层对Li+输运的影响。富含lipo4的SEI的高吸附能增强了其在循环过程中对Li+的亲和力,抑制了阳极界面的溶剂分解,从而提高了快速充电性能和电极稳定性。因此,Si@C@LPO阳极在8 a g-1下的比容量为605.67 mAh g-1,并且在1 a g-1下循环100次后,其容量保持率高达73.3%,显着提高了循环耐久性。这一策略在SEI组分、Li+输运动力学和高性能锂离子阳极材料的界面结构设计之间建立了明确的相关性。
{"title":"Li<sub>3</sub>PO<sub>4</sub>-enriched solid electrolyte interphase on Si-based anode for enhanced Li<sup>+</sup> transport and interfacial stability in lithium batteries.","authors":"Guang Ma, Chong Xu, Sai Che, Dongyuan Zhang, Shuang Liu, Junjie Fu, Gong Cheng, Ye Wang, Yang Sun, Chao Dong, Wenyue Gao, Yongfeng Li","doi":"10.1016/j.jcis.2025.138710","DOIUrl":"10.1016/j.jcis.2025.138710","url":null,"abstract":"<p><p>The structure and composition of the solid electrolyte interphase (SEI) exerts a significant influence on the fast-charging capability and stability of lithium-ion batteries (LIBs). However, elucidating the design principles governing anode interfacial structures and revealing the kinetics and mechanisms of Li<sup>+</sup> transport remain challenging. SEI layer. Herein, we present an efficient synthesis strategy for fabricating LIBs anodes consisting of silicon nanoparticles coated with a Li<sub>3</sub>PO<sub>4</sub>-modified carbon shell (Si@C@LPO). Through a combination of comprehensive experimental investigations and density functional theory (DFT) calculations, we elucidate the influence of SEI layer enriched with various inorganic components on Li<sup>+</sup> transport. The high adsorption energy of the LiPO<sub>4</sub>-enriched SEI enhances its affinity for Li<sup>+</sup> during the cycling process and suppresses solvent decomposition at the anode interface, thereby improving both fast-charging performance and electrode stability. Consequently, the Si@C@LPO anode exhibit a specific capacity of 605.67 mAh g<sup>-1</sup> at 8 A g<sup>-1</sup> and significantly enhanced cycling durability with a higher capacity retention of 73.3 % after 100 cycles at 1 A g<sup>-1</sup>. This strategy establishes a clear correlation among SEI components, Li<sup>+</sup> transport kinetics, and the design of interfacial structures in high performance LIBs anode materials.</p>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"701 ","pages":"138710"},"PeriodicalIF":9.7,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144937794","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
Phosphate ion functionalized Ni(OH)2/Ni/MoO2 composite for enhanced alkaline hydrogen evolution. 磷酸离子功能化Ni(OH)2/Ni/MoO2复合材料增强碱性析氢。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-01 Epub Date: 2025-08-14 DOI: 10.1016/j.jcis.2025.138724
Yuyang Liu, Huiping You, Tiancheng Geng, Jing Zhang, Enlai Hu, Yining Zhang, Zhongwei Chen

The development of efficient electrocatalysts for hydrogen evolution reaction (HER) is important in advancing sustainable energy technologies. This work introduces a phosphate ion modified Ni(OH)2/Ni/MoO2 (PNNM) composite, elaborately constructed by a one-pot electrodeposition method. The integration of heterostructure engineering and ion modification strategies significantly endows the composite with remarkable electrocatalytic performance. The prepared PNNM has excellent HER activity, with a low overpotential of 35 mV to achieve a current density of 10 mA cm-2 and a favorable Tafel slope of 59.5 mV dec-1. Meanwhile, PNNM also possesses prominently long-term durability with the current density retention rate of 90.1 % after 240 h. In-situ Raman, electrochemical analysis, and theoretical calculation results reveal that the enhanced HER activity of PNNM results from the moderated hydrogen adsorption strength, robust water adsorption, and accelerated water dissociation process. This study highlights the potential of PNNM as a promising candidate for scalable alkaline hydrogen generation, offering significant advancements in renewable energy applications.

开发高效析氢电催化剂对推进可持续能源技术具有重要意义。本文介绍了一种磷酸离子修饰的Ni(OH)2/Ni/MoO2 (PNNM)复合材料,采用一锅电沉积法制备。异质结构工程和离子修饰策略的结合显著地赋予了复合材料卓越的电催化性能。制备的PNNM具有优异的HER活性,其过电位为35 mV,电流密度为10 mA cm-2, Tafel斜率为59.5 mV / dec1。同时,PNNM还具有显著的长期耐久性,240 h后电流密度保持率为90.1%。原位拉曼、电化学分析和理论计算结果表明,PNNM的HER活性增强是由于其氢吸附强度减弱、水吸附强度增强和水解离过程加快。这项研究强调了PNNM作为可扩展碱性制氢的有前途的候选物的潜力,为可再生能源的应用提供了重大进展。
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引用次数: 0
Linkage unit modulation of the polymers induces type-I to S-scheme transition in polymer/g-C3N4 heterojunctions for enhanced hydrogen evolution and chromium (VI) reduction. 聚合物的链接单元调制诱导聚合物/g-C3N4异质结中i型向s型转变,从而增强析氢和铬(VI)还原。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-01 Epub Date: 2025-08-07 DOI: 10.1016/j.jcis.2025.138661
Xiao Han, Xiujuan Zhong, Fanpeng Meng, Jinsheng Zhao, Jun Yang, Yongfa Zhu, Qian Xu, Jun Hu, Ningqiang Zhang

Building polymer heterojunctions (PHJs) is a promising way to enhance the performance of single-polymer photocatalysts, but it's still challenging to design the ideal structure with well-matched energy levels and strong interface synergy by precisely tuning the molecular structure of polymer. Herein, two triazine-based conjugated porous polymers (CPPs) were synthesized in advance including TB and TR via linkage unit modulation at the molecular level, and then their PHJs with carbon nitride (g-C3N4) nanosheet including TB/CN and TR/CN were successfully constructed by the convenient physical ball milling method. Theoretical calculations, electron paramagnetic resonance (EPR), and in situ X-ray absorption near-edge structure (XANES) spectra show that replacing thiophene rings in TR with phenyl rings in TB changes the PHJ structure from type-I (TR/CN) to an S-scheme (TB/CN) heterojunction. Compared to TR/CN, TB/CN exhibits a stronger internal electric field (IEF), better redox ability, longer exciton lifetime, and improved charge separation and transport. As a result, TB (Wang et al., 2023a (20))/CN achieves a much higher hydrogen evolution rate (HER) of 9.11 mmol g-1 h-1, which is 1.8 times of TR (Wang et al., 2023a (20))/CN and 6.6 times of pure g-C3N4. TB (Wang et al., 2023a (20))/CN also shows superior Cr(VI) reduction efficiency (98.5 % in 60 min), outperforming TR (Wang et al., 2023a (20))/CN (82.0 %) and g-C3N4 (21.8 %). This study shows that adjusting the linkage units can effectively tune the interface properties of PHJs, offering a promising strategy for designing efficient polymer-based photocatalysts.

构建聚合物异质结(PHJs)是提高单聚合物光催化剂性能的一种很有前景的方法,但通过精确调整聚合物的分子结构来设计具有良好匹配能级和强界面协同作用的理想结构仍然是一项挑战。本文首先在分子水平上通过键联单元调制,预先合成了TB和TR两种三嗪基共轭多孔聚合物(CPPs),然后通过简便的物理球磨法成功构建了含TB/CN和TR/CN的氮化碳(g-C3N4)纳米片的phj。理论计算、电子顺磁共振(EPR)和原位x射线吸收近边结构(XANES)光谱表明,用TB中的苯基环取代TR中的噻吩环使PHJ结构从i型(TR/CN)转变为s型(TB/CN)异质结。与TR/CN相比,TB/CN具有更强的内部电场(IEF)、更好的氧化还原能力、更长的激子寿命和更好的电荷分离和输运。结果表明,TB (Wang et al., 2023a (20))/CN的析氢速率(HER)为9.11 mmol g-1 h-1,是TR (Wang et al., 2023a (20))/CN的1.8倍,是纯g-C3N4的6.6倍。TB (Wang et al., 2023a (20))/CN也表现出优异的Cr(VI)还原效率(60 min内98.5%),优于TR (Wang et al., 2023a (20))/CN(82.0%)和g-C3N4(21.8%)。该研究表明,调整连接单元可以有效地调整phj的界面性质,为设计高效的聚合物基光催化剂提供了一种有前途的策略。
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引用次数: 0
Ab-initio analysis of CrX2 (X = S, Se and Te) monolayers as bifunctional electrocatalysts for oxygen reduction and evolution reaction in nonaqueous lithium-oxygen batteries. CrX2 (X = S, Se和Te)单层双功能电催化剂在非水锂氧电池中氧还原和析出反应的Ab-initio分析
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-01 Epub Date: 2025-08-19 DOI: 10.1016/j.jcis.2025.138775
Nikhil M Solanki, Suresh V Chaudhary, Gaushiya A Shaikh, Sanjeev K Gupta, P N Gajjar

Lithium-oxygen batteries are next-generation battery devices due to lightweight nature and high energy density with compared to conventional Li-ion batteries. These batteries consist a metal anode terminal and an oxygen diffused cathode terminal, in which oxygen is used as a reactant with metal atoms from surrounding air. Nonetheless, these systems facing the problems related to sluggish kinetics and higher overpotential due to formation of insoluble products at negative electrode during redox reaction. To address these major issues, the requirement of catalyst materials is raised to enhance the battery performance. Keep this in mind, we have investigated the potential of CrX2 (X = S, Se and Te) monolayer (ML) as a catalyst material for LiO2 batteries. Here, we systematically examined the stability and electronic properties of CrX2 ML using density functional theory (DFT) approach. For the dynamical and thermal stabilities, the phonon dispersion curves and ab initio molecular dynamics (AIMD) simulation were performed. All three materials exhibit outstanding conductivity and are energetically favourable for adsorption of Li atoms and O2 molecules. The initial nucleation process in all materials begins with the adsorption of Li metal and follows *Li➔*LiO2 path. Further, analysis the adsorption behaviour, structural geometries and charge distribution of LixO2y reaction intermediates during oxygen reduction reaction mechanism, show that CrX2 MLs follows four electron pathways, resulting in 2(Li2O) as the final discharge product. Additionally, we have investigated the free energy for corresponding intermediates involved in both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) process. The calculated ORR and OER overpotentials are notably low: CrS2 (0.27 V and 0.71 V), CrSe2 (0.22 V and 0.71 V) and CrTe2 (0.17 V and 0.33 V). Our results shows that CrX2 MLs are serve as high performance catalyst materials to expedite the catalytic activities for LiO2 battery systems.

与传统锂离子电池相比,锂氧电池重量轻,能量密度高,是下一代电池设备。这些电池包括一个金属阳极终端和一个氧扩散阴极终端,其中氧被用作与周围空气中的金属原子的反应物。然而,这些系统在氧化还原反应过程中由于在负极形成不溶性产物而面临动力学缓慢和过电位高的问题。针对这些主要问题,提出了提高电池性能对催化剂材料的要求。考虑到这一点,我们已经研究了CrX2 (X = S, Se和Te)单层(ML)作为LiO2电池催化剂材料的潜力。本文采用密度泛函理论(DFT)方法系统地研究了CrX2 ML的稳定性和电子性质。在动力学和热稳定性方面,进行了声子色散曲线和从头算分子动力学(AIMD)模拟。这三种材料都表现出优异的导电性,并且在能量上有利于Li原子和O2分子的吸附。所有材料的初始成核过程始于Li金属的吸附,并遵循*Li LiO2路径。进一步分析了氧还原反应机理中LixO2y反应中间体的吸附行为、结构几何形状和电荷分布,表明CrX2 MLs遵循4条电子路径,最终放电产物为2(Li2O)。此外,我们还研究了氧还原反应(ORR)和析氧反应(OER)过程中相应中间体的自由能。计算得到的ORR和OER过电位明显较低:CrS2 (0.27 V和0.71 V)、CrSe2 (0.22 V和0.71 V)和CrTe2 (0.17 V和0.33 V)。研究结果表明,CrX2 MLs是一种高性能的催化剂材料,可以加快LiO2电池系统的催化活性。
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引用次数: 0
Integrating inorganic Zn-ion conductor with nanocellulose towards separator-free and long-life aqueous zinc ion batteries. 无机锌离子导体与纳米纤维素相结合制备无分离器长寿命水性锌离子电池。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-01 Epub Date: 2025-08-06 DOI: 10.1016/j.jcis.2025.138635
Jingxuan Yu, Minfeng Chen, Hong Ma, Wenhui Liu, Qinghua Tian, Jizhang Chen

Aqueous zinc-ion batteries (AZIBs) have emerged as a promising energy storage system due to their inherent safety, cost-effectiveness, large power density, and environmental sustainability. However, the widespread adoption of AZIBs is impeded by critical challenges associated with zinc anodes, including uncontrolled dendrite growth, hydrogen evolution, and corrosion, as well as the reliance on thick separators that reduce the battery's energy density. To overcome these limitations, this study introduces a separator-free AZIB design featuring a multifunctional protective coating composed of zinc monofluorophosphate and nanocellulose on the Zn electrode. The hybrid coating with a low thickness of 15 μm serves a dual purpose, not only mitigating dendrite formation and parasitic reactions but also eliminating the need for conventional separators. The electrochemical characterization reveals that the hybrid coating enables superior corrosion resistance, extended electrochemical stability window, improved Zn2+ ion transport, facilitated desolvation process, lowered overpotential, and uniformized Zn deposition. Thanks to these benefits, the Zn//Zn cell offers a long life span up to 1200 h at 10 mA cm-2 and 2 mAh cm-2, and the full battery delivers great rate capability and cycling stability even under a low negative-to-positive capacity ratio. This work provides an appropriate solution to the development of high-energy-density and durable AZIBs.

水性锌离子电池(azib)由于其固有的安全性、成本效益、大功率密度和环境可持续性而成为一种有前途的储能系统。然而,azib的广泛采用受到锌阳极相关的关键挑战的阻碍,包括不受控制的枝晶生长、析氢和腐蚀,以及对降低电池能量密度的厚隔板的依赖。为了克服这些限制,本研究引入了一种无分离器的AZIB设计,其特点是在锌电极上具有由单氟磷酸锌和纳米纤维素组成的多功能保护涂层。这种厚度为15 μm的混合涂层具有双重用途,不仅可以减少枝晶的形成和寄生反应,还可以消除对传统分离器的需求。电化学表征表明,杂化涂层具有优异的耐腐蚀性,延长了电化学稳定窗口,改善了Zn2+离子的传输,促进了脱溶过程,降低了过电位,使锌沉积均匀。由于这些优点,Zn//Zn电池在10 mA cm-2和2 mAh cm-2下可提供长达1200小时的长寿命,并且即使在低负极容量比下,全电池也能提供出色的倍率能力和循环稳定性。这项工作为开发高能量密度和耐用的azib提供了合适的解决方案。
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引用次数: 0
Facet-selective synthesis of cadmium sulfide photocatalysts for high-efficiency CO2 conversion. 高效CO2转化用硫化镉光催化剂的面选择性合成。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-01 Epub Date: 2025-08-14 DOI: 10.1016/j.jcis.2025.138723
Xingwang Zhu, Xiang Liu, Xiang Shi, Fujiang Huang, Hangmin Xu, Ganghua Zhou, Xiaozhi Wang, Xu Dong, Penghui Ding, Jianning Ding, Hui Xu

The surface of photocatalysts plays a key role in the adsorption and activation of CO2 molecules. Establishing the conformational relationship between the crystalline phase of the photocatalysts and the CO2 reduction reaction (CO2RR) activity is crucial to understanding the catalytic reaction mechanism. Herein, we synthesized CdS catalysts with different exposed crystalline facets (CdS[100], CdS[001], and CdS[111]) using hydrothermal and water bath methods and evaluated their photocatalytic CO2RR performances. The results showed that CdS[001] displayed an optimal activity with a 203.2 μmol g-1 h-1 of CO generation rate compared with CdS[100] and CdS[111]. More importantly, the CdS[001] catalyst shows the best CO selectivity (SCO: ∼86.6 %) and CO2 reduction selectivity (SCO2: ∼95.4 %) compared with CdS[100] (SCO: 79.3 %; SCO2: 90.0 %) and CdS[111] (SCO: 79.6 %; SCO2: 82.8 %). The optimal CdS[001] catalyst significantly inhibited the competing hydrogen evolution reaction. The adsorption and activation behaviors of CO2 on various exposed surfaces of CdS are explored in depth based on density functional theory calculations and in-situ Fourier transform infrared spectra measurements. This work provides new insights into understanding the role of facet control in enhancing photocatalytic CO2 conversion.

光催化剂的表面对CO2分子的吸附和活化起着关键作用。建立光催化剂的晶相与CO2还原反应(CO2RR)活性之间的构象关系对理解催化反应机理至关重要。本文采用水热法和水浴法合成了不同暴露晶面的CdS催化剂(CdS[100]、CdS[001]和CdS[111]),并对其光催化CO2RR性能进行了评价。结果表明,与CdS[100]和CdS[111]相比,CdS[001]的CO生成速率为203.2 μmol g-1 h-1,表现出最佳活性。更重要的是,与CdS[100] (SCO: 79.3%; SCO2: 90.0%)和CdS[111] (SCO: 79.6%; SCO2: 82.8%)相比,CdS[001]催化剂表现出最好的CO选择性(SCO: ~ 86.6%)和CO2还原选择性(SCO2: ~ 95.4%)。优选的CdS[001]催化剂显著抑制了竞争性析氢反应。基于密度泛函理论计算和现场傅立叶变换红外光谱测量,深入探讨了CO2在CdS不同暴露表面的吸附和活化行为。这项工作为理解facet控制在增强光催化CO2转化中的作用提供了新的见解。
{"title":"Facet-selective synthesis of cadmium sulfide photocatalysts for high-efficiency CO<sub>2</sub> conversion.","authors":"Xingwang Zhu, Xiang Liu, Xiang Shi, Fujiang Huang, Hangmin Xu, Ganghua Zhou, Xiaozhi Wang, Xu Dong, Penghui Ding, Jianning Ding, Hui Xu","doi":"10.1016/j.jcis.2025.138723","DOIUrl":"10.1016/j.jcis.2025.138723","url":null,"abstract":"<p><p>The surface of photocatalysts plays a key role in the adsorption and activation of CO<sub>2</sub> molecules. Establishing the conformational relationship between the crystalline phase of the photocatalysts and the CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) activity is crucial to understanding the catalytic reaction mechanism. Herein, we synthesized CdS catalysts with different exposed crystalline facets (CdS[100], CdS[001], and CdS[111]) using hydrothermal and water bath methods and evaluated their photocatalytic CO<sub>2</sub>RR performances. The results showed that CdS[001] displayed an optimal activity with a 203.2 μmol g<sup>-1</sup> h<sup>-1</sup> of CO generation rate compared with CdS[100] and CdS[111]. More importantly, the CdS[001] catalyst shows the best CO selectivity (S<sub>CO</sub>: ∼86.6 %) and CO<sub>2</sub> reduction selectivity (S<sub>CO2</sub>: ∼95.4 %) compared with CdS[100] (S<sub>CO</sub>: 79.3 %; S<sub>CO2</sub>: 90.0 %) and CdS[111] (S<sub>CO</sub>: 79.6 %; S<sub>CO2</sub>: 82.8 %). The optimal CdS[001] catalyst significantly inhibited the competing hydrogen evolution reaction. The adsorption and activation behaviors of CO<sub>2</sub> on various exposed surfaces of CdS are explored in depth based on density functional theory calculations and in-situ Fourier transform infrared spectra measurements. This work provides new insights into understanding the role of facet control in enhancing photocatalytic CO<sub>2</sub> conversion.</p>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"701 ","pages":"138723"},"PeriodicalIF":9.7,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144937819","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
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Journal of Colloid and Interface Science
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