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Glucosamine functionalized gold nanoparticles for specific detection and colorimetric assay of Glutathione from real samples 用于特异性检测和比色测定实际样品中谷胱甘肽的氨基葡萄糖功能化金纳米粒子
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4nj02620a
Anurag Kumar Singh, Saumya Singh, Raksha Singh, Manish Sharma, Ida Tiwari, Kaushal Kumar Upadhyay
In this study, we report an experimental protocol based on gold nano particles (GNPs) for the selective and efficient chromogenic detection and determination of glutathione from its two pharmaceutical samples viz. Maxiliv and Glutaderm in real time. The glucosamine hydrochloride driven hydrothermal (400C) wet chemical reduction of gold (III)chloride trihydrate resulted into gold sol with ruby red color exhibiting its surface plasmon resonance (SPR) at 521nm. The most frequent average size of these GNPs was found to be 23 nm while their concentration was evaluated to be 8.4 nM. The zeta potential measurements and interaction of these GNPs against NaCl of varying molarities indicated their long-term stability. These GNPs exhibited the morphology of nanowire in their SEM picture and produced a categorical color change from ruby red to blue selectively with GSH from a wide range of similar type of analytes in real time. The UV-Vis, FT-IR, XPS, SEM, TEM, AFM, EDAX, DLS, Zeta potential etc. were used to characterize the as synthesized GNPs as well as to study their interaction pattern with glutathione.
在本研究中,我们报告了一种基于金纳米粒子(GNPs)的实验方案,用于从 Maxiliv 和 Glutaderm 这两种药物样品中选择性、高效地实时检测和测定谷胱甘肽的色原。在盐酸氨基葡萄糖的驱动下,三水氯化金(III)经热液(400℃)湿化学还原后形成金溶胶,呈宝石红色,在 521 纳米波长处显示出表面等离子体共振(SPR)。这些 GNPs 最常见的平均尺寸为 23 nm,浓度为 8.4 nM。这些 GNPs 对不同摩尔浓度的 NaCl 的 zeta 电位测量和相互作用表明它们具有长期稳定性。这些 GNPs 在扫描电子显微镜(SEM)照片中呈现出纳米线的形态,并能从多种同类分析物中实时选择性地与 GSH 产生从宝石红色到蓝色的颜色变化。紫外可见光、傅立叶变换红外光谱、XPS、扫描电镜、TEM、原子力显微镜、EDAX、DLS、Zeta 电位等被用来表征合成的 GNPs,以及研究它们与谷胱甘肽的相互作用模式。
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引用次数: 0
Enhancing photocatalytic hydrogen evolution from water splitting over CaTaO2N via engineering surface of platinum cocatalyst 通过对铂协同催化剂表面进行工程设计,提高 CaTaO2N 光催化水分离制氢能力
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4nj03029j
Xuecheng Liu, Tingting Pei, Linjie Yan, Xiaoyi Lei, Tingting Zheng, Xia Ha, Hui Xu
The cocatalyst loading is of critical importance in efficient photocatalytic water splitting over perovskite oxynitrides. Perovskite CaTaO2N was synthesized for enhancing the photocatalytic hydrogen evolution via decoration of Pt cocatalyst by impregnation-reduction and photodeposition methods. The Pt-loaded CaTaO2N photocatalyst evolves 6.4 μmol H2 per hour, with an apparent quantum yield as high as 0.67% at the wavelength of 420 nm. Decorating cocatalyst with uniform dispersion and intimate contact onto the surface of narrow-bandgap perovskite oxynitrides is an efficient method to upgrade the photocatalytic hydrogen evolution from water splitting.
在过氧化物氧化物上进行高效光催化水分离时,茧催化剂的负载量至关重要。通过浸渍-还原和光沉积方法,合成了包晶氧化物 CaTaO2N,并在其中添加了铂催化剂,从而提高了光催化氢气进化的能力。铂负载的 CaTaO2N 光催化剂每小时可产生 6.4 μmol H2,在波长为 420 纳米时,表观量子产率高达 0.67%。在窄带隙过氧化物氮化物表面装饰均匀分散和紧密接触的共催化剂,是提高光催化水分裂氢气进化的有效方法。
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引用次数: 0
HF-Addition to Haloacetyl Fluorides in Superacidic Media 超酸性介质中卤乙酰氟化物的 HF 添加剂
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4nj02884h
Sebastian Steiner, Zurwa Shafiq, Alexander Nitzer, Dirk Hollenwäger, Andreas Kornath
The reactions of difluoroacetyl fluoride and trifluoroacetyl fluoride were investigated in the binary superacid HF/SbF5 by low-temperature NMR spectroscopy. Whereas both haloacetyl fluorides form oxonium species after the addition of HF, the protonated acyl fluorides were not observed. Protonated 1,1,2,2-tetrafluoroethanol was isolated as a solid and represents an example of a protonated α-fluoroalcohol. The salt was characterized by low-temperature vibrational spectroscopy and single-crystal X-ray diffraction. [CHF2CF2OH2][SbF6] crystallizes in the triclinic space group P−1 with two formula units per unit cell. Protonated perfluoroethanol is only stable in solution. The reactivity of both haloacyl fluorides is discussed based on quantum chemical calculations at the MP2/aug-cc-pVTZ-level of theory.
通过低温核磁共振光谱研究了二氟乙酰氟和三氟乙酰氟在二元超酸 HF/SbF5 中的反应。虽然这两种卤乙酰氟化物在加入 HF 后会形成羰基物种,但却没有观察到质子化酰基氟化物。质子化 1,1,2,2- 四氟乙醇以固体形式分离出来,是质子化 α-氟乙醇的一个实例。该盐通过低温振动光谱法和单晶 X 射线衍射法进行了表征。[CHF2CF2OH2][SbF6]在三菱空间群 P-1 中结晶,每个单胞有两个式样单元。质子化全氟乙醇仅在溶液中稳定。根据 MP2/aug-cc-pVTZ 级理论的量子化学计算,讨论了这两种卤酰氟的反应性。
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引用次数: 0
Cucurbit[8]uril Mediated Triphenylamine Coumarin Derivative Cascade Assembly for NIR Targeted Cell Imaging 葫芦[8]脲介导的三苯胺香豆素衍生物级联组装用于近红外靶向细胞成像
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4nj01843e
Zhen-Hai Yu, Hui-Juan Wang, Qingwen Cheng, Heng-Yi Zhang, Yu Liu
The coumarin-modified tris[4-(4-pyridyl)phenyl]amine compound was encapsulated in the cavity of cucurbit[8]uril with a 2:3 stoichiometric ratio, which not only effectively enhances guest fluorescence emission with hypsochromic shift about 51 nm by macrocycle confinement, but also cascades assembling with β-cyclodextrin-grafted hyaluronic acid (HACD) to construct a ternary supramolecular network. Furthermore, doping with Sulfo-Cyanine 5 into β-cyclodextrin cavity of HACD through host-guest interaction achieved a high efficiency Föster resonance energy transfer system from supramolecular network to dyes, which successfully applied to the near-infrared mitochondria-targeted imaging in Hela cells.
香豆素修饰的三[4-(4-吡啶基)苯基]胺化合物以2:3的化学计量比被包封在葫芦素[8]脲的空腔中,不仅通过大环限制有效地增强了客体荧光发射,产生约51 nm的低色移,而且与β-环糊精接枝透明质酸(HACD)级联组装,构建了三元超分子网络。此外,通过主客体相互作用,在HACD的β-环糊精空腔中掺入Sulfo-Cyanine 5,实现了从超分子网络到染料的高效福斯特共振能量转移系统,并成功应用于Hela细胞的近红外线粒体靶向成像。
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引用次数: 0
Effect of Substitution on Second-order Nonlinear Optical Properties in Ferrocene Appended Donor-π-Acceptor Y-shaped Trifluoromethyl Imidazole Chromophores 二茂铁添加供体-π-受体 Y 型三氟甲基咪唑发色团中取代作用对二阶非线性光学特性的影响
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4nj02079k
Selvam Prabu, Francesco Fagnani, Alessia Colombo, Claudia Dragonetti, Dominique Roberto, Logesh Mathivathanan, Nallasamy Palanisami
New Y-shaped ferrocene (Fc) conjugated trifluoromethyl substituted imidazole (IM) donor-π-acceptor [(D-π)2-IM-D′-π-CF3] “push-pull” chromophores [(Fc-CH=CH)2-IM-C6H4-R-C6H4-CF3] {R= -OCH3 (1); -N(C2H5)2 (2)} were synthesized and structurally characterized. The structure of the chromophores was confirmed by single crystal X-ray diffraction studies. They crystallized in triclinic with P-1 (for 1) and monoclinic with P21/c (for 2) space group. Thermogravimetric analysis (TGA) was used to study the thermal stability of chromophores 1 and 2, and it was found that both were stable at temperatures of about 300 °C. The redox properties were studied by cyclic voltammetry (CV), which revealed one-electron transfer from the ferrocene to ferrocenium ion (Fe2+↔Fe3+), and potentials were utilized to calculate the energy gap (that is 2.16 eV for 1 and 2.12 eV for 2). The second order nonlinear optical (NLO) properties of the chromophores 1 and 2 were explored by Electric-Field-Induced Second Harmonic generation (EFISH) technique in CHCl3 solution with an incident wavelength of 1907 nm. μβEFISH value are: −725 ×10-48 esu and −806 ×10-48 esu, for (1) and (2) respectively. The μβEFISH values were feebly decreased, compared with reported ferrocene conjugated Y-shaped imidazole chromophores, due to the substitution on imidazole nitrogen, which increases the steric hindrance and reduces the ICT process in the chromophores. In addition, frontier molecular orbital levels, excited and ground state dipole moments (μe and μg), and electronic absorption spectra were studied by density functional theory (DFT) and time-dependent density functional theory (TD-DFT) with B3LYP method using 6-31+G** as basis set.
合成了新型 Y 型二茂铁(Fc)共轭三氟甲基取代咪唑(IM)供体-π-受体[(D-π)2-IM-D′-π-CF3]"推拉 "发色团[(Fc-CH=CH)2-IM-C6H4-R-C6H4-CF3] {R= -OCH3 (1); -N(C2H5)2 (2)} ,并对其进行了结构表征。单晶 X 射线衍射研究证实了发色团的结构。它们的结晶空间群分别为 P-1(1)三linic 和 P21/c(2)单斜。热重分析(TGA)被用来研究发色团 1 和 2 的热稳定性,结果发现这两种发色团在约 300 °C 的温度下都很稳定。通过循环伏安法(CV)研究了氧化还原特性,发现二茂铁与铁硒离子(Fe2+↔Fe3+)之间存在单电子转移,并利用电位计算了能隙(1 为 2.16 eV,2 为 2.12 eV)。在入射波长为 1907 nm 的 CHCl3 溶液中,利用电场诱导二次谐波发生(EFISH)技术探讨了发色团 1 和 2 的二阶非线性光学(NLO)特性:(1)和(2)的μβEFISH 值分别为:-725 ×10-48 esu 和 -806 ×10-48 esu。与已报道的二茂铁共轭 Y 型咪唑发色团相比,μβEFISH 值微弱下降,这是由于咪唑氮上的取代增加了立体阻碍,降低了发色团中的 ICT 过程。此外,还以 6-31+G** 为基集,通过密度泛函理论(DFT)和时间相关密度泛函理论(TD-DFT),采用 B3LYP 方法研究了前沿分子轨道水平、激发态和基态偶极矩(μe 和 μg)以及电子吸收光谱。
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引用次数: 0
Construction of a novel isopinocamphone-based fluorescent probe for rapid and specific detection of ClO‒ and its application in environmental analysis and biological imaging 构建一种基于异松霉素的新型荧光探针,用于快速特异性检测 ClO-,并将其应用于环境分析和生物成像中
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4nj02375g
Qian Ye, Kai Xu, Zhiyuan Meng, Xinyan Li, Zhonglong Wang, Shifa Wang
Hypochlorite (ClO‒) is an important oxidant and disinfectant in the human body and nature. Nevertheless, it may exert adverse impact on the environment and biological systems when its concentration is not appropriate. It is necessary to develop an accurate method for detecting ClO‒. Herein, an isopinocamphone-based fluorescent probe DMTI for selective recognition of ClO‒ was successfully synthesized. DMTI exhibited an obvious fluorescence enhancement towards ClO‒ accompanied by its color shifted from colorless to bright blue. The experimental results displayed that the probe DMTI had the merits of high selectivity, good sensitivity, wide detection pH range (6-10) for ClO‒ detection, and the detection limit reached 2.6×10-7 mol/L. The sensing mechanism of DMTI to ClO‒ was confirmed by the 1H NMR and HRMS analysis. More importantly, the probe DMTI has been effectively utilized to detect ClO‒ in environmental water samples, living cells and zebrafish encouraged by its excellent performance.
次氯酸盐(ClO-)是人体和自然界中一种重要的氧化剂和消毒剂。然而,当次氯酸盐的浓度不合适时,它可能会对环境和生物系统产生不利影响。因此,有必要开发一种精确检测 ClO- 的方法。在此,我们成功合成了一种基于异品酮的荧光探针 DMTI,用于选择性识别 ClO-。DMTI 对 ClO- 具有明显的荧光增强作用,颜色也从无色变为亮蓝色。实验结果表明,探针 DMTI 具有选择性高、灵敏度好、检测 ClO- 的 pH 值范围宽(6-10)等优点,检测限达到 2.6×10-7 mol/L。1H NMR 和 HRMS 分析证实了 DMTI 对 ClO- 的感应机制。更重要的是,探针 DMTI 在环境水样、活细胞和斑马鱼中检测 ClO- 的优异性能得到了有效利用。
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引用次数: 0
Sustainable Layered Double Hydroxide-Pine Cone Biochar (LDH/PCBC) composite for Enhanced Removal of Ciprofloxacin from Water 可持续的层状双氢氧化物-松果生物炭(LDH/PCBC)复合材料用于提高水中环丙沙星的去除率
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4nj02064b
Prakash Bobde, Jitendra K Pandey, Ranjit Kumar, Amit Kumar Sharma, Sukdeb Pal, Shikha Wadhwa
To address ciprofloxacin's (CPF) persistent presence in water and potential ecological and health hazard, the challenge is to develop an effective method for its removal from wastewater. This work is aimed at optimizing the adsorptive removal of ciprofloxacin (CPF) utilizing a Layered Double Hydroxide Pine Cone Biochar composite (LDH/PCBC). Response Surface Methodology (RSM) is employed to design the experiments to obtain optimal experimental conditions for improved adsorption processes. The CPF removal efficiency of LDH/PCBC from aqueous solution is found to be 97.6% under optimized conditions (pH = 7, adsorbent dose = 0.45 g/L, initial CPF concentration = 52 mg/L and temperature = 303K). The Freundlich isotherm confirms the best fit, and the Langmuir adsorption capacity of the LDH/PCBC is determined to be 476.2 mg/g at 303K. The pseudo-second-order model fitted the best for adsorption kinetics, suggesting that the adsorption process is directed by chemisorption. The thermodynamic investigation confirmed the endothermic and spontaneous adsorption process (ΔHo=56.9 kJ and ΔGo from -3.2 kJ at 278K to -10.8 kJ at 318K). The study reveals that the LDH/PCBC can be reused effectively with insignificant loss of removal efficiency (~ 6%). The cost of the development and large-scale application of LDH/PCBC for the removal of CPF is $988.75 per ton. The results indicate that the LDH/PCBC outperforms the reported adsorbents for sustainable removal of CPF from aqueous solutions. This is the first report on the use of LDH/PCBC as a cheaper and environment friendly method for the removal of CPF from water.
环丙沙星(CPF)长期存在于水中,对生态和健康具有潜在危害,因此,开发一种有效的方法来去除废水中的环丙沙星是一项挑战。本研究旨在利用层状双氢氧化物松果生物炭复合材料(LDH/PCBC)优化环丙沙星(CPF)的吸附去除。采用响应面方法(RSM)设计实验,以获得改善吸附过程的最佳实验条件。在优化条件下(pH = 7、吸附剂剂量 = 0.45 g/L、CPF 初始浓度 = 52 mg/L、温度 = 303K),LDH/PCBC 从水溶液中去除 CPF 的效率为 97.6%。Freundlich 等温线的拟合效果最佳,在 303K 温度下,LDH/PCBC 的朗缪尔吸附容量被确定为 476.2 mg/g。伪二阶模型对吸附动力学的拟合效果最好,表明吸附过程是由化学吸附引导的。热力学研究证实了吸附过程是内热和自发的(ΔHo=56.9 kJ,ΔGo 从 278K 时的 -3.2 kJ 到 318K 时的 -10.8 kJ)。研究表明,LDH/PCBC 可以有效地重复使用,而且去除效率损失不大(约 6%)。开发和大规模应用 LDH/PCBC 去除氯化石蜡的成本为每吨 988.75 美元。结果表明,LDH/PCBC 在可持续去除水溶液中的 CPF 方面优于已报道的吸附剂。这是首次报道使用 LDH/PCBC 作为一种更便宜、更环保的方法来去除水中的氯化石蜡。
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引用次数: 0
EPICHLOROHYDRIN-BASED CuAAC DENDRIMERS WITH CALIX[4]ARENE CORE AND POLAR HYDROXYL/OXYETHYL TERMINAL GROUPS: SYNTHESIS, AGGREGATION AND USE IN CATALYSIS 以钙钛矿[4]烯为核心、具有极性羟基/氧乙基末端基团的环氧乙烷基 CuAAC 二聚体:合成、聚集和催化应用
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4nj02942a
Eugeny Ocherednyuk, Elza Sultanova, Egor G. Makarov, Angelina A. Fedoseeva, Artur Khannanov, Vladimir Evtugin, Svetlana Solovieva, Vladimir Burilov, Igor S. Antipin
1st generation dendrimers containing polar hydroxyl and both 1st and 2nd generation dendrimers with oxyethyl groups were obtained using convergent approach and CuAAC reaction. Three types of dendrimer nuclei were utilized: the macrocyclic nucleus of calix[4]arene bearing 2/4 dendron and 2/4 alkyl fragments and the non-macrocyclic analog of calixarene bearing one dendron/alkyl fragment. Nanoparticle tracking analysis reveals self-organization of the obtained dendrimers in aqueous solution into submicron/nanoparticles with sizes of 80-250 nm. The lowest CAC values in the series are possessed by tetra-alkyl substituted calix[4]arenes (1.6-1.8 μM), while the low molecular weight analog of calixarenes possesses a CAC one to two orders of magnitude larger (44-350 μM). When the obtained dendrimers were used as stabilizers of palladium nanoparticles, the formation of spherical palladium nanodendrites (50-60 nm ) consisting of metal Pd and PdO was found using TEM and SAED. The micellar effect of using stabilized palladium particles with dendrimers at concentrations higher their CAC in catalysis of Suzuki reactions and nitro aromatics reduction is shown. In the p-nitrophenol reduction reaction, the catalytic activity of the obtained systems (maximum kapp in series was 0.47 min-1) exceeds many known Pd-based systems.
利用聚合法和 CuAAC 反应,获得了含有极性羟基的第一代树状分子以及含有氧乙基的第一代和第二代树状分子。利用了三种树枝状聚合物核:含有 2/4 个树枝状基团和 2/4 个烷基片段的钙[4]炔大环核,以及含有一个树枝状基团/烷基片段的钙[4]炔非大环类似物。纳米粒子跟踪分析表明,所获得的树枝状聚合物在水溶液中自组织成尺寸为 80-250 纳米的亚微米/纳米粒子。在该系列中,四烷基取代的钙[4]烯的 CAC 值最低(1.6-1.8 μM),而钙烯类的低分子量类似物的 CAC 值则高出一到两个数量级(44-350 μM)。当把获得的树枝状聚合物用作钯纳米粒子的稳定剂时,利用 TEM 和 SAED 发现形成了由金属钯和钯氧化物组成的球形钯纳米树枝状物(50-60 nm)。结果表明,在催化铃木反应和硝基芳烃还原反应时,使用浓度高于 CAC 的树枝状聚合物稳定钯粒子具有胶束效应。在对硝基苯酚还原反应中,所获得体系的催化活性(系列中的最大 kapp 为 0.47 min-1)超过了许多已知的钯基体系。
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引用次数: 0
Boosting the catalytic activity via acid-base synergistic effect for CO2 and methanol direct to dimethyl carbonate 通过酸碱协同效应提高二氧化碳和甲醇直接转化为碳酸二甲酯的催化活性
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4nj01567c
Tian-Tian Huang, Yu-Ping Xu, Zheng-Lan Bai, Ming-Sheng Wang, Bin-Wen Liu, Zhong-Ning Xu, Guo-Cong Guo
Direct synthesis of dimethyl carbonate (DMC) from CO2 and CH3OH holds significant economic and environmental value. Numerous catalysts have been employed for this reaction, yet further enhancement of its activity requires a deeper understanding of the catalyst's structure-activity relationship and catalytic mechanism. In this study, we utilized structurally well-defined and highly tunable MOF-808 as a research platform. Functionalizing MOF-808 with ethylenediamine (MOF-808-ED) boosted the space time yield of DMC from 3.25 mmol·g-1·h-1 to 7.23 mmol·g-1·h-1. Experimental results demonstrate that the reaction involves acid-base synergistic catalysis, where an appropriate balance of acid-base sites content is crucial for CO2 and CH3OH to produce DMC, as it facilitates the formation of the key intermediates (CH3OCOO*). Additionally, the nucleophilicity of N is stronger than that of O, further promoting the catalyst's enrichment and activation of CO2. Finally, employing in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) testing, we elucidated the mechanism by which the MOF-808-ED catalyst, with -NH2 as base sites and Zr as acid sites, facilitates the synergistic catalysis of the reaction. This study provides insights into the synergistic effects of acid-base sites on the synthesis of DMC from CO2 and methanol, offering valuable guidance for the development of high-performance catalysts.
从二氧化碳和 CH3OH 直接合成碳酸二甲酯(DMC)具有重要的经济和环境价值。该反应已使用了大量催化剂,但要进一步提高其活性,还需要对催化剂的结构-活性关系和催化机理有更深入的了解。在本研究中,我们利用结构明确且高度可调的 MOF-808 作为研究平台。用乙二胺对 MOF-808 进行官能化(MOF-808-ED),可将 DMC 的时空产率从 3.25 mmol-g-1-h-1 提高到 7.23 mmol-g-1-h-1。实验结果表明,该反应涉及酸碱协同催化,酸碱位点含量的适当平衡对 CO2 和 CH3OH 生成 DMC 至关重要,因为它有利于关键中间产物(CH3OCOO*)的形成。此外,N 的亲核性强于 O,进一步促进了催化剂对 CO2 的富集和活化。最后,通过原位漫反射红外傅立叶变换光谱 (DRIFTS) 测试,我们阐明了以 -NH2 为碱基位点和以 Zr 为酸性位点的 MOF-808-ED 催化剂促进该反应协同催化的机理。这项研究深入揭示了酸碱位点对二氧化碳和甲醇合成 DMC 的协同作用,为开发高性能催化剂提供了宝贵的指导。
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引用次数: 0
Co@Ir Core-shell Nanochain Aerogels for Hydrogen Evolution Reaction and Oxygen Evolution Reaction in Alkaline Media 用于碱性介质中氢气进化反应和氧气进化反应的 Co@Ir 核壳纳米链气凝胶
IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-15 DOI: 10.1039/d4nj02733g
Jiacheng Chen, Zihao Xie, Yujun Tang, Zhenghua Tang, Xiufang Wang
Developing efficient and stable oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) catalysts is critical for realizing large-scale hydrogen production via electrochemical water splitting. Here, we report a facile one-step over-reduction method to fabricate IrCo aerogels as efficient and durable HER and OER catalysts. Multiple characterizations revealed that, IrCo aerogels possess a nano-chain-like structure composed of interconnected Co@Ir core-shell nanosphere particles. The as-prepared IrCo aerogels especially the Ir7Co3 sample showed excellent HER performance, evidenced by a small overpotential of 20.5 mV @10 mA·cm-2 and a low Tafel slope of 28.87 mV·dec-1 in 1.0 M KOH, which was significantly superior to the commercial Pt/C benchmark catalyst, and its OER performance is also better than the RuO2 benchmark, manifested by an overpotential of 269 mV @ 10 mA·cm-2 and a Tafel slope of 31 mV·dec-1. Moreover, in the overall water splitting (OWS) test, an applied voltage of 1.55 V was able to achieve a current density of 10 mA·cm-2. Furthermore, the Ir7Co3 sample demonstrated remarkable long-term stability and was able to function continuously in the HER, OER, and OWS processes, maintaining a negligible-changed current density of 10 mA·cm-2 for 35, 37, and 44 hours, respectively. Such superior electrocatalytic properties of the Ir7Co3 aerogel is mainly attributed to the alloying effect and the structural features, which can increase the exposed metal active sites, improve the electrical conductivity, facilitate the electron shuttling and mass transport during the electrocatalytic process. This study provides a facile and efficient generic approach for fabricating metallic aerogel toward HER, OER, OWS and beyond.
开发高效稳定的氧进化反应(OER)和氢进化反应(HER)催化剂对于通过电化学水分离实现大规模制氢至关重要。在此,我们报告了一种简单的一步过还原法来制备 IrCo 气凝胶,作为高效、持久的 HER 和 OER 催化剂。多种表征结果表明,IrCo 气凝胶具有由相互连接的 Co@Ir 核壳纳米颗粒组成的纳米链状结构。制备的 IrCo 气凝胶尤其是 Ir7Co3 样品表现出优异的 HER 性能,在 1.0 M KOH 中过电位为 20.5 mV @ 10 mA-cm-2,Tafel 斜率为 28.87 mV-dec-1,明显优于商用 Pt/C 基准催化剂;其 OER 性能也优于 RuO2 基准催化剂,过电位为 269 mV @ 10 mA-cm-2,Tafel 斜率为 31 mV-dec-1。此外,在整体水分裂(OWS)测试中,1.55 V 的外加电压能够达到 10 mA-cm-2 的电流密度。此外,Ir7Co3 样品还表现出显著的长期稳定性,能够在 HER、OER 和 OWS 过程中连续发挥作用,分别在 35、37 和 44 小时内保持 10 mA-cm-2 的电流密度,其变化可忽略不计。Ir7Co3 气凝胶之所以具有如此优异的电催化性能,主要归功于其合金化效应和结构特征,它们可以增加暴露的金属活性位点,提高导电性,促进电催化过程中的电子穿梭和质量传输。这项研究为制备金属气凝胶以实现 HER、OER、OWS 等目标提供了一种简便、高效的通用方法。
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