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Stable and ligand-free gold nanoparticles produced by laser ablation as efficient electrocatalysts for electrochemical sensing of dopamine 激光烧蚀制备稳定无配体金纳米颗粒作为多巴胺电化学传感的高效电催化剂
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-10-15 Epub Date: 2023-08-23 DOI: 10.1016/j.jelechem.2023.117744
L.S. De Bortoli , C.R. Vanoni , C.L. Jost , D.Z. Mezalira , M.C. Fredel

The possibility of producing high-purity and ligand-free nanoparticles makes laser ablation in liquids (LAL) an interesting method to produce gold nanoparticles (AuNPs). AuNPs play an important role in the manufacture of electrochemical sensors due to their excellent electrical conductivity and chemical stability. In this study, stable and ligand-free AuNPs were produced by LAL (AuNP/LAL) using a nanosecond pulsed laser. The control of this single-step production was facilitated by adding sodium chloride (NaCl), resulting in the reduction of AuNPs size (10 ± 2 nm) and higher stability (monitored for 12 weeks). The potential of NaCl-stabilized AuNPs/LAL as modifiers agents were investigated for dopamine (DA) sensing by cyclic voltammetry for the first time. The novel electrochemical sensor (GCE/AuNPs.LAL/Nafion) achieved an increase in the peak current of ca. 3 and 6 times for oxidation and reduction, respectively. A comparison of chemical syntheses and LAL approaches was given for electrochemical sensing applications; the AuNPs/LAL showed to be more efficient in facilitating the electronic transfer and electrocatalytic reactions. The estimated limit of detection values for DA sensing was 0.77 µmol/L (oxidation) and 1.08 µmol/L (reduction). The method hereby proposed is promising for clinical applications as the new electrochemical sensor allowed proper sensitivity for DA.

制备高纯度和无配体纳米颗粒的可能性使液体激光烧蚀(LAL)成为一种有趣的制备金纳米颗粒(AuNPs)的方法。aunp由于其优异的导电性和化学稳定性,在电化学传感器的制造中发挥着重要作用。本研究利用纳秒脉冲激光制备了稳定且无配体的AuNP (AuNP/LAL)。通过添加氯化钠(NaCl)控制单步生产,使AuNPs尺寸减小(10±2 nm),稳定性提高(监测12周)。首次利用循环伏安法研究了nacl稳定AuNPs/LAL作为多巴胺(DA)传感改性剂的潜力。新型电化学传感器(GCE/AuNPs.LAL/Nafion)的氧化和还原峰值电流分别提高了约3倍和6倍。比较了化学合成法和LAL法在电化学传感中的应用;AuNPs/LAL在促进电子转移和电催化反应方面更有效。估计DA传感的检出限为0.77µmol/L(氧化)和1.08µmol/L(还原)。该方法具有良好的DA灵敏度,具有较好的临床应用前景。
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引用次数: 2
Electrostatic modification of expanded graphite cathode for high-performance aluminum-ion batteries 高性能铝离子电池用膨胀石墨阴极的静电改性研究
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-10-15 Epub Date: 2023-09-01 DOI: 10.1016/j.jelechem.2023.117761
Changsheng An , Xiaobo Ma , Jiajie Wu , Jianmei Li , Jinfeng Li , Shiying Zhang , Shumin Zhang , Chao Cai

Graphite and its derivatives, as cathode materials for aluminum-ion batteries (AIBs), have excellent cyclic properties, so they have garnered significant research interest over the years. Preliminary research has demonstrated that expanded graphite (EG) exhibits a dual aluminum storage mechanism, i.e., intercalation (1.5–2.5 V) and adsorption (0.5–2.5 V). In this study, for the adsorption mechanism, we propose positively charged EG as a cathode material for AIBs. Using electrostatic modification methods, we found that positive charge on the surface of EG can depress the surface barrier and lead to the adsorption of more anions through electrostatic forces during chemical reactions. Moreover, the improvement of adsorption capacity could play a synergistic coupling role to improve the intercalation kinetics of anions, in which has a high reversible capacity and excellent rate cycling property. Thus, positively charged EG with a large layer space (0.41 nm) demonstrates a high reversible capacity of 118.3 mAh/g at a current density of 1 A/g, along with a conspicuous rate performance of 74.8 mAh/g at 15 A/g. Additionally, as-prepared EG hybrids indicate superb cyclic stability with a retained capacity of 101.8 mAh/g over 10,000 cycles at 5 A/g. The electrostatic modification strategy and expansion of the layer space could facilitate the development of high property graphite cathode materials for AIBs.

石墨及其衍生物作为铝离子电池的正极材料,具有优良的循环性能,近年来引起了广泛的研究兴趣。初步研究表明,膨胀石墨(EG)具有插层(1.5-2.5 V)和吸附(0.5-2.5 V)的双重储铝机制。在本研究中,我们提出了带正电荷的膨胀石墨作为AIBs的正极材料。利用静电改性方法,我们发现EG表面的正电荷可以在化学反应过程中通过静电力抑制表面势垒,从而吸附更多的阴离子。此外,提高吸附容量可以发挥协同耦合作用,提高阴离子的插层动力学,具有较高的可逆容量和优良的速率循环性能。因此,具有大层空间(0.41 nm)的正电荷EG在电流密度为1 a /g时具有118.3 mAh/g的高可逆容量,同时在15 a /g时具有74.8 mAh/g的显着速率性能。此外,制备的EG混合材料表现出极好的循环稳定性,在5 a /g下,在10,000次循环中保持101.8 mAh/g的容量。静电改性策略和层空间的扩大有利于高性能石墨阴极材料的发展。
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引用次数: 0
Facile synthesis of Fe3O4 ultrathin layer coated Fe2O3 composite anode for enhanced lithium-ion storage 制备Fe3O4超薄层包覆Fe2O3复合阳极增强锂离子存储性能
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-10-15 Epub Date: 2023-08-30 DOI: 10.1016/j.jelechem.2023.117758
Xiaoxin Lv , Yan Zhang , Lin Wen , Aomen Yang , Jun Liang

Fe2O3 has been considered as a promising anode material for lithium-ion batteries (LIBs) owing to its high specific capacity. However, its sluggish charge transfer resulting from the poor electrical conductivity severely limits the electrochemical performance. In this work, an ultrathin Fe3O4 layer-coated Fe2O3 composite was fabricated through a facile one-step hydrothermal method with hydrazine hydrate as the reductant in an alkaline environment. Upon use as the anode for LIBS, the as-resulted Fe2O3@Fe3O4 composite achieves a high specific capacity of 1539.5 mA h g−1 at a current density of 100 mA g−1 and simultaneously maintains a high discharge capacity of 707.8 mAh g−1 after 800 cycles at 1000 mA g−1, outperforming the commercial Fe2O3 sample. Electrochemical characterizations reveal that the improved electrochemical performance can be attributed to the combined effects of higher theoretical specific capacity of Fe2O3 and superior electrical conductivity of Fe3O4.

Fe2O3具有较高的比容量,被认为是一种很有前途的锂离子电池负极材料。但其导电性差导致的电荷转移缓慢严重限制了其电化学性能。在碱性环境下,以水合肼为还原剂,采用简单的一步水热法制备了超薄Fe3O4层包覆Fe2O3复合材料。作为LIBS的阳极,Fe2O3@Fe3O4复合材料在100 mA g - 1的电流密度下获得了1539.5 mAh g - 1的高比容量,同时在1000 mA g - 1下800次循环后保持了707.8 mAh g - 1的高放电容量,优于商业Fe2O3样品。电化学表征表明,Fe2O3较高的理论比容量和Fe3O4优越的导电性是其电化学性能提高的共同作用。
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引用次数: 0
Construction of Ce-MOF@COF hybrid nanostructure with controllable thickness for the electrochemical sensitive detection of metol 用于金属电化学敏感检测的Ce-MOF@COF厚度可控杂化纳米结构的构建
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-10-15 Epub Date: 2023-08-31 DOI: 10.1016/j.jelechem.2023.117756
Xiaoxian Hu , Jing Qian , Juan Yang , Xiaomin Hu , Yanjiao Zou , Nianjun Yang

Covalent organic frameworks (COFs), a newly emerging kind of porous material, have gained extensive attention due to their fascinating structural features. However, the superiority of COFs as electrochemical sensing materials has not yet been adequately explored. Herein, a new type of core–shell metal–organic framework (MOF)@COF composites are synthesized through in situ growth of TAPB-DMTP-COF on the pre-synthesized Ce-BDC core. The thickness of the COF shell can be controlled to 20–50 nm by adjusting the Ce-MOF mass. It is found that the obtained MOF@COF composite possesses a larger electrochemical active area and faster electron transfer kinetic than its single component. As a case application of this composite, it has been employed as a sensing material for voltammetric detection of metol, where a linear range from 0.1 − 200 μM and a detection limit of 30 nM have been obtained. This study provides a new strategy to synthesize COF-based electrode materials as well as to explore their electrochemical properties and applications.

共价有机骨架(COFs)是一种新兴的多孔材料,因其独特的结构特点而受到广泛关注。然而,COFs作为电化学传感材料的优越性尚未得到充分的探讨。本文通过在预合成的Ce-BDC核上原位生长TAPB-DMTP-COF,合成了一种新型的核-壳金属-有机骨架(MOF)@COF复合材料。通过调整Ce-MOF的质量,可以将COF的壳层厚度控制在20 ~ 50 nm之间。所得MOF@COF复合材料具有较大的电化学活性面积和较快的电子转移动力学。作为该复合材料的一个案例应用,该材料已被用作金属伏安检测的传感材料,其线性范围为0.1 ~ 200 μM,检测限为30 nM。本研究为合成cof基电极材料提供了新的思路,并对其电化学性能和应用进行了探索。
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引用次数: 0
Symmetrical dicyano-based imidazole molecule-assisted crystallization and defects passivation for high-performance perovskite solar cells 高性能钙钛矿太阳能电池的对称二氰基咪唑分子辅助结晶和缺陷钝化
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-10-13 DOI: 10.1016/j.jelechem.2023.117857
Xumeng Hu , Shaolin Chen , Shiqi Huang , Minghuang Guo , Jingwei Zhu , Ping Hu , Yafeng Li , Mingdeng Wei

Benefiting from the simple and low-cost fabrication of the one-step anti-solvent spin-coating process, the perovskite solar cells (PSCs) have a boost development. However, a great number of defects are generated during solution-fabrication process, retarding the development of PSCs seriously. In this study, the utilization of 4,5-dicyanoimidazole (DCI) as an additive for perovskite precursor solution was investigated. The presence of the double –CN groups in DCI facilitated the formation of Lewis acid-base coordination with unsaturated Pb2+ ions, as well as interaction with I- anions by the –NH- moiety, resulting in the enhanced perovskite film crystallinity, the reduced grain boundaries, and a significant reduction in the defects density of the perovskite film. The decreased trap-assisted recombination and voltage open circuit (VOC) losses in the PSC resulted in the improved photovoltaic performance of device treated by DCI molecule, the PCE increased from 19.59 % to 21.87 % significantly. Moreover, the unencapsulated device with DCI additive exhibited a remarkable 87.8 % retention of its initial PCE after exposure under 10–20 % relative humidity for 60 days, demonstrating an excellent stability than control device.

得益于一步反溶剂旋涂工艺的简单和低成本制造,钙钛矿太阳能电池(PSC)得到了发展。然而,在溶液制备过程中会产生大量的缺陷,严重阻碍了PSCs的发展。在本研究中,研究了4,5-二氰基咪唑(DCI)作为钙钛矿前体溶液的添加剂的应用。DCI中双-CN基团的存在促进了与不饱和Pb2+离子形成Lewis酸碱配位,以及通过-NH-部分与I-阴离子的相互作用,从而增强了钙钛矿膜的结晶度,减少了晶界,并显著降低了钙钛矿膜中的缺陷密度。PSC中陷阱辅助复合和电压开路(VOC)损失的降低导致DCI分子处理的器件的光伏性能提高,PCE从19.59%显著提高到21.87%。此外,含有DCI添加剂的未封装装置在10–20%相对湿度下暴露60天后,其初始PCE的保留率为87.8%,表现出比对照装置优异的稳定性。
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引用次数: 0
4,4′-Biphenyldicarboxylic acid as an anode for sodium-ion batteries: Different electrochemical behaviors in ester and ether-based electrolytes 4,4′-联苯二羧酸作为钠离子电池阳极:在酯基和醚基电解质中的不同电化学行为
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-10-11 DOI: 10.1016/j.jelechem.2023.117852
Siyao Li , Huijia Wu , Chunjie Wu , Meng Jin , Huan Yi , Shi-Yu Lu , Yan Zhang

Organic electrode materials have been regarded as sustainable alternatives for sodium-ion batteries (SIBs) due to their high theoretical specific capacity, large reserves and wide sources from biomass. However, the variety of presently reported organic electrode materials is very limited and their essential electrochemical sodium storage behaviors also deserve further investigating. In this paper, we explore the electrochemical sodium storage behavior of a conjugated aromatic acid (4,4′-biphenyldicarboxylic acid, H2bpdc) in esters and ethers-based electrolytes. The results illustrate that in esters-based electrolytes, H2bpdc just shows limited capacity and poor electrochemical sodium storage kinetics. By contrast, in ethers-based electrolytes, H2bpdc experiences a process similar to conversion type mechanism from pristine acid to sodium salt, displaying fast kinetics and delivers a high reversible capacity of 280 mA h g−1. This research would provide basic and novel insights to the electrochemical sodium storage behaviors of promising organic electrode materials and accelerate the new materials exploration process for SIBs.

有机电极材料由于其高理论比容量、大储量和广泛的生物质来源,被认为是钠离子电池的可持续替代品。然而,目前报道的有机电极材料的种类非常有限,其基本的电化学钠存储行为也值得进一步研究。在本文中,我们探索了共轭芳香酸(4,4′-联苯二羧酸,H2bpdc)在基于酯和醚的电解质中的电化学钠存储行为。结果表明,在酯类电解质中,H2bpdc的容量有限,电化学储钠动力学较差。相比之下,在基于醚的电解质中,H2bpdc经历了类似于从原始酸到钠盐的转化型机制的过程,表现出快速的动力学,并提供280 mA h g−1的高可逆容量。这项研究将为有前景的有机电极材料的电化学钠存储行为提供基础和新的见解,并加速SIBs的新材料探索过程。
{"title":"4,4′-Biphenyldicarboxylic acid as an anode for sodium-ion batteries: Different electrochemical behaviors in ester and ether-based electrolytes","authors":"Siyao Li ,&nbsp;Huijia Wu ,&nbsp;Chunjie Wu ,&nbsp;Meng Jin ,&nbsp;Huan Yi ,&nbsp;Shi-Yu Lu ,&nbsp;Yan Zhang","doi":"10.1016/j.jelechem.2023.117852","DOIUrl":"https://doi.org/10.1016/j.jelechem.2023.117852","url":null,"abstract":"<div><p>Organic electrode materials have been regarded as sustainable alternatives for sodium-ion batteries (SIBs) due to their high theoretical specific capacity, large reserves and wide sources from biomass. However, the variety of presently reported organic electrode materials is very limited and their essential electrochemical sodium storage behaviors also deserve further investigating. In this paper, we explore the electrochemical sodium storage behavior of a conjugated aromatic acid (4,4′-biphenyldicarboxylic acid, H<sub>2</sub>bpdc) in esters and ethers-based electrolytes. The results illustrate that in esters-based electrolytes, H<sub>2</sub>bpdc just shows limited capacity and poor electrochemical sodium storage kinetics. By contrast, in ethers-based electrolytes, H<sub>2</sub>bpdc experiences a process similar to conversion type mechanism from pristine acid to sodium salt, displaying fast kinetics and delivers a high reversible capacity of 280 mA h g<sup>−1</sup>. This research would provide basic and novel insights to the electrochemical sodium storage behaviors of promising organic electrode materials and accelerate the new materials exploration process for SIBs.</p></div>","PeriodicalId":50545,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"950 ","pages":"Article 117852"},"PeriodicalIF":4.5,"publicationDate":"2023-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41227869","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Effect of plasma treatment on electrochemical performance of lignin-based carbon fibers 等离子体处理对木质素基碳纤维电化学性能的影响
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-10-01 Epub Date: 2023-08-19 DOI: 10.1016/j.jelechem.2023.117723
R.K. Azega , Mazharul Haque , Qi Li , Omid Hosseinaei , Hans Theliander , Peter Enoksson , Per Lundgren

The abundant and renewable nature of lignin obtained from wood renders it as a sustainable carbon resource for energy storage applications. However, their environmentally unfavorable processing conditions and limited energy storage performance prohibit the use of lignin-based carbon materials' use as supercapacitor electrodes. The material's properties require advancement to overcome the limitation of low specific capacitances. In this study, we report on the impact on the electrochemical performance of inherently hydrophobic lignin-based carbon fibers (LCF) by subjecting them to a mild plasma treatment. The electrode’s capacitance was thus increased by 20%, with better rate capability and energy-power performance (11 Wh/kg and 0.8 kW/kg) in the KOH electrolyte. The quantified improvements were attributed to the capacitive functional groups, and enhanced surface wettability, which increased ion accessibility to active surface area improving charge-transfer ability to the surface with more additional functional groups. Remarkably, the selected plasma conditions introduced mostly desirable functional groups that limited any parasitic faradaic reactions prone to affect the device's long-term cycling stability and self-discharge characteristics. Furthermore, the impact of different inherent and introduced oxygen surface functional groups, including COO, COH, CO, and CO, on the capacitive performance of these fibers at different device conditions (such as cycling and electrochemical activation) was investigated in different aqueous electrolytes. To ensure environmental favorability, the electrospinning of lignin fibers was conducted using a high molecular fraction of lignin without the inclusion of any fossil-based co-spinning polymers.

从木材中获得的丰富和可再生的木质素使其成为能源储存应用的可持续碳资源。然而,其环境不利的加工条件和有限的储能性能限制了木质素基碳材料作为超级电容器电极的使用。该材料的性能需要改进,以克服低比容的限制。在这项研究中,我们报告了对木质素基碳纤维(LCF)进行轻度等离子体处理对其电化学性能的影响。电极的电容增加了20%,在KOH电解质中具有更好的倍率能力和能量功率性能(11 Wh/kg和0.8 kW/kg)。量化的改进归因于电容官能团和增强的表面润湿性,这增加了离子对活性表面积的可及性,提高了具有更多附加官能团的表面的电荷转移能力。值得注意的是,所选择的等离子体条件引入了大多数理想的官能团,限制了任何容易影响器件长期循环稳定性和自放电特性的寄生法拉第反应。此外,研究了不同的固有氧和引入氧表面官能团,包括COO−、COH、CO和CO,在不同的设备条件下(如循环和电化学活化),在不同的水溶液中对这些纤维电容性能的影响。为了确保对环境有利,木质素纤维的静电纺丝是使用木质素的高分子部分而不包含任何化石基共纺丝聚合物进行的。
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引用次数: 0
A label-free photoelectrochemical sensor based on BiVO4@graphene oxide hybrid for analysis of the antioxidant capacity in food 一种基于BiVO4@graphene氧化物杂化物的无标签光电化学传感器,用于分析食品中的抗氧化能力
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-10-01 Epub Date: 2023-08-12 DOI: 10.1016/j.jelechem.2023.117713
Fangjie Han , Shulin Luo , Zhifang Wu , Zhishan Liang , Wenxin Yang , Dongxue Han , Zhonghui Sun , Zhenbang Liu , Li Niu

Antioxidant can protect body from free radical and dietary intake is a major source of antioxidants for human body. Therefore, it is particularly important to evaluate the antioxidant capacity of food and drink in daily diet. Herein, a label-free photoelectrochemical (PEC) sensor based on BiVO4@graphene oxide (GO) hybrid has been developed for antioxidants analysis and applied it to antioxidant capacity detection of real samples. Five representative antioxidants including ascorbic acid (AA), caffeic acid (CA), chlorogenic acid (CHA), fisetin (FT) and quercetin (QT) were determined by this PEC sensor to acquire photocurrent response at different concentrations. This PEC sensor exhibited excellent sensitivity and anti-interference. Furthermore, antioxidant capacity of food samples was assessed utilizing this PEC sensor, indicating the practicability and accuracy of this PEC sensor. This study suggests that BiVO4@GO composites constructed PEC sensor can provide a practical and fast method for detecting antioxidant capacity in the field of food.

抗氧化剂可以保护人体免受自由基的侵害,饮食摄入是人体抗氧化剂的主要来源。因此,在日常饮食中评估食品和饮料的抗氧化能力就显得尤为重要。本文研制了一种基于BiVO4@graphene氧化物(GO)杂化物的无标记光电化学(PEC)传感器,用于抗氧化剂分析,并将其应用于实际样品的抗氧化能力检测。用该传感器测定了抗坏血酸(AA)、咖啡酸(CA)、绿原酸(CHA)、非西汀(FT)和槲皮素(QT)等5种具有代表性的抗氧化剂在不同浓度下的光电流响应。该传感器具有良好的灵敏度和抗干扰性。利用该传感器对食品样品的抗氧化能力进行了评价,验证了该传感器的实用性和准确性。该研究表明BiVO4@GO复合材料构建的PEC传感器可为食品领域抗氧化能力的检测提供一种实用、快速的方法。
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引用次数: 0
CuO quantum dots embedded Cu3(BTC)2/CuO sugar gourd-like nanoarrays on copper foil as free-standing anodes for lithium-ion batteries with boosted performance 在铜箔上嵌入Cu3(BTC)2/CuO糖葫芦状纳米阵列的CuO量子点作为锂离子电池的独立阳极,提高了性能
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-10-01 Epub Date: 2023-08-12 DOI: 10.1016/j.jelechem.2023.117714
Qinxing Xie , Shoumin Zhang , Weiping Huang , Peng Zhao

CuO quantum dots (QDs)-embedded Cu3(BTC)2/CuO sugar gourd-like nanoarrays are successfully assembled on copper foil through a two-step wet-chemical growth method. As a free-standing anode for lithium-ion batteries, the resultant composite (Cu-BTC/QDs/CuO@Cu) delivers a high specific capacity of 813 mAh/g at a current density of 0.2 A/g after 150 cycles, and 452 mAh/g at 1.0 A/g after 500 cycles, demonstrating excellent cycling stability and rate performance. The superior energy storage capability is attributed to a synergistic effect from the individual components including the electro-active organic ligand, porous framework and CuO nanowires/QDs. As an efficient binder-free anode, Cu-BTC/QDs/CuO@Cu can be a promising candidate for the development of high-performance and cost-effective LIBs with exceptional energy density and power density capabilities.

采用两步湿化学生长方法在铜箔上成功组装了CuO量子点(QDs)嵌入Cu3(BTC)2/CuO糖葫芦纳米阵列。作为锂离子电池的独立阳极,该复合材料(Cu-BTC/QDs/CuO@Cu)在150次循环后电流密度为0.2 a /g时可提供813 mAh/g的高比容量,在500次循环后电流密度为1.0 a /g时可提供452 mAh/g的高比容量,具有优异的循环稳定性和倍率性能。优异的储能能力归因于各个组成部分的协同效应,包括电活性有机配体、多孔框架和CuO纳米线/量子点。作为一种高效的无粘结剂阳极,Cu-BTC/QDs/CuO@Cu具有优异的能量密度和功率密度能力,是开发高性能和经济高效的锂离子电池的有希望的候选者。
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引用次数: 1
Promotion of nitrate reduction reaction activity by Co3O4@MoS2 Particle-Support system Co3O4@MoS2颗粒-载体体系对硝酸还原反应活性的促进作用
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-10-01 Epub Date: 2023-08-07 DOI: 10.1016/j.jelechem.2023.117702
Yanli Zhang, Jiuqing Xiong, Shihai Yan, Bingping Liu

Electrochemical reduction of nitrate to NH3 is a very promising alternative reaction to the Haber-Bosch process, and it is necessary to develop the efficient electrocatalysts. In this study, a particle-support mode Co3O4 catalyst was synthesized with ZIF-67 as the precursor, and then dispersed on MoS2 nanoflowers by hydrothermal method. The Co3O4 is anchored to MoS2 by forming Co-S coordination bond. Furthermore, the particle-supported Co3O4 exhibits better performance than Co3O4 alone, as is manifested by higher Faradaic efficiencies and NH3 yield rate at − 0.64 V (52.69% vs 32.03%; 4539.61 μg h−1 mg−1cat vs 2048.63 μg h−1 mg−1cat), lower energy barriers (0.96 eV vs 1.19 eV), and better electronic conductivity (Bandwidth: 0.581 eV vs 0.613 eV). In addition, this research provides an effective solution to solve the aggregation problem of metal oxide nanoparticles.

电化学还原硝态氮为NH3是一种很有前途的替代Haber-Bosch法的反应,有必要开发高效的电催化剂。本研究以ZIF-67为前驱体合成了一种颗粒支撑型Co3O4催化剂,并通过水热法将其分散在MoS2纳米花上。Co3O4通过形成Co-S配位键锚定在MoS2上。此外,颗粒负载的Co3O4比单独的Co3O4表现出更好的性能,表现在- 0.64 V时更高的法拉第效率和NH3产率(52.69% vs 32.03%;4539.61 μg h−1 mg−1cat vs 2048.63 μg h−1 mg−1cat),更低的能垒(0.96 eV vs 1.19 eV)和更好的电子导电性(带宽:0.581 eV vs 0.613 eV)。此外,本研究为解决金属氧化物纳米颗粒的聚集问题提供了有效的解决方案。
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引用次数: 0
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Journal of Electroanalytical Chemistry
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