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A Sensing Platform Based on Ni/Mn Bimetal-Organic Framework for Electrochemical Detection of Osimertinib 基于镍/锰双金属有机框架的传感平台用于奥希替尼的电化学检测
IF 3.1 4区 化学 Q2 Chemistry Pub Date : 2023-12-07 DOI: 10.1007/s12678-023-00857-4
Zahra Mirzaei Karazan, Mahmoud Roushani

In this study, the synthesis and properties of a selective electrochemical sensor for the determination of osimertinib (OSIM) as an anticancer drug using the bimetal-organic framework (MOF) were reported. Herein, MOF based on nickel/manganese (Ni/Mn-MOFs) was successfully created using the solvothermal method and applied for the amperometric detection of OSIM. Then, Ni/Mn-MOF was analyzed through a field emission scanning electron microscope (FE-SEM) and X-ray diffraction (XRD). The electrocatalytic performance of the introduced MOF is used in the electrochemical determination of the OSIM drug. The synthesized MOF leads to a noticeable improvement in the electrochemical performance which is ascribed to the many electrocatalytic sites, wide electrode–electrolyte contact area, and excellent electrical conductivity. This is the first study on the use of Ni/Mn-MOF to detect of OSIM. The Ni/Mn-MOF modified glassy carbon electrode (Ni/Mn-MOF/GCE) exhibited a good linear range from 0.5 to 800 μM and 800 to 1800 μM with a low detection limit (LOD) as 0.16 μM. In addition, the proposed sensor possessed good anti-interference properties, repeatability, stability, and reproducibility. The mentioned substrate to detect OSIM in the samples of blood serum was successfully applied. This research displays that MOFs are reliable materials for designing effective electrochemical sensors to detect drugs easily. The existing research results provide insights into the promotion and development of the bimetal-organic framework in the field of electrochemical applications and promising for usage in other electrochemical studies.

本研究报告了利用双金属有机框架(MOF)测定抗癌药物奥西替尼(OSIM)的选择性电化学传感器的合成及其特性。本文采用溶热法成功制备了基于镍/锰(Ni/Mn-MOFs)的MOF,并将其应用于OSIM的安培检测。然后,通过场发射扫描电子显微镜(FE-SEM)和 X 射线衍射(XRD)对镍/锰-MOF 进行了分析。引入的 MOF 的电催化性能被用于 OSIM 药物的电化学测定。合成的 MOF 明显改善了电化学性能,这归功于其众多的电催化位点、宽广的电极-电解质接触面积和优异的导电性。这是首次使用 Ni/Mn-MOF 检测 OSIM 的研究。经 Ni/Mn-MOF 修饰的玻璃碳电极(Ni/Mn-MOF/GCE)在 0.5 至 800 μM 和 800 至 1800 μM 之间具有良好的线性范围,检出限(LOD)低至 0.16 μM。此外,该传感器还具有良好的抗干扰性、重复性、稳定性和再现性。上述基底已成功用于检测血清样品中的 OSIM。这项研究表明,MOFs 是设计有效电化学传感器的可靠材料,可轻松检测药物。现有研究成果为双金属有机框架在电化学应用领域的推广和发展提供了启示,并有望用于其他电化学研究。
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引用次数: 0
Correction to: Pt‑modified Fe3O4 Supported on Ni Foam Nanocomposite for Electrocatalytic Nitrate Reduction to Ammonia 更正为以镍泡沫纳米复合材料为支撑的铂改性 Fe3O4 电催化硝酸盐还原氨的研究
IF 3.1 4区 化学 Q2 Chemistry Pub Date : 2023-12-04 DOI: 10.1007/s12678-023-00858-3
S. Mahmood, O. Alduhaish, Muhammad Ammar, Shahid Khan, Niaz Ahmad, G. A. Ashraf, Noshin Afshan, Noor Hassan
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引用次数: 0
Electrochemical Activity of Carbon-Supported Pt-Nanoparticles: Effect of Pt-Precursor Ligand and/or Presence of Anions During Polyol Synthesis 碳负载的pt纳米颗粒的电化学活性:pt前体配体和/或阴离子在多元醇合成过程中的影响
IF 3.1 4区 化学 Q2 Chemistry Pub Date : 2023-11-30 DOI: 10.1007/s12678-023-00856-5
Kristian Juul Omann, Raghunandan Sharma, Shuang Ma Andersen

This study revisits the impacts of the presence of OH and Cl anions and/or different forms of Pt precursors during polyol synthesis of carbon-supported electrocatalysts. Efficiency of the synthesis process in terms of the %conversion of a Pt complex to Pt metal has been quantified. It is observed that Pt precursors based on [PtCl6]2− are reduced easily compared to those based on [Pt(OH)6]2−. Furthermore, presence of excess Cl during synthesis results in decreased %conversion and reduced ECSA, which is opposite from other reported work synthesized at higher temperature and pure solvents. For Pt/C synthesis under mild conditions, 100 °C and 30 vol% EG in water as solvent, presence of OH during synthesis decreases the ECSA and hence increases the Pt nanoparticle size and change of catalyst surface structure. Finally, a method to get insights into the surface structure of Pt-nanoparticles through analysis of the H-adsorption/H-desorption peaks has been proposed.

Graphical Abstract

本研究回顾了OH -和Cl -阴离子的存在和/或不同形式的Pt前体在碳负载电催化剂多元醇合成过程中的影响。以Pt配合物转化为Pt金属的百分比来量化合成过程的效率。与基于[Pt(OH)6]2−的铂前驱体相比,基于[PtCl6]2−的铂前驱体更容易还原。此外,合成过程中过量Cl−的存在导致转化率降低和ECSA降低,这与其他在高温和纯溶剂下合成的研究相反。在较温和的条件下,以100°C和30 vol% EG为溶剂,合成Pt/C时,OH -的存在降低了ECSA,从而增加了Pt纳米颗粒的尺寸和催化剂表面结构的变化。最后,提出了一种通过分析h -吸附/ h -解吸峰来深入了解pt纳米颗粒表面结构的方法。图形抽象
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引用次数: 0
Dual-Atomic Porphyry Molecular Systems as Efficient Electrocatalysts for N2 Reduction Reaction: a Theoretical Investigation 双原子斑岩分子体系作为N2还原反应高效电催化剂的理论研究
IF 3.1 4区 化学 Q2 Chemistry Pub Date : 2023-11-21 DOI: 10.1007/s12678-023-00855-6
Anuj Kuma, Ram K. Gupta, Nangan Senthilkumar, Bidhan Pandit, Abdullah M. Al-Enizi, Mohd Ubaidullah

Metallo-porphyry-based frameworks have been utilized to construct single-atom catalysts (SACs), but their use in the fabrication of dual-atom catalysts (DACs) for the nitrogen reduction reaction (NRR) electrocatalytically is limited. Herein, a binuclear phthalocyanine (bN-Pc) was assessed based on a theoretical model to construct dual-atom systems (MoMo-bN-Pc, WW-bN-Pc, and MoW-bN-Pc) along with NRR activity and respective mechanisms, exploiting density functional theory (DFT) calculations. A cis-bridged N2-adduct, with N-atoms coordinating on both sides, resulted in these dual-atom systems, keeping adjacent metals in close proximity. Gibbs free energy studies revealed that the potential-determining step (PDS) for these catalysts appeared to be the protonation of adsorbed N2 on dual-atom sites (*N2H). Following the enzymatic pathway, MoW-bN-Pc had the lowest limiting potential (− 0.32 V) than other systems, indicating its higher NRR activity. The synergistic orbital coupling between Mo(4d) and W(5d) due to their intimate proximity significantly raised the energy of the highest occupied molecular orbital of Mo to facilitate the electron donation to the antibonding orbital of N2, endowing the NRR of MoW-bN-Pc as compared to other systems. This work is sure to create interest for future studies on the construction of DAC-based active sites using molecular models.

基于金属斑岩的框架已被用于构建单原子催化剂(SACs),但它们在制备用于氮还原反应(NRR)的双原子催化剂(dac)中的应用受到限制。本文利用密度泛函理论(DFT)计算,基于理论模型构建双核酞菁(bN-Pc)双原子体系(MoMo-bN-Pc、WW-bN-Pc和MoW-bN-Pc)以及NRR活性和各自机制。顺式桥接的n2加合物,两侧有n原子配位,形成了这些双原子体系,使相邻的金属保持在很近的距离。Gibbs自由能研究表明,这些催化剂的电位决定步骤(PDS)似乎是吸附N2在双原子位点(*N2H)上的质子化反应。在酶促途径下,MoW-bN-Pc具有最低的极限电位(- 0.32 V),表明其具有较高的NRR活性。由于Mo(4d)和W(5d)之间的密切关系,它们之间的协同轨道耦合显著提高了Mo的最高已占据分子轨道的能量,从而促进了电子给能到N2的反键轨道,从而赋予了MoW-bN-Pc相对于其他体系的NRR。这项工作必将为未来利用分子模型构建dac基活性位点的研究创造兴趣。
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引用次数: 0
Electrochemical Deposition of Pt and Pd on TiO2 Nanotubes for Application in the Photoelectrocatalytic Conversion of Biomethane and Biogas for Hydrogen Generation Pt和Pd在TiO2纳米管上的电化学沉积及其在生物甲烷和沼气光电催化转化制氢中的应用
IF 3.1 4区 化学 Q2 Chemistry Pub Date : 2023-11-16 DOI: 10.1007/s12678-023-00854-7
Laís Bresciani, Simone Stülp

The photoelectrocatalytic conversion of biomethane/biogas using semiconductor materials is a promising method for production of green H2, the fuel of the future. In this work, TiO2 nanotubes (TiO2NTs) prepared by electrochemical anodization were modified with Pt and Pd nanoparticles by electrochemical deposition using cyclic voltammetry, producing TiO2NTs/Pt and TiO2NTs/Pd catalysts, respectively. Evaluation of the morphology, composition, and crystallinity of the materials employed scanning electron microscopy, energy dispersive spectroscopy, and X-ray diffraction. The photoactivities of the electrodes were studied using linear scanning voltammetry, chronoamperometry, and electrochemical impedance spectroscopy. The introduction of Pt and Pd on the TiO2NTs resulted in electrodes that presented excellent photogenerated charge separation and transfer properties. In the presence of methane, the current densities obtained increased further, by around 2.23- and 2.95-fold for the TiO2NTs/Pt and TiO2NTs/Pd electrodes, respectively, compared to the pure TiO2NTs, confirming the capacity of CH4 to act as a hole scavenger. The maximum amounts of H2 obtained from the photoelectrocatalytic conversion of methane were 120.7, 304.7, and 393 mmol.cm−2 for the TiO2NTs, TiO2NTs/Pt, and TiO2NTs/Pd electrodes, respectively, clearly showing the positive contribution of the metallic nanoparticles electrodeposited on the TiO2NTs surface. A lower amount of H2 was produced in the photoelectrocatalytic conversion of biogas, with the possible occurrence of additional reactions, such as the reduction of CO2.

Graphical Abstract

利用半导体材料对生物甲烷/沼气进行光电催化转化是一种很有前途的生产未来燃料——绿色H2的方法。本文采用循环伏安法对电化学阳极氧化法制备的TiO2纳米管(TiO2NTs)进行了Pt和Pd纳米粒子的电化学沉积修饰,分别制备了TiO2NTs/Pt和TiO2NTs/Pd催化剂。利用扫描电子显微镜、能量色散光谱和x射线衍射对材料的形态、组成和结晶度进行评价。采用线性扫描伏安法、计时安培法和电化学阻抗法研究了电极的光活性。在TiO2NTs上引入Pt和Pd,使得电极具有优异的光电电荷分离和转移性能。在甲烷的存在下,得到的电流密度进一步增加,与纯tio2相比,TiO2NTs/Pt和TiO2NTs/Pd电极分别增加了约2.23倍和2.95倍,证实了CH4的空穴清除剂作用。甲烷光电催化转化氢气的最大产氢量分别为120.7、304.7和393 mmol。对于TiO2NTs, TiO2NTs/Pt和TiO2NTs/Pd电极分别为cm−2,清楚地显示了电沉积在TiO2NTs表面的金属纳米颗粒的积极贡献。在沼气的光电催化转化过程中,氢气的产生量较低,并可能发生额外的反应,如CO2的还原。图形抽象
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引用次数: 0
Theoretical Study on the Electroreduction of CO2 to α-Olefins by Tandem Catalysis of Polymetallic Phthalocyanine Two-Dimensional Carbon-Rich Conjugated Frameworks (CCFs) 多金属酞菁二维富碳共轭框架串联催化CO2电还原制α-烯烃的理论研究
4区 化学 Q2 Chemistry Pub Date : 2023-11-14 DOI: 10.1007/s12678-023-00853-8
Jinping Du, Ling Guo
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引用次数: 0
Pt-modified Fe3O4 Supported on Ni Foam Nanocomposite for Electrocatalytic Nitrate Reduction to Ammonia 镍泡沫纳米复合材料负载pt改性Fe3O4电催化还原硝酸盐制氨
4区 化学 Q2 Chemistry Pub Date : 2023-11-11 DOI: 10.1007/s12678-023-00851-w
Sajid Mahmood, Osamah Alduhaish, Muhammad Ammar, Shahid Khan, Niaz Ahmad, Ghulam Abbas Ashraf, Noshin Afshan, Noor Hassan
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引用次数: 0
Hydrogen-Mediated Photoelectrocatalysis with Nickel-Modified Poly(Heptazine Imides) 镍修饰聚七嗪酰亚胺氢介导的光电催化
4区 化学 Q2 Chemistry Pub Date : 2023-11-11 DOI: 10.1007/s12678-023-00852-9
Sirlon F. Blaskievicz, Ivo F. Teixeira, Lucia H. Mascaro, Mariolino Carta, Neil B. McKeown, Yuanzhu Zhao, Frank Marken
Abstract Polymeric carbon nitrides (C 3 N 4 ) are photochemically active organic semiconductors that can be produced in a wide range of structural types. Here, a poly-(heptazine imide) containing nickel single atoms (Ni-PHI) is employed for photochemical hydrogen production and is compared to the non-nickel-doped semiconductor. Film deposits are formed on a platinum disk electrode (to detect hydrogen) and a coating of the molecularly rigid polymer of intrinsic microporosity PIM-1 is applied to (i) mechanically stabilize the photo-catalyst film without impeding photocatalysis and (ii) assist in the interfacial hydrogen capture/oxygen suppression process. In the presence of hole quenchers such as methanol or ethanol, anodic photocurrents linked to hydrogen production/oxidation are observed. A comparison with an experiment on glassy carbon confirms the formation of interfacial hydrogen as a mediator. The effects of hole quencher concentration are evaluated. The system Pt/Ni-PHI/PIM-1 is employed in a single-compartment photo-fuel cell. Graphical Abstract
摘要:聚合物碳氮化合物(c3n4)是光化学活性有机半导体,可以生产出各种结构类型。本文采用含镍单原子(Ni-PHI)的聚七嗪亚胺进行光化学制氢,并与未掺杂镍的半导体进行了比较。在铂盘电极上形成薄膜沉积(用于检测氢),并应用具有固有微孔的分子刚性聚合物(PIM-1)涂层来(i)在不阻碍光催化的情况下机械地稳定光催化剂薄膜,以及(ii)协助界面捕氢/抑氧过程。在孔猝灭剂如甲醇或乙醇存在的情况下,观察到与氢气产生/氧化有关的阳极光电流。通过与玻碳实验的比较,证实了界面氢作为介质的形成。评价了孔淬剂浓度的影响。Pt/Ni-PHI/PIM-1系统用于单室光燃料电池。图形抽象
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引用次数: 0
Nitrogen-Doped Carbon Derived from Metal Organic Frameworks (ZIF67) Modified Electrochemically with Non-precious Metal Nanoparticles: Synthesis and Application for Oxygen Evolution Reaction 非贵金属纳米粒子电化学修饰金属有机骨架(ZIF67)的氮掺杂碳:合成及其在析氧反应中的应用
4区 化学 Q2 Chemistry Pub Date : 2023-11-10 DOI: 10.1007/s12678-023-00848-5
Mostafa Torabi, Seyed Mahdi Shahrokhi, Reza Karimi Shervedani
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引用次数: 0
Correction to: Fabrication of Well‑dispersed IrO2 Anchored on rGO Composite for High‑Performance OER Electrocatalyst Application by Microwave‑Assisted Method 修正:用微波辅助方法制备用于高性能OER电催化剂的分散良好的IrO2锚定在氧化石墨烯复合材料上
IF 3.1 4区 化学 Q2 Chemistry Pub Date : 2023-11-02 DOI: 10.1007/s12678-023-00849-4
Pyeongkang Yoo, Mino Woo, Hae In Lee, Hee Soo Kim, Dong‑Ha Lim
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引用次数: 0
期刊
Electrocatalysis
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