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Properties of hollow yolk-shell NiS2/FeS2@NC@NiFe LDH/FeO(OH) nanoflower microspheres as anode materials for lithium-ion batteries 中空蛋黄壳NiS2/FeS2@NC@NiFe LDH/FeO(OH)纳米花微球作为锂离子电池负极材料的性能
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-08-15 DOI: 10.1016/j.jelechem.2023.117606
Ying Liu, Xue Zhou, Ping Chen, Xinrong Cao, Dongxuan Liu, Ruiqi Wang

As an anode material of lithium-ion batteries, transition metal sulfides have high theoretical capacity, and the structure design is an effective strategy to gain better electrochemical performance. Layered double hydroxides (LDHs) have significant preponderances in the field of energy storage on account of their exchangeable anions and biggish specific surface area. Nevertheless, its defects such as poor conductivity, easy agglomeration of nanosheets and biggish volume change during the cycle result in poor cycling durability and rate performance, which gravely constrain its further application. In this study, hollow yolk-shell NiS2/FeS2@NC@NiFe LDH/FeO(OH) nanoflower microspheres are prepared successfully by solvothermal and hydrothermal methods. Firstly, introducing N-doped carbon layer can availably heighten the electro-conductivity of the materials and stop the metallic particles from falling off to boost the structural stability. The design of hollow yolk-shell and nanoflower structure can effectively inhibit cubical expansion. In addition, the unique layered structure of the nanosheets can provide more active sites, shorten the ion transport path, and enhance the lithium storage performance. As a result, the NiS2/FeS2@NC@NiFe LDH/FeO(OH) electrode has splendid cycling performance (709.9 mAh g−1 at 0.2 A g−1 after 200 cycles). These prominent electrochemical properties demonstrate convincingly that the NiS2/FeS2@NC@NiFe LDH/FeO(OH) is a viable anode material.

过渡金属硫化物作为锂离子电池的负极材料,具有较高的理论容量,其结构设计是获得更好电化学性能的有效策略。层状双氢氧化物(LDHs)由于其阴离子的可交换性和较大的比表面积在储能领域具有显著优势。但其导电性差、纳米片易团聚、循环过程中体积变化大等缺陷导致其循环耐久性和倍率性能较差,严重制约了其进一步应用。本研究通过溶剂热法和水热法成功制备了中空的蛋黄壳NiS2/FeS2@NC@NiFe LDH/FeO(OH)纳米花微球。首先,引入n掺杂碳层可以有效地提高材料的导电性,防止金属颗粒脱落,从而提高结构的稳定性。中空蛋黄壳和纳米花结构的设计可以有效地抑制立方膨胀。此外,纳米片独特的层状结构可以提供更多的活性位点,缩短离子传输路径,提高锂的存储性能。结果表明,NiS2/FeS2@NC@NiFe LDH/FeO(OH)电极具有优异的循环性能,在0.2 a g−1下循环200次后可达到709.9 mAh g−1。这些优异的电化学性能有力地证明了NiS2/FeS2@NC@NiFe LDH/FeO(OH)是一种可行的阳极材料。
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引用次数: 0
Electrochemical degradation of the antibiotic ceftazidime by La doped modified PbO2 electrode: Catalytic conditions and degradation pathway La掺杂修饰PbO2电极电化学降解抗生素头孢他啶:催化条件和降解途径
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-08-15 DOI: 10.1016/j.jelechem.2023.117620
Ziming Chen , Yafei Du , Guangming Yang , Jian Wang , Yulong Ma , Yonggang Sun , Yongsheng Ren , Xiaoxiao Duan

The use of antibiotics continues to increase, and its unreasonable use and discharge have caused great harm. Electrochemical oxidation is an effective method to solve this problem. In this work, which was prepared by electrodeposition of Ti/PbO2 and Ti/PbO2-La electrodes, using the above electrode explores the ceftazidime electrochemical degradation. The results indicated that the electrode doped with La had more active sites and better electrochemical performance. Through 2 h of degradation, the removal rate of ceftazidime attained 96.12 %. Meanwhile, the influence of current density, electrode spacing, electrolyte concentration, and initial concentration of ceftazidime on the degradation efficiency were systematically evaluated. Based on the identification of intermediate products, the degradation pathway was proposed, and ceftazidime was finally degraded to some small molecules. A new method was developed to remove the ceftazidime.

抗生素的使用不断增加,其不合理的使用和排放造成了很大的危害。电化学氧化是解决这一问题的有效方法。本文通过电沉积制备Ti/PbO2和Ti/PbO2- la电极,探讨了利用上述电极对头孢他啶的电化学降解。结果表明,掺杂镧的电极具有更多的活性位点和更好的电化学性能。经过2 h的降解,头孢他啶的去除率达到96.12%。同时系统评价了电流密度、电极间距、电解质浓度和头孢他啶初始浓度对降解效率的影响。在中间产物鉴定的基础上,提出了头孢他啶的降解途径,最终将其降解为一些小分子。提出了一种去除头孢他啶的新方法。
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引用次数: 0
A redox accessible Cu-BTC metal organic framework-based nanocomposite for selective and sensitive electrochemical sensing of Triclosan in real sample 一种氧化还原可及的Cu-BTC金属有机骨架纳米复合材料,用于三氯生在实际样品中的选择性和敏感电化学传感
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-08-15 DOI: 10.1016/j.jelechem.2023.117589
Shital Jyotsna Sahoo , Bapun Barik , Banalata Maji , Pratap S. Nayak , Narmada Behera , Priyabrat Dash

Extended use of Triclosan (TCS), in many pharmaceutical, medical devices, personal care products and home cleaning products constitutes a potential concern to the human health and ecological system due to its vast exposure into ground water, sediments and surface water. Its prolonged environmental presence and recognized persistence have sparked scientific and societal concern, which has promoted research into efficient remediation methods. In order to resolve this concern, we have designed a ternary nanocomposite of rGO modified porous Cu-benzene tricarboxylic acid metal organic framework (Cu-BTC MOF) decorated NiCo bimetallic nanoparticle by adopting a solvothermal route. High electrical conductivity of rGO, greater surface area of Cu-BTC MOF, and the electrocatalytic nature of NiCo bimetallic nanoparticles collectively enhance the electrochemical property of the designed sensor. Cyclic voltammetry and impedance measurement showcased our fabricated nanocomposite possessed highest conductivity and supported our aim to achieve a potential sensor for electrochemical sensing of TCS. Under optimum conditions, from the square wave voltammetry (SWV) analysis our sensor was found to have detection limit 0.23 × 10−12 M (0.67 × 10−7µg/ml) and a wide linear detection range of 49 × 10−6 M to 0.39 × 10−12 M with sensitivity of 0.196 µA/mM. The proposed sensor further displayed desired selectivity, outstanding stability, and good repeatability, demonstrating its successful detection capabilities for harmful TCS.

由于大量暴露在地下水、沉积物和地表水中,三氯生(TCS)在许多制药、医疗器械、个人护理产品和家庭清洁产品中的广泛使用,对人类健康和生态系统构成了潜在的威胁。它在环境中的长期存在和公认的持久性引起了科学和社会的关注,这促进了对有效补救方法的研究。为了解决这一问题,我们采用溶剂热途径设计了还原氧化石墨烯修饰多孔铜苯三羧酸金属有机骨架(Cu-BTC MOF)修饰镍双金属纳米颗粒的三元纳米复合材料。rGO的高导电性、Cu-BTC MOF的更大表面积以及NiCo双金属纳米颗粒的电催化性质共同提高了所设计传感器的电化学性能。循环伏安法和阻抗测试表明,我们制备的纳米复合材料具有最高的电导率,支持了我们实现TCS电化学传感的潜在传感器的目标。在最佳条件下,通过方波伏安法(SWV)分析,我们的传感器检测限为0.23 × 10−12 M (0.67 × 10−7µg/ml),线性检测范围为49 × 10−6 M至0.39 × 10−12 M,灵敏度为0.196µa /mM。该传感器进一步显示出理想的选择性、出色的稳定性和良好的可重复性,证明了其对有害TCS的成功检测能力。
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引用次数: 2
Simultaneous electrochemical detection of Cd (II) and Pb (II) based on L-cysteine functionalized gold nanoparticles/metal-organic frameworks-graphene oxide nanocomposites 基于l-半胱氨酸功能化金纳米粒子/金属-有机骨架-氧化石墨烯纳米复合材料的Cd (II)和Pb (II)的同步电化学检测
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-08-15 DOI: 10.1016/j.jelechem.2023.117573
Birui Wang , Jin Chen , Huapei Tong , Yumeng Huang , Bo Liu , Xiaolan Yang , Zhaohong Su , Xinman Tu , Xiaoli Qin

In this paper, a facile electrochemical sensor for simultaneous detection of Cd2+ and Pb2+ was fabricated, on the base of in situ growing gold nanoparticles (AuNPs) on L-cysteine functionalized metal-organic frameworks (L-MOFs) and graphene oxide (GO) nanocomposites (L-Au-MOFs-GO). First, L-MOFs were in-situ synthesized on the GO nanosheets by a one-step hydrothermal method. Then, the L-cysteine in L-MOFs-GO nanocomposite was used as a reductant to react with HAuCl4 and in-situ obtain AuNPs, finally forming the L-Au-MOFs-GO composite. This L-Au-MOFs-GO composite not only can enhance the conductivity of the composite by accelerating the electron transfer, but also can act as an enrichment medium phase of heavy metal ions because of the interaction between metal cations and hydrophilic groups of L-MOFs or GO. The morphology of L-Au-MOFs-GO composites were characterized by transmission electron microscope (TEM), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectrometer (FT-IR), and X-ray diffraction (XRD). The results showed that the electrochemical performance of L-Au-MOFs-GO composite was better than GO material or MOFs-GO composite. Under the optimal conditions, the L-Au-MOFs-GO modified electrode was successfully applied to individually and simultaneously detect the Cd2+ and Pb2+ in an acetic acid buffer solution with good selectivity and high sensitivity. This method was utilized for simultaneous detection of Cd2+ and Pb2+ in river water and the leaching solution of watermelon with great reliability and accuracy. This new nanomaterial for simultaneous detection of Cd2+ and Pb2+ has the potential application in complicated samples.

在l-半胱氨酸功能化金属-有机骨架(L-MOFs)和氧化石墨烯(GO)纳米复合材料(L-Au-MOFs-GO)上原位生长金纳米粒子(AuNPs),制备了一种同时检测Cd2+和Pb2+的简易电化学传感器。首先,采用一步水热法在氧化石墨烯纳米片上原位合成L-MOFs。然后,L-MOFs-GO纳米复合材料中的l -半胱氨酸作为还原剂与HAuCl4反应,原位得到AuNPs,最终形成L-Au-MOFs-GO复合材料。这种L-Au-MOFs-GO复合材料不仅可以通过加速电子转移来增强复合材料的导电性,而且由于金属阳离子与l - au - mofs或GO的亲水性基团之间的相互作用,可以作为重金属离子的富集介质相。采用透射电镜(TEM)、扫描电镜(SEM)、x射线光电子能谱(XPS)、傅里叶变换红外光谱仪(FT-IR)和x射线衍射仪(XRD)对L-Au-MOFs-GO复合材料的形貌进行了表征。结果表明,L-Au-MOFs-GO复合材料的电化学性能优于GO材料或MOFs-GO复合材料。在最佳条件下,L-Au-MOFs-GO修饰电极成功地分别和同时检测了醋酸缓冲溶液中的Cd2+和Pb2+,具有良好的选择性和高灵敏度。该方法可用于河水和西瓜浸出液中Cd2+和Pb2+的同时检测,具有较高的可靠性和准确性。这种同时检测Cd2+和Pb2+的新型纳米材料在复杂样品中具有潜在的应用前景。
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引用次数: 2
The semiconductor properties and tin segregation mechanism in the passive film formed on the electrodeposited Ni-Sn coatings 研究了Ni-Sn镀层钝化膜的半导体特性和锡偏析机理
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-08-15 DOI: 10.1016/j.jelechem.2023.117588
Donatien Ngendabanyikwa , Zhengyi Xu , Guozhe Meng , Yanqiu Wang , Junyi Wang , Yawei Shao

The nanocrystalline Ni-Sn coatings (average grain size 15.78 nm) formed of relatively ordered circular particles covering the entire surface characterized with nodule-like endings were successfully electrodeposited using pulse electrodeposition technique. Scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy (SEM-EDS) and X-ray diffraction (XRD) were used to analyse the film microstructure. The corrosion resistance and semiconducting properties of Ni-Sn coatings were investigated in borate buffer solution. The EIS measurements showed that Ni-Sn alloys developed, in the passive zone, a good corrosion resistance as demonstrated by a thin film thickness, the low capacitance value, high polarization resistance, and the high value of electric field strength. Mott-Schottky analysis showed that the passive film formed on Ni-Sn coatings presents an p-n heterojunction characteristic indicating that the charge carrier densities are composed of cation (NA) and anion (ND) vacancies. The high density of point defects (NA + ND ∼ 1021cm−3) induces a high electronic conductivity in the Ni-Sn coatings passive film. The XPS analysis showed that the passive film formed on Ni-Sn alloys is composed of NiO, Ni(OH)2, NiOOH, SnO, and SnO2 species and an enrichment of Sn in the passive film. The mechanisms of passive film growth and Sn segregation in the Ni-Sn passive film are suggested in conjunction with the Point Defect Model (PDM). The good corrosion resistance and high electronic conductivity achieved in this work suggest that Ni-Sn Coating is a good candidate for water electrolysis applications.

采用脉冲电沉积技术,成功地沉积了镍锡纳米晶涂层(平均晶粒尺寸为15.78 nm),该涂层由相对有序的圆形颗粒覆盖整个表面,其末端呈结节状。利用扫描电子显微镜、能量色散x射线能谱仪(SEM-EDS)和x射线衍射仪(XRD)对膜的微观结构进行了分析。研究了镍锡镀层在硼酸盐缓冲溶液中的耐蚀性和半导体性能。EIS测试结果表明,Ni-Sn合金在钝化区具有良好的耐蚀性,表现为薄膜厚度薄、电容值低、极化电阻高、电场强度高。Mott-Schottky分析表明,Ni-Sn镀层上形成的钝化膜呈现p-n异质结特征,表明载流子密度由阳离子(NA)和阴离子(ND)空位组成。高密度的点缺陷(NA + ND ~ 1021cm−3)使Ni-Sn镀层具有较高的电子导电性。XPS分析表明,Ni-Sn合金表面形成的钝化膜主要由NiO、Ni(OH)2、NiOOH、SnO和SnO2组成,且钝化膜中Sn元素富集。结合点缺陷模型(PDM)提出了Ni-Sn钝化膜生长和锡偏析的机理。镍锡镀层具有良好的耐腐蚀性和高的电子导电性,是一种很好的水电解材料。
{"title":"The semiconductor properties and tin segregation mechanism in the passive film formed on the electrodeposited Ni-Sn coatings","authors":"Donatien Ngendabanyikwa ,&nbsp;Zhengyi Xu ,&nbsp;Guozhe Meng ,&nbsp;Yanqiu Wang ,&nbsp;Junyi Wang ,&nbsp;Yawei Shao","doi":"10.1016/j.jelechem.2023.117588","DOIUrl":"https://doi.org/10.1016/j.jelechem.2023.117588","url":null,"abstract":"<div><p>The nanocrystalline Ni-Sn coatings (average grain size 15.78 nm) formed of relatively ordered circular particles covering the entire surface characterized with nodule-like endings were successfully electrodeposited using pulse electrodeposition technique. Scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy (SEM-EDS) and X-ray diffraction (XRD) were used to analyse the film microstructure. The corrosion resistance and semiconducting properties of Ni-Sn coatings were investigated in borate buffer solution. The EIS measurements showed that Ni-Sn alloys developed, in the passive zone, a good corrosion resistance as demonstrated by a thin film thickness, the low capacitance value, high polarization resistance, and the high value of electric field strength. Mott-Schottky analysis showed that the passive film formed on Ni-Sn coatings presents an p-n heterojunction characteristic indicating that the charge carrier densities are composed of cation (<em>N</em><sub>A</sub>) and anion (<em>N</em><sub>D</sub>) vacancies. The high density of point defects (<em>N</em><sub>A</sub> + <em>N</em><sub>D</sub> ∼ 10<sup>21</sup>cm<sup>−3</sup>) induces a high electronic conductivity in the Ni-Sn coatings passive film. The XPS analysis showed that the passive film formed on Ni-Sn alloys is composed of NiO, Ni(OH)<sub>2</sub>, NiOOH, SnO, and SnO<sub>2</sub> species and an enrichment of Sn in the passive film. The mechanisms of passive film growth and Sn segregation in the Ni-Sn passive film are suggested in conjunction with the Point Defect Model (PDM). The good corrosion resistance and high electronic conductivity achieved in this work suggest that Ni-Sn Coating is a good candidate for water electrolysis applications.</p></div>","PeriodicalId":50545,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"943 ","pages":"Article 117588"},"PeriodicalIF":4.5,"publicationDate":"2023-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1806860","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
Synergetic effect of TiO2 coating and oxygen vacancy boosting LiMn2O4 cathode for stable aqueous zinc-ion batteries TiO2涂层与氧空位增强阴极LiMn2O4对稳定水锌离子电池的协同效应
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-08-15 DOI: 10.1016/j.jelechem.2023.117597
Yunhao Wu, Meng Shi, Dan Luo, Zhaolong Zhang, Zhi Li, Zhiming Cheng, Xiaohong Kang

LiMn2O4 cathode materials have been regarded as one of the promising candidates for aqueous zinc-ion batteries. However, their actual application is still hindered by the Mn2+ dissolution and structural transformation during the charge/discharge cycling. Herein, we synthesized LiMn2O4 cathode materials with octahedron morphologies and followed introducing oxygen vacancies by the calcination treatment in Ar. Octahedral shape is beneficial to the improvement of cycle stability of LiMn2O4 cathode materials. Oxygen vacancies contribute to the rate performance by improving the electronic conductivity. Nevertheless, the cycling stability of LiMn2O4 cathode materials with oxygen vacancies is not satisfactory. So, we proposed the synergistic strategy of TiO2-coating LiMn2O4 and oxygen vacancies. TiO2@(LMO-A0.5) sample with uniform thin TiO2 coating was obtained by regulating the hydrolysis reaction of tetrabutyl titanate. Consequently, TiO2@(LMO-A0.5) exhibits the impressive rate capability and cycling stability (as high as 85 mAh/g and 91.22% capacity retentions after 200 cycles at 0.1 A g−1) as the cathode materials for aqueous zinc-ion batteries. The synergetic development of multiple strategies may endow LiMn2O4 cathode materials with magical perspectives in aqueous zinc-ion batteries.

LiMn2O4正极材料被认为是有前途的水性锌离子电池的候选材料之一。然而,在充放电循环过程中,Mn2+的溶解和结构转变仍然阻碍了它们的实际应用。在此,我们合成了具有八面体结构的LiMn2O4正极材料,然后在Ar中通过煅烧处理引入氧空位。八面体结构有利于提高LiMn2O4正极材料的循环稳定性。氧空位通过提高电子导电性来提高速率性能。然而,含氧空位的LiMn2O4正极材料的循环稳定性并不令人满意。因此,我们提出了tio2涂层LiMn2O4和氧空位的协同策略。通过调节钛酸四丁酯的水解反应,得到了具有均匀薄薄的TiO2涂层的TiO2@(LMO-A0.5)样品。因此,TiO2@(LMO-A0.5)表现出令人印象深刻的倍率性能和循环稳定性(高达85 mAh/g,在0.1 A g−1下循环200次后容量保留率为91.22%)。多种策略的协同发展,将赋予LiMn2O4正极材料在水锌离子电池中的神奇前景。
{"title":"Synergetic effect of TiO2 coating and oxygen vacancy boosting LiMn2O4 cathode for stable aqueous zinc-ion batteries","authors":"Yunhao Wu,&nbsp;Meng Shi,&nbsp;Dan Luo,&nbsp;Zhaolong Zhang,&nbsp;Zhi Li,&nbsp;Zhiming Cheng,&nbsp;Xiaohong Kang","doi":"10.1016/j.jelechem.2023.117597","DOIUrl":"https://doi.org/10.1016/j.jelechem.2023.117597","url":null,"abstract":"<div><p>LiMn<sub>2</sub>O<sub>4</sub> cathode materials have been regarded as one of the promising candidates for aqueous zinc-ion batteries. However, their actual application is still hindered by the Mn<sup>2+</sup> dissolution and structural transformation during the charge/discharge cycling. Herein, we synthesized LiMn<sub>2</sub>O<sub>4</sub><span> cathode materials with octahedron<span> morphologies and followed introducing oxygen vacancies<span> by the calcination treatment in Ar. Octahedral shape is beneficial to the improvement of cycle stability of LiMn</span></span></span><sub>2</sub>O<sub>4</sub> cathode materials. Oxygen vacancies contribute to the rate performance by improving the electronic conductivity. Nevertheless, the cycling stability of LiMn<sub>2</sub>O<sub>4</sub> cathode materials with oxygen vacancies is not satisfactory. So, we proposed the synergistic strategy of TiO<sub>2</sub>-coating LiMn<sub>2</sub>O<sub>4</sub> and oxygen vacancies. TiO<sub>2</sub>@(LMO-A0.5) sample with uniform thin TiO<sub>2</sub> coating was obtained by regulating the hydrolysis reaction of tetrabutyl titanate. Consequently, TiO<sub>2</sub>@(LMO-A0.5) exhibits the impressive rate capability and cycling stability (as high as 85 mAh/g and 91.22% capacity retentions after 200 cycles at 0.1 A g<sup>−1</sup>) as the cathode materials for aqueous zinc-ion batteries. The synergetic development of multiple strategies may endow LiMn<sub>2</sub>O<sub>4</sub> cathode materials with magical perspectives in aqueous zinc-ion batteries.</p></div>","PeriodicalId":50545,"journal":{"name":"Journal of Electroanalytical Chemistry","volume":"943 ","pages":"Article 117597"},"PeriodicalIF":4.5,"publicationDate":"2023-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2620198","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
Electrochemical performance optimization of NMC811 through the structure design of its precursor 通过对NMC811前驱体的结构设计,优化其电化学性能
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-08-15 DOI: 10.1016/j.jelechem.2023.117630
Maria Laura Para, Andrea Querio, Julia Amici, Daniele Versaci, Antonello A. Barresi, Silvia Bodoardo, Daniele Marchisio

This paper presents a study on the effect of the precursor structure on NMC811 electrochemical properties. The influence of different parameters, such as morphology and crystallinity of the precursor, Ni0.8Mn0.1Co0.1(OH)2, on the final electrochemical performance of NMC811 are analyzed. To ensure a correct and fast mixing of the precursor reactants and prepare the Ni0.8Co0.1Mn0.1(OH)2, a novel approach is used employing a micromixer, thus enabling the collection of the precipitated metal hydroxide within a few seconds after its precipitation. Then the precursor is calcinated together with a Li source to obtain the NMC811 cathode material. When analyzing the aging time of the precursor, between collection and calcination, it is observed that the primary particles of the precursor grow and become more crystalline, adopting a lamellar shape, while the secondary particles turn more compact, when increasing the aging time. The NMC materials synthesized from the aged precursors have smoother primary particles, exposing clearer crystalline planes. This change in morphology is also evidenced in the crystalline structure where an increase in the aging time produces better layered materials with a lower cation mixing index. The well-ordered structure impacts the electrochemical characteristics; indeed, the aged precursor produces NMC with higher specific capacity, better cyclability and lower capacity fade.

研究了前驱体结构对NMC811电化学性能的影响。分析了前驱体Ni0.8Mn0.1Co0.1(OH)2的形貌和结晶度等不同参数对NMC811最终电化学性能的影响。为了保证前驱物的正确和快速混合,制备Ni0.8Co0.1Mn0.1(OH)2,采用了一种新颖的方法,在沉淀后的几秒钟内就可以收集沉淀的金属氢氧化物。然后将前驱体与Li源一起煅烧,得到NMC811正极材料。通过对前驱体时效时间的分析,在收集和煅烧过程中,随着时效时间的延长,前驱体的初级颗粒逐渐长大并变得更加结晶,呈片层状,而次级颗粒则变得更加致密。由老化前驱体合成的NMC材料初生颗粒更光滑,晶面更清晰。这种形貌上的变化也体现在晶体结构上,随着时效时间的增加,层状材料的质量越高,阳离子混合指数越低。有序结构影响电化学特性;老化前驱体产生的NMC具有更高的比容量、更好的循环性和更低的容量衰减。
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引用次数: 0
An electrochemical biosensor based on CuFe PBA/MoS2 nanocomposites for stable and sensitive detection of hydrogen peroxide and carcinoembryonic antigen 基于CuFe - PBA/MoS2纳米复合材料的过氧化氢和癌胚抗原稳定灵敏检测电化学生物传感器
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-08-15 DOI: 10.1016/j.jelechem.2023.117592
Yuelin Zhou , Xin Guan , Ru Wu , Yuan Dang , Sha Yu , Yuanzhen Zhou , Jieli Tang

An increasing number of electrochemical biosensors have been constructed to detect single bioactive substances with high sensitivity, but not multiple bioactive substances with different properties. Therefore, we incorporated Cu and Fe elements into Prussian blue to form Prussian blue analogues (PBA) to improve the electrochemical catalytic activity of Prussian blue. At the same time, MoS2 is used as the material substrate to increase the electrochemical active site of the composite. We have constructed a universal electrochemical sensing platform using composite materials (CuFe PBA/MoS2) as electrode modification materials for detecting two different types of representative cancer biomarkers, hydrogen peroxide (H2O2) and carcinoembryonic antigen (CEA). The universal electrochemical biosensor showed a significant linear response to both H2O2 and CEA with the lowest detection limits of 0.23 μM and 0.01 ng mL−1, respectively, and it had high selectivity, reproducibility, and stability. The universal electrochemical biosensor is successfully applied to detect H2O2 released from human breast cancer (MCF-7) cells and CEA expressed on the surface of human cervical cancer (HeLa) cells. The developed biosensor has potential in the dynamic detection of the flux of H2O2 and the expression level of CEA from living cells. The high sensitivity of this universal sensor provides a novel strategy for simultaneously detecting multiple cancer biomarkers.

越来越多的电化学生物传感器被用于检测具有高灵敏度的单一生物活性物质,而不是具有不同性质的多种生物活性物质。因此,我们在普鲁士蓝中加入Cu和Fe元素,形成普鲁士蓝类似物(PBA),以提高普鲁士蓝的电化学催化活性。同时,采用二硫化钼作为材料衬底,增加了复合材料的电化学活性位点。我们利用复合材料(CuFe PBA/MoS2)作为电极修饰材料构建了通用电化学传感平台,用于检测过氧化氢(H2O2)和癌胚抗原(CEA)两种不同类型的代表性癌症生物标志物。该通用型电化学生物传感器对H2O2和CEA均具有良好的线性响应,最低检出限分别为0.23 μM和0.01 ng mL−1,具有较高的选择性、重复性和稳定性。该通用电化学生物传感器成功应用于检测人乳腺癌(MCF-7)细胞释放的H2O2和人宫颈癌(HeLa)细胞表面表达的CEA。该传感器在动态检测活细胞中H2O2通量和CEA表达水平方面具有一定的应用前景。这种通用传感器的高灵敏度为同时检测多种癌症生物标志物提供了一种新的策略。
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引用次数: 1
Dodecahedral NC-doped CoSe2 nanoparticles with excellent stability for high-performance flexible solid-state supercapacitors 具有优异稳定性的十二面体nc掺杂CoSe2纳米粒子,用于高性能柔性固态超级电容器
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-08-15 DOI: 10.1016/j.jelechem.2023.117612
Xiaojuan Wang , Cheng Qian , Tian Zou , Hao Ding , Feng Jiang , Huiyu Li , Haijing Cao , Zebo Fang , Yan Xu , Jinkun Liu , Yanyan Zhu

In this study, CoSe2/NC composites with stable dodecahedral structures were prepared by a simple one-step carbonization-selenization method using ZIF-67 as the precursor, and the effect of annealing time on their morphology and properties was investigated. SEM and TEM characterization results showed that the material with an annealing time of 1 h had the most stable framework structure and complete selenization. Under a three-electrode system with 2.0 M KOH as the electrolyte, CoSe2/NC-1 possesses a high capacity of 554.4F/g at 1 A/g and excellent cycling stability (92% capacity retention after 21,000 cycles). In addition, a flexible solid-state supercapacitor was assembled with CoSe2/NC-1 as the positive electrode and AC as the negative electrode. The power density was 800 W/Kg at 1 A/g, and the cycling stability was tested at 91.53% after 6000 cycles at 2 A/g. The flexible solid-state supercapacitors were tested for suppleness, and their voltage could still reach 1.6 V with stable specific capacity and light up LED bulbs when measured at 0°, 90° and 180°. Undoubtedly, the CoSe2/NC-1 material prepared in this study exhibits promising electrochemical characteristics, making it a viable candidate for implementation in flexible solid-state supercapacitors.

本研究以ZIF-67为前驱体,采用简单的一步碳化-硒化法制备了具有稳定十二面体结构的CoSe2/NC复合材料,并研究了退火时间对其形貌和性能的影响。SEM和TEM表征结果表明,退火时间为1 h的材料具有最稳定的框架结构和完全的硒化。在以2.0 M KOH为电解液的三电极体系下,CoSe2/NC-1在1 a /g下具有554.4F/g的高容量,并且具有良好的循环稳定性(21,000次循环后容量保持率为92%)。此外,还以CoSe2/NC-1为正极,AC为负极组装了柔性固态超级电容器。功率密度为800 W/Kg,电压为1 A/g,在2 A/g下循环6000次,循环稳定性为91.53%。测试了柔性固态超级电容器的柔韧性,在0°、90°和180°测量时,其电压仍可达到1.6 V,比容量稳定,并能点亮LED灯泡。毫无疑问,本研究中制备的CoSe2/NC-1材料具有良好的电化学特性,使其成为柔性固态超级电容器的可行候选材料。
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引用次数: 1
Promoting active species generation by sculpting Co3S4/Co(OH)2 nanotubes with rich sulfide/hydroxide interfaces for efficient oxygen evolution reaction 利用丰富的硫化物/氢氧化物界面雕刻Co3S4/Co(OH)2纳米管促进高效析氧反应的活性物质生成
IF 4.5 3区 化学 Q1 Chemical Engineering Pub Date : 2023-08-15 DOI: 10.1016/j.jelechem.2023.117619
Defeng Qi , Ying Wang , Xinru Xu , Xiao Jiang , Mushtaq Ahmad , Zhao Chao , Zhenyi Yu , Meiling Lian , Yong Wang , Zhen Zhang

Nanostructured transition metal sulfides (TMSs) have attracted great attention owing to their superior electric conductivity and easy redox reaction properties in oxygen evolution reaction (OER) catalysts. However, the strong metal-metalloid bonds (M−S) and metalloid-metalloid (SS) bonds in the crystal structure of TMSs are difficult to break, which might result in the insufficient formation of electrocatalytically active metal hydroxide species on the surface and prevent the realization of their full OER potential. Herein, we demonstrate an approach by sculpting Co(OH)2 on Co3S4 nanotubes (Co3S4/Co(OH)2) as highly reactive and stable electrocatalysts for efficient OER. The electron transfer between cobalt and sulfur and the pre-sculpted Co(OH)2 promote the formation of rich hydroxide active species on the surface of Co3S4/Co(OH)2. The optimized Co3S4/Co(OH)2–0.8 catalyst possesses excellent electrocatalytic activity for OER in an alkaline medium, with a relatively low OER overpotential of 269 mV (at 10 mA cm−2) and a Tafel slope of 95.2 mV dec-1. This work provides a new sight of designing TMS electrocatalysts for practical application in efficient water splitting.

纳米结构的过渡金属硫化物(tms)因其优异的导电性和在析氧反应(OER)催化剂中易于氧化还原反应而受到广泛关注。然而,tms晶体结构中的强金属-类金属键(M−S)和金属-类金属键(SS)难以断裂,这可能导致表面电催化活性金属氢氧化物的形成不足,阻碍其OER电位的充分发挥。在这里,我们展示了一种通过在Co3S4纳米管(Co3S4/Co(OH)2)上雕刻Co(OH)2作为高效OER的高活性和稳定的电催化剂的方法。Co3S4/Co(OH)2表面通过钴和硫之间的电子转移和预雕刻的Co(OH)2促进了丰富的氢氧化物活性物质的形成。优化后的Co3S4/Co(OH)2 - 0.8催化剂在碱性介质中具有良好的OER电催化活性,OER过电位较低,为269 mV (10 mA cm−2),Tafel斜率为95.2 mV dec1。本研究为TMS电催化剂在高效水分解中的应用提供了新的思路。
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引用次数: 0
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Journal of Electroanalytical Chemistry
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