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Boosting the Capacity and Life-span of Zn-Supplied Cathode in “Rocking-Chair” Aqueous Zn-Ion Batteries by Vanadium-Manganese Coupling Strategy 通过钒锰耦合策略提高 "摇椅式 "锌离子水电池中锌供应阴极的容量和寿命
IF 9.3 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-19 DOI: 10.1016/j.mtener.2024.101505
Jian Wu, Quan Kuang, Pan Jiang, Minghui Huang, Jixiang Wei, Qinghua Fan, Youzhong Dong, Yanming Zhao

Owing to the scarcity of eminent Zn-supplied cathodes, traditional aqueous Zn-ion batteries (AZIBs) still pins the hope on unstable Zn-metal anode to supply charge carriers, thus suffering from the dendrite growth and side reactions. Herein, by vanadium-manganese coupling in the spinel matrix, Zn2.5Mn0.5V3O8, a Zn2+ supplied cathode material with outstanding performance, has been prepared to completely get rid of the dependence on Zn-metal anode. Concretely, it delivers a high specific capacity of 355 mA•h g-1 at 200 mA g-1 and comforting retention of 75.7 % after 4500 cycles at 5 A g-1. The energy storage mechanism can be summarized as two-step phase transformation in the first charge process, and the intercalation of Zn2+/H+ into host structure accomplished with a conversion reaction in the subsequent cycles. After discarding the Zn-metal anode, a “rocking-chair” AZIB of Zn2.5Mn0.5V3O8 // anthraquinone has been established, in which Zn2.5Mn0.5V3O8 exhibits the superb specific capacities (190.9 mA•h g-1 at 200 mA g-1) and stable cycling performance (80.8% after 1000 cycles at 200 mA g-1 and 96.4% after 1000 cycles at 2.0 A g-1). This work may accelerate the development of both traditional and “rocking-chair” aqueous batteries.

传统的锌离子水溶液电池(AZIBs)由于缺乏优秀的锌负极材料,仍然寄希望于不稳定的锌金属负极来提供电荷载体,因而饱受枝晶生长和副反应的困扰。在这里,通过在尖晶石基体中进行钒锰耦合,制备出了性能优异的 Zn2+ 负极材料 Zn2.5Mn0.5V3O8,彻底摆脱了对 Zn 金属负极的依赖。具体而言,在 200 mA g-1 电流条件下,它能提供 355 mA-h g-1 的高比容量,在 5 A g-1 电流条件下循环 4500 次后,其舒适度保持率为 75.7%。其储能机理可概括为:在第一次充电过程中发生两步相变,在随后的循环中通过转换反应将 Zn2+/H+ 插层到宿主结构中。在摒弃了锌-金属阳极后,建立了一种 Zn2.5Mn0.5V3O8 // anthraquinone 的 "摇椅式 "AZIB,其中 Zn2.5Mn0.5V3O8 表现出超强的比容量(200 mA g-1 时为 190.9 mA-h g-1)和稳定的循环性能(200 mA g-1 时循环 1000 次后为 80.8%,2.0 A g-1 时循环 1000 次后为 96.4%)。这项工作可能会加速传统电池和 "摇椅 "水电池的开发。
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引用次数: 0
Cooperative Co Single Atoms and Co2P Nanoparticles as Catalytic Tandem for Boosting Redox Kinetics in Li–S Batteries 合作钴单原子和 Co2P 纳米粒子作为催化剂串联促进锂-S 电池的氧化还原动力学
IF 9.3 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-18 DOI: 10.1016/j.mtener.2024.101504
Haorui Zhao, Qin Yang, Daming Zhu, Wenqiang Yang, Zixiong Shi, Xia Li, Yifan Ding, Wenyi Guo, Jiaxi Gu, Yingze Song, Jingyu Sun

Notorious shuttle effect and sluggish redox kinetics as major bottlenecks have nowadays hindered the commercial implementation of lithium–sulfur batteries. The activity design of catalysts has attracted increasing attention in this realm thus far. Herein, we devise a Co-based electrocatalytic tandem (Co–N–P) encompassing (N,P)-coordinated Co single atoms and Co2P nanoparticles for guiding the dual-directional sulfur evolution reactions. Such a Co–N–P tandem synergizes high atom utilization, large catalyst loading and smooth charge migration, thereby resulting in the high activity for dictating the Li2S nucleation and decomposition. As a result, the full cell incorporating the Co–N–P modified separator harvests 0.1% capacity decay after 500 cycles at 1.0 C. In addition, a favorable areal capacity output of 4.2 mAh cm–2 is obtained under a sulfur loading of 5.3 mg cm–2. We anticipate that this work would offer insight into the hybrid catalyst design affording high activity and stability for emerging energy applications.

众所周知的穿梭效应和缓慢的氧化还原动力学是目前锂硫电池商业化的主要瓶颈。迄今为止,催化剂的活性设计在这一领域引起了越来越多的关注。在此,我们设计了一种 Co 基电催化串联(Co-N-P),其中包括(N,P)配位 Co 单原子和 Co2P 纳米颗粒,用于引导双向硫进化反应。这种 Co-N-P 串联协同提高了原子利用率、催化剂负载量和电荷迁移的平稳性,从而产生了支配 Li2S 成核和分解的高活性。此外,在 5.3 毫克/厘米-2 的硫负载条件下,还能获得 4.2 毫安时/厘米-2 的良好面积容量输出。我们希望这项研究能为新兴能源应用领域提供高活性和高稳定性的混合催化剂设计。
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引用次数: 0
Environmental energy harvesting boosts self-powered sensing 环境能量采集推动自供电传感技术发展
IF 9.3 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-17 DOI: 10.1016/j.mtener.2024.101502
Hongchun Luo, Tao Yang, Xingjian Jing, Yingxuan Cui, Weiyang Qin

Self-powered sensing technology has extremely important application value in many areas, like healthcare, meteorology, internet of things (IoT) and so on. The progress of energy harvesting technology suitable for various environments is essential for the advancement of self-powered sensors. Mechanical energy has the characteristics of wide distribution, diverse forms and dispersion. The efficient collection of environmental energy is always a difficult problem in the development of self-power supply technology. In this paper, the latest research progress of mechanical energy acquisition technology, the development of self-powered sensors, the methods to improve the efficiency of energy acquisition and the key technical problems of self-powered sensors are reviewed. Especially the latest progresses in improving the output and mechanical stability of piezoelectric, magnetoelectric, triboelectric, thermoelectric nanogenerators are discussed, including nonlinear structure design, resonant tuning technology, power management circuit design, new material preparation, hybrid energy harvesting. Finally, the application prospect and future development of self-powered sensing are discussed.

自供电传感技术在许多领域都具有极其重要的应用价值,如医疗保健、气象、物联网(IoT)等。适合各种环境的能量采集技术的进步对于自供电传感器的发展至关重要。机械能具有分布广泛、形式多样和分散等特点。如何有效收集环境能量一直是自供电技术发展中的难题。本文综述了机械能采集技术的最新研究进展、自供电传感器的发展、提高能量采集效率的方法以及自供电传感器的关键技术问题。特别讨论了提高压电、磁电、三电、热电纳米发电机输出和机械稳定性的最新进展,包括非线性结构设计、谐振调谐技术、电源管理电路设计、新材料制备、混合能量采集等。最后,讨论了自供电传感的应用前景和未来发展。
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引用次数: 0
Recent advances of tailoring defects and pores in hard carbon for sodium storage 定制硬碳中的缺陷和孔隙以储存钠的最新进展
IF 9.3 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-13 DOI: 10.1016/j.mtener.2024.101501
Chenyang Huang, Junyi Yin, Weichen Shi, Yonghong Cheng, Xin Xu

Sodium-ion batteries (SIBs) are promising alternatives for Lithium-ion batteries in the field of large-scale energy storage for abundant sodium resources. Hard Carbons (HCs) are the most commonly used anode materials of SIBs for balanced electrochemical performance. The major challenges lie in low initial coulombic efficiency (ICE), insufficient reversible capacity, and the costs. Defects, pores, and graphitization degree are the main characteristics of HCs. The synergistic effects of defects and pores decide the surface adsorption distribution of electrolytes and the real electrochemical active area, which determine the solid-electrolyte interface formation process and ICE values. Sodium cluster stored in closed pores contributes to low-voltage plateau capacity with high reversibility. Suitable defect distribution on the inner wall of the closed pores ensures stable cluster formation. This review focuses on the defects and pores of HC and corresponding modification strategies, which are highlighted by their synergistic effects. We expect to offer valuable guidance for constructing next-generation HC anodes.

钠离子电池(SIB)是锂离子电池的替代品,在大规模储能领域具有广阔的前景,因为钠资源丰富。硬碳(HC)是钠离子电池最常用的阳极材料,具有均衡的电化学性能。其主要挑战在于初始库仑效率(ICE)低、可逆容量不足以及成本高。缺陷、孔隙和石墨化程度是碳氢化合物的主要特征。缺陷和孔隙的协同作用决定了电解质的表面吸附分布和实际电化学活性面积,从而决定了固体-电解质界面的形成过程和 ICE 值。储存在封闭孔隙中的钠簇有助于形成具有高可逆性的低电压高原容量。封闭孔隙内壁上适当的缺陷分布可确保簇的稳定形成。本综述重点介绍了碳氢化合物的缺陷和孔隙以及相应的改性策略,这些策略的协同效应突出了碳氢化合物的缺陷和孔隙。我们希望能为构建下一代碳氢化合物阳极提供有价值的指导。
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引用次数: 0
Novel S-scheme Bi24O31Cl10/Bi7Fe2Ti2O17Cl Heterojunction for Efficient and Stable Photocatalytic Activities 新型 S 型 Bi24O31Cl10/Bi7Fe2Ti2O17Cl 异质结实现高效稳定的光催化活性
IF 9.3 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-13 DOI: 10.1016/j.mtener.2024.101498
Yunxiang Zhang, Zhichao Mu, Chenliang Zhou, Zhe Zhang, Zhili Chen, Xiangyu Cheng, Hazem Abdelsalam, Wei Chen, Diab Khalafallah, Qinfang Zhang

The strategy to boost photocatalytic activities towards CO2 reduction and organic pollutants degradation is still a key challenge for novel Sillén-Aurivillius oxyhalides. In this work, a S-scheme heterojunction of Bi24O31Cl10 and Bi7Fe2Ti2O17Cl is designed for CO2 reduction and organic pollutants degradation. The as-synthesized 5% Bi24O31Cl10/Bi7Fe2Ti2O17Cl (BOC/BFTOC-5) composites depicts an appealing CO2 reduction and removal rate for RhB organic pollutants in comparison with pristine Bi24O31Cl10 and Bi7Fe2Ti2O17Cl oxyhalides. This fascinating photocatalytic performance could be ascribed to the synergic effect of the enhanced visible light adsorption and photo-generated carriers separation derived from the Bi24O31Cl10/Bi7Fe2Ti2O17Cl heterojunction. Simultaneously, the trapping experiments confirm that the main active species during the catalytic process are the photo-generated hole (h+) and the hydroxy free radical (·OH). This work aims at providing a S-scheme heterojunction via Bi-based oxyhalides for efficient photocatalytic activity.

对于新型 Sillén-Aurivillius 氧卤化物来说,提高光催化活性以实现二氧化碳还原和有机污染物降解的策略仍然是一个关键挑战。本研究设计了 Bi24O31Cl10 和 Bi7Fe2Ti2O17Cl 的 S 型异质结,用于还原二氧化碳和降解有机污染物。与原始的 Bi24O31Cl10 和 Bi7Fe2Ti2O17Cl 氧卤化物相比,合成的 5% Bi24O31Cl10/Bi7Fe2Ti2O17Cl (BOC/BFTOC-5)复合材料的二氧化碳还原率和 RhB 有机污染物的去除率都很高。这种迷人的光催化性能可归因于 Bi24O31Cl10/Bi7Fe2Ti2O17Cl 异质结所产生的增强可见光吸附和光生载流子分离的协同效应。同时,捕获实验证实,催化过程中的主要活性物种是光生空穴(h+)和羟基自由基(-OH)。这项工作旨在通过 Bi 基氧卤化物提供一种 S 型异质结,以实现高效的光催化活性。
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引用次数: 0
Improving the Ohmic polarization of high temperature proton exchange membrane fuel cells using crosslinked polybenzimidazole membranes containing acidophilic quaternary ammonium groups synthesized by one-step strategy 利用一步法合成的含有亲酸性季铵基团的交联聚苯并咪唑膜改善高温质子交换膜燃料电池的欧姆极化性能
IF 9.3 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-11 DOI: 10.1016/j.mtener.2024.101499
Jin Li, Guoliang Liu, Fangfang Zhang, Jun Liao, Haolin Tang, Haining Zhang

Ingenious crosslinked network structure in phosphoric acid doped polybenzimidazole membranes can mitigate the mutual restriction of proton conductivity and mechanical properties. However, the complicated synthesis of tailored macromolecular crosslinker and the time-consuming post-treatment hinder their practical application as high temperature proton exchange membranes. Herein, crosslinked polybenzimidazole membranes are synthesized using small molecular crosslinker containing acidophilic quaternary ammonium groups through a one-step crosslinking strategy. After doping with phosphoric acid, the quaternary ammonium-biphosphate ion-pair coordination and the crosslinked structure result in the improved anhydrous proton conductivity, oxidation stability, and mechanical strength of the formed membranes compared to sample without crosslinking structure. Membrane with the optimized degree of crosslinking exhibits an anhydrous conductivity of 72.27 mS cm-1 at 160 °C with a tensile strength of 12.14 MPa. Benefiting from the crosslinked structure and high proton conductivity, the accordingly formed membrane electrode assembly possesses a high open circuit voltage of 1.01 V and the improved Ohmic polarization, delivering a peak power density of 0.66 W cm-2 using hydrogen as fuel and air as oxidant.

掺杂磷酸的聚苯并咪唑膜中巧妙的交联网络结构可以缓解质子传导性和机械性能之间的相互限制。然而,定制大分子交联剂的复杂合成和耗时的后处理阻碍了其作为高温质子交换膜的实际应用。本文采用一步交联策略,使用含有亲酸性季铵基团的小分子交联剂合成了交联聚苯并咪唑膜。在掺入磷酸后,季铵-二磷酸离子对配位和交联结构使形成的膜与无交联结构的样品相比,在无水质子传导性、氧化稳定性和机械强度方面都得到了改善。具有优化交联度的膜在 160 °C 时的无水电导率为 72.27 mS cm-1,抗拉强度为 12.14 MPa。得益于交联结构和高质子传导性,相应形成的膜电极组件具有 1.01 V 的高开路电压和改进的欧姆极化,使用氢气作为燃料和空气作为氧化剂可提供 0.66 W cm-2 的峰值功率密度。
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引用次数: 0
Carbon nanotube-bridged MXene nanoarchitectures decorated with ultrasmall Rh nanoparticles for efficient methanol oxidation 用超小型 Rh 纳米粒子装饰的碳纳米管桥接 MXene 纳米结构用于高效甲醇氧化
IF 9.3 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-10 DOI: 10.1016/j.mtener.2024.101495
Yan Wang, Xiang Yang, Yike Zhang, Chi Zhang, Lu Yang, Quanguo Jiang, Haiyan He, Guobing Ying, Huajie Huang

Rational design and precise synthesis of cost-effective and highly-active Pt-alternative anode catalysts are important paths to accelerate the application and promotion of direct methanol fuel cell. Herein, a robust and controllable synthetic strategy is developed to the bottom-up construction of carbon nanotube-bridged Ti3C2Tx MXene nanoarchitectures decorated with ultrasmall Rh nanoparticles (Rh/CNT-MX) through a facile co-assembly process. The existence of MXene nanosheets with abundant anchoring sites can immobilize nanosized Rh crystals and facilitate their dispersion, while the integration of CNT skeletons effectively separates the neighboring MXene layers and offers unimpeded electron transport channels, which are conducive to making full use of respective catalytic functions for each component. As a consequence, the optimized Rh/CNT-MX catalyst expresses superior methanol oxidation performance with a considerable electrochemically active surface area of 89.4 m2 g-1, high mass/specific activity of 911.0 mA mg-1/1.02 mA cm-2, and reliable long-term durability, which has obvious competitive advantages over the conventional Rh/carbon black, Rh/CNT, Rh/MXene as well as commercial Pt/carbon black and Pd/carbon black catalysts.

合理设计和精确合成高性价比、高活性的铂替代阳极催化剂是加速直接甲醇燃料电池应用和推广的重要途径。本文开发了一种稳健、可控的合成策略,通过简便的共组装工艺,自下而上地构建了以超小型 Rh 纳米颗粒为装饰的碳纳米管桥接 Ti3C2Tx MXene 纳米结构(Rh/CNT-MX)。具有丰富锚定位点的 MXene 纳米片能够固定纳米级 Rh 晶体并促进其分散,而 CNT 骨架的集成则有效地分隔了相邻的 MXene 层,并提供了畅通无阻的电子传输通道,有利于充分发挥各组分各自的催化功能。因此,优化后的 Rh/CNT-MX 催化剂具有优异的甲醇氧化性能,其电化学活性表面积高达 89.4 m2 g-1,质量/比活度高达 911.0 mA mg-1/1.02 mA cm-2,并具有可靠的长期耐久性,与传统的 Rh/炭黑、Rh/CNT、Rh/MXene 以及商用的 Pt/ 炭黑和 Pd/ 炭黑催化剂相比具有明显的竞争优势。
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引用次数: 0
Human-friendly flexible solid-state biodegradable supercapacitor based on Ti3C2Tx MXene film without adhesive structure 基于无粘合剂结构 Ti3C2Tx MXene 薄膜的人体友好型柔性固态可生物降解超级电容器
IF 9.3 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-09 DOI: 10.1016/j.mtener.2024.101496
Xiaofeng Zhang, Muhammad Sufyan Javed, Hongjia Ren, Xinze Zhang, Salamat Ali, Kaiming Han, Awais Ahmad, Ammar M. Tighezza, Weihua Han, Kui-Qing Peng

With the rapid development of biomedical technology, biodegradable and implantable energy storage devices for biosensor and bioelectronics applications have attracted the great attention of scientists. However, the limited energy density, poor biocompatibility and excessive space occupation of existing biodegradable energy storage devices pose major challenges to their application in the biomedical field. To address these challenges, in this work, flexible Ti3C2Tx film with an adhesive-free structure constructed is proposed as electrode material for the flexible solid-state biodegradable supercapacitor (FSBSC). The morphology and structure of MXene films were characterized by XRD, XPS, Raman, SEM and TEM. A 0.9% NaCl saline, similar human body fluids was used as the electrolyte solution to construct symmetrical FSBSC (Ti3C2Tx//NaCl-PVA//Ti3C2Tx-FSBSC). The Ti3C2Tx//NaCl-PVA//Ti3C2Tx-FSBSC exhibits a high capacitance of 112 F/g at 1 A/g, excellent rate capability (73.2% at 20 A/g), long lifetime (81.6 % after 10,000 cycles), and high specific energy/power (62.3 Wh/kg at 1,000.8 W/kg). The charge storage mechanism was analyzed using ex-situ XRD, XPS and density function theory (DFT). DFT results show that the Ti3C2Tx (Tx = O)) electrode possesses metallic properties. The calculated adsorption energies (Eads) and smaller diffusion barriers of Na+-ions further proved the outstanding performance of the Ti3C2Tx electrode. Moreover, the apparatus is entirely biodegradable, thereby paving a promising path for the progression of bioelectronics and biomedical energy storage technologies.

随着生物医学技术的飞速发展,用于生物传感器和生物电子学的可生物降解和植入式储能器件引起了科学家们的极大关注。然而,现有生物可降解储能器件的能量密度有限、生物相容性差、占用空间过大等问题给其在生物医学领域的应用带来了巨大挑战。为了应对这些挑战,本研究提出了无粘合剂结构的柔性 Ti3C2Tx 薄膜作为柔性固态生物可降解超级电容器(FSBSC)的电极材料。通过 XRD、XPS、拉曼、扫描电镜和 TEM 对 MXene 薄膜的形貌和结构进行了表征。以类似人体体液的 0.9% 氯化钠生理盐水作为电解质溶液,构建了对称的 FSBSC(Ti3C2Tx//NaCl-PVA//Ti3C2Tx-FSBSC)。Ti3C2Tx//NaCl-PVA//Ti3C2Tx-FSBSC 在 1 A/g 时具有 112 F/g 的高电容、出色的速率能力(20 A/g 时为 73.2%)、长寿命(10,000 次循环后为 81.6%)和高比能量/功率(1,000.8 W/kg 时为 62.3 Wh/kg)。利用原位 XRD、XPS 和密度函数理论(DFT)分析了电荷存储机制。DFT 结果表明,Ti3C2Tx(Tx = O)电极具有金属特性。计算得出的吸附能(Eads)和较小的 Na+ 离子扩散障碍进一步证明了 Ti3C2Tx 电极的卓越性能。此外,该装置完全可生物降解,从而为生物电子学和生物医学储能技术的发展铺平了道路。
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引用次数: 0
Enhancing Lithium-Sulfur Battery Performance through Electronic/Ionic Co-Conductive MWCNTs/LLTO Separator Modification 通过电子/离子共导 MWCNT/LLTO 隔膜改性提高锂硫电池性能
IF 9.3 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-09 DOI: 10.1016/j.mtener.2024.101497
Shanshan Liang, Susana Chauque, Marco Ricci, Remo Proietti Zaccaria

As one of the most promising energy storage devices, Lithium-sulfur batteries (LSBs or Li-S batteries) are still facing obstacles due to the notorious shuttling of soluble polysulfide intermediates, accompanied by low S utilization, corrosion of the lithium anode, and rapid capacity fading leading to a short cycling life. To overcome these issues and achieve high-performance LSBs, we introduce a modified separator composed of multi-walled carbon nanotubes/lithium lanthanum titanium oxide (MWCNTs/LLTO). The proposed MWCNTs/LLTO-modified separator improves the redox reaction kinetics from soluble higher-order lithium polysulfides to the insoluble lower-order ones and ultimately to Li2S, thereby reducing the polysulfides dissolved in the electrolyte. It also serves as a physical barrier to adsorb polysulfides, efficiently preventing their diffusion from the cathode to the anode. LSBs adopting the MWCNTs/LLTO-modified separator exhibit higher ionic and electronic conductivity than the un-modified counterparts, leading to an initial specific capacity of 1496 mA h g−1 (∼90% of the theoretical capacity) at 0.1C, an excellent rate capability performance, and a remarkable capacity retention of 80% after 200 cycles. Furthermore, the cells with S loading reaching up to 4.18 mg cm-2 further confirmed the beneficial impact of the MWCNTs/LLTO-modified separator.

作为最有前途的储能设备之一,锂硫电池(LSBs 或 Li-S 电池)仍然面临着各种障碍,因为可溶性多硫化物中间体的穿梭是众所周知的,同时还伴随着 S 利用率低、锂阳极腐蚀以及容量快速衰减导致循环寿命短等问题。为了克服这些问题并实现高性能的 LSB,我们引入了一种由多壁碳纳米管/锂镧钛氧化物(MWCNTs/LLTO)组成的改良隔膜。所提出的 MWCNTs/LLTO 改性隔膜改善了从可溶的高阶多硫化锂到不溶的低阶多硫化锂,最终到 Li2S 的氧化还原反应动力学,从而减少了溶解在电解液中的多硫化物。它还可作为吸附多硫化物的物理屏障,有效阻止多硫化物从阴极向阳极扩散。采用 MWCNTs/LLTO 改性隔膜的 LSB 比未改性的 LSB 具有更高的离子导电性和电子导电性,因此在 0.1C 时的初始比容量为 1496 mA h g-1(理论容量的 90%),具有出色的速率性能,在 200 个循环后的容量保持率高达 80%。此外,S 负载高达 4.18 mg cm-2 的电池进一步证实了 MWCNTs/LLTO 改性隔膜的有利影响。
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引用次数: 0
PdOs bimetallene for energy-saving hydrogen production coupled with ethanol electro-oxidation 结合乙醇电氧化工艺的 PdOs 双金属节能制氢技术
IF 9.3 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-06 DOI: 10.1016/j.mtener.2024.101493
Ziqiang Wang, Min Li, Shan Xu, Hongjie Ye, Kai Deng, You Xu, Hongjing Wang, Liang Wang

The replacement of sluggish oxygen evolution reaction by more thermodynamically favorable ethanol oxidation reaction (EOR) is a promising strategy for co-production of hydrogen and valuable chemicals in energy-saving mode. Here, we propose the synthesis of highly curved PdOs bimetallene, which possesses high active sites atomic utilization and conductivity. Furthermore, alloy effect can regulate electronic structure and optimize adsorption energy of reactants. Therefore, PdOs bimetallene exhibits superior performance for hydrogen evolution reaction (HER) and EOR under basic solutions, with overpotential of 36 mV at 10 mA cm-2 and mass activity of 1.51 mA μg-1Pd, respectively. In the EOR-HER co-electrolysis system, PdOs bimetallene requires low voltage of 0.801 V for concurrent production of hydrogen and acetate at 50 mA cm−2, which greatly reduces energy consumption compared to conventional water electrolysis (1.976 V). This method provides a promising strategy for designing bimetallic electrocatalysts towards simultaneous energy-saving generation of hydrogen and high-value chemicals by replacing sluggish OER with more favorable ethanol oxidation reaction.

用热力学上更有利的乙醇氧化反应(EOR)取代缓慢的氧进化反应,是一种以节能模式联合生产氢气和有价值化学品的有前途的战略。在此,我们提出了高弯曲 PdOs 双金属的合成方法,它具有高活性位点原子利用率和导电性。此外,合金效应可以调节电子结构,优化反应物的吸附能。因此,在碱性溶液条件下,PdOs 双茂钛在氢进化反应(HER)和 EOR 方面表现出卓越的性能,在 10 mA cm-2 条件下的过电位为 36 mV,质量活度为 1.51 mA μg-1Pd。在 EOR-HER 共电解系统中,PdOs 双茂钛需要 0.801 V 的低电压才能在 50 mA cm-2 的条件下同时产生氢气和醋酸盐,与传统的水电解(1.976 V)相比,大大降低了能耗。这种方法为设计双金属电催化剂提供了一种前景广阔的策略,通过用更有利的乙醇氧化反应取代迟缓的 OER,从而实现同时生成氢气和高价值化学品的节能目标。
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引用次数: 0
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Materials Today Energy
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