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NHC-Ligated gold nanoparticles derived from cluster precursors for carbon monoxide oxidation reactions
IF 4 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2025-03-24 DOI: 10.1039/d5dt00601e
Xiao-Ke Feng, Ren Chen, Pei-Qiong Chen, Guan-Di Wang, Peng-Chao Ren, Xiang-Kun Guo, Yujing Weng, Xi-Yan Dong
Trinuclear gold clusters functionalized with N-heterocyclic carbene (NHC) ligands were thermally decomposed to form NHC-stabilized gold nanoparticles. By systematically adjusting the substituents and electronic structures of the N-heterocyclic carbenes, the size and Auδ- active sites of the resulting gold nanoparticles was controlled, thereby modulating their catalytic performance in the conversion of CO to CO2 at the minimum temperature of 50 oC with an excellent efficiency.
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引用次数: 0
Relativistic Effect behind the Molybdenum vs. Tungsten Selectivity in Enzymes
IF 4 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2025-03-24 DOI: 10.1039/d5dt00001g
Udita Das, Ankita Das, Asim Kumar Das
: Molybdenum and tungsten being congeners of the 6th group of d-bock elements are similar in many respects in terms of their properties and in fact, both the molybdoenzymes and tungstoenzymes participate in similar type oxotransferase activity in their enzymes. Molybdenum is found as the heaviest essential trace metal in all forms of life but its next heavier congener, tungsten, as the heaviest metal is found only in some prokaryotic organisms. The tungstoenzymes are generally selected by nature for carrying out the low potential redox activities under the anaerobic conditions in the prokaryotic organisms. This nature’s molybdenum vs. tungsten selectivity for their biological functions under different working conditions (surrounding temperature and aerobic/anaerobic environment) is determined mainly by the relativistic effect which is experienced in different extents by these two congeners. Understanding the mechanistic aspects of the relativistic effect controlled enzymatic activities of the tungstoenzymes is of an immense biotechnological interest to develop the eco-friendly and cost effective methods of commercial synthesis of acetaldehyde through hydration of acetylene, and commercial production of hydrogen (H2, a green fuel) by producing the tungsten incorporated nitrogenase (W-N2-ase) in CA6 (mutant strain), and to develop a biomimetic method to replace the hazardous Birch reduction in organic synthesis, etc.
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引用次数: 0
Regioselective Oxidative Bromination of Arenes by Metal-Organic Framework Confined Mono-Bipyridyl Iron(III) Catalyst
IF 4 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2025-03-24 DOI: 10.1039/d5dt00443h
Rahul Kalita, Aditya Kumar, Poorvi Gupta, Bharti Rana, Bitan Sardar, Manav Chauhan, Biplab Ghosh, Yukti Monga, Kuntal Manna
Oxidative bromination of arenes is an effective and environmentally friendly method for synthesizing bromoarenes. We have developed a highly robust zirconium-metal-organic framework (MOF)-supported mono bipyridyl-iron(III) chloride catalyst (bpy-UiO-FeCl3) for oxidative bromination of arenes using H2O2 as the oxidant and KBr as the bromine source. The bpy-UiO-FeCl3 catalyst exhibits high conversion rates for various substituted arenes, yielding significant amounts of bromoarenes with excellent regioselectivity, and recyclability under mild reaction conditions. The MOF-catalyst outperforms its homogeneous counterparts in terms of both activity and regioselectivity due to the stabilization of the mononuclear bipyridyl-iron(III) species within the active sites in the MOF's pores. Furthermore, the confinement of these active sites within the robust, well-defined, and uniform porous framework enhances the regioselectivity of the bromination through shape-selective catalysis. The mechanism of bpy-UiO-FeCl3 catalyzed oxidative bromination of arenes was thoroughly investigated by a combination of control experiments, spectroscopic analyses, and computational studies. These findings underscore the importance of MOFs in the development of heterogeneous catalysts based on earth-abundant metals for the sustainable synthesis of haloarenes.
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引用次数: 0
Main group element compounds in materials and catalysis
IF 3.5 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2025-03-24 DOI: 10.1039/D5DT90053K
Selvarajan Nagendran, Ramaswamy Murugavel and Eric Rivard

A graphical abstract is available for this content

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引用次数: 0
Straightforward encapsulation of ultrastable CsPbBr3 PQDs and rare-earth emitters in zeolite for ratiometric temperature sensing and wet fingerprint recognition
IF 4 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2025-03-21 DOI: 10.1039/d5dt00368g
Zhou Yuan, Yuchi Zhang, Le Han, Yan Xu
All-inorganic metal halide perovskite quantum dots (PQDs) hybrids with high stability, multi-model emission and responsive luminescence are of great importance for optical applications. Herein, a dual-emitting CsPbBr3/Si-1:Eu3+ composite was successfully prepared by simultaneous encapsulation of CsPbBr3 PQDs and EuBr3 through a one-step thermal diffusion method. The partial destruction of five-membered rings in Silicalite-1 (Si-1) zeolite resulted from the PbBr2 etching effect at high temperatures enhances the bonding formation between Eu3+ and Si-OH, leading to the grafting of Eu3+ onto Si-1 zeolite framework. The strongly confined CsPbBr3 PQDs in CsPbBr3/Si-1:Eu3+ exhibit ultrastable green-emission over 30 days of soaking in water. Particularly, the CsPbBr3 PQDs and red-light Eu3+ emission center display distinct thermal quenching behaviors at elevated temperatures. So the CsPbBr3/Si-1:Eu3+ composite can serve as an effective ratiometric thermometer using the fluorescence intensity ratio (FIR) technique, showing a high sensitivity of 3.4 % ℃-1 at 54 ℃ and a temperature resolution of less than 0.2 ℃ in the range of 20-100 ℃. The water-stable CsPbBr3/Si-1:Eu3+ composite is also suitable for wet fingerprint recognition. This work introduces a straightforward method for preparing dual-emissive CsPbBr3/Si-1: Eu3+ composite for multimodal applications.
全无机金属卤化物包光体量子点(PQDs)具有高稳定性、多模式发射和响应发光等特性,在光学应用中具有重要意义。本文通过一步热扩散法同时封装 CsPbBr3 PQDs 和 EuBr3,成功制备了 CsPbBr3/Si-1:Eu3+ 双发射复合材料。在高温下,PbBr2 的蚀刻作用导致硅胶-1(Si-1)沸石中的五元环部分破坏,增强了 Eu3+ 与 Si-OH 之间的成键作用,从而使 Eu3+ 接枝到 Si-1 沸石框架上。在 CsPbBr3/Si-1:Eu3+ 中强致密的 CsPbBr3 PQDs 在水中浸泡 30 天后显示出超稳定的绿色发射。特别是在高温条件下,CsPbBr3 PQDs 和红光 Eu3+ 发射中心显示出不同的热淬行为。因此,CsPbBr3/Si-1:Eu3+ 复合材料可以利用荧光强度比(FIR)技术作为一种有效的比率温度计,在 54 ℃ 时的灵敏度高达 3.4 % ℃-1,在 20-100 ℃ 范围内的温度分辨率小于 0.2 ℃。水稳定性 CsPbBr3/Si-1:Eu3+ 复合材料也适用于湿指纹识别。这项工作介绍了一种制备双发射 CsPbBr3/Si-1: Eu3+ 复合材料的简单方法,可用于多模态应用。
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引用次数: 0
Controllable distribution of surface modified MIL-53 with ruthenium nanoparticles on nickel foam and its high efficiency electrocatalytic hydrogen evolution
IF 4 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2025-03-21 DOI: 10.1039/d5dt00287g
Yuhang Wang, Gui-Xin Yang, Chao Wang, Hongtao Liu, Xinming Wang, Haijun Pang
In the development of electrocatalysts that are cost-effective and highly functional, central to this endeavor is the synthesis of materials and the meticulous delineation of their morphology. This article introduces a solvent-thermal method for constructing ruthenium-based electrocatalysts (Ru/MIL-53@NF), distinguished by the in situ generation of ruthenium nanoparticles (NPs) on MIL-53 with notable dispersion. The procedure requires precise control over ruthenium integration, resulting in electrocatalysts with exceptional dispersion properties. Furthermore, the optimally engineered Ru/MIL-53@NF exhibited outstanding electrocatalytic hydrogen evolution performance, registering an overpotential of merely 17 mV at 10 mA·cm-2 and a Tafel slope of 53.7 mV·dec-1, thus outstripping the standard 20 wt% Pt/C benchmark. This research highlights the careful calibration of synthetic parameters to forge ruthenium-based electrocatalysts with both high efficacy and stability.
在开发具有成本效益和高功能性的电催化剂的过程中,材料的合成及其形态的精细描绘是核心所在。本文介绍了一种构建钌基电催化剂(Ru/MIL-53@NF)的溶剂-热方法,其特点是在 MIL-53 上原位生成钌纳米粒子(NPs),且分散性极佳。该过程需要精确控制钌的整合,从而产生具有特殊分散特性的电催化剂。此外,经过优化设计的 Ru/MIL-53@NF 还表现出卓越的电催化氢气进化性能,在 10 mA-cm-2 条件下,过电位仅为 17 mV,Tafel 斜坡为 53.7 mV-dec-1,因此超过了标准的 20 wt% Pt/C 基准。这项研究突出表明,要锻造出高效、稳定的钌基电催化剂,必须仔细校准合成参数。
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引用次数: 0
Pt/SnO2/Sb2O4 nanoparticle catalyst embedded in Multi-walled carbon nanotubes as active material for electrochemical hydrogen storage inquiries
IF 4 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2025-03-21 DOI: 10.1039/d5dt00336a
Raziyeh Akbarzadeh
Hydrogen storage and safe transport are the most important issues for hydrogen energy applications. Hydrogen has the necessary potential to provide clean fuel for heating and transportation because its only product of this combustion is pure water. Hydrogen is identified as one of the most renewable energy sources by supplying an efficient storage method. The electrochemical method with high energy conversion efficiency, through absorbtion/desorbtion mechanisms, is considered an appropriate strategy to achieve hydrogen storage. Hence, we propose a hydrogen energy storage system based on efficient electrode materials and electrochemical method. Due to obtaining high efficiency hydrogen storage, the Pt/SnO2/Sb2O4 nanoparticle catalyst embedded in multi-walled carbon nanotubes (MWCNTs) is synthesized via a facile polyol method, as active material. The sample structure was characterized by different techniques to determine its crystal structure, surface morphology, elements and porosity. Further, the electrochemical hydrogen storage abilities and the specific capacitance values of the as-prepared nanocomposite were assessed in alkaline media by chronopotentiometry analysis. The XRD studies exhibit that the average crystallite size of the Pt/SnO2/Sb2O4 nanoparticle catalyst is estimated to be around 7.5 nm. Also, the BET measurement shows a specific surface area, pore volume and pore diameter of 137.89 m2g-1, 0.3379 cm3g-1 and 9.8 nm for Pt/SnO2/Sb2O4/MWCNTs nanocomposite, respectively. The electrochemical consequences indicate that the incorporation of Pt/SnO2/Sb2O4 nanoparticle catalyst with MWCNTs showed excellent cycle stability and a high degree of electrochemical reversibility as an optimistic active candidate for use in electrochemical hydrogen storage. The maximum discharge capacity of Pt/ SnO2/Sb2O4 /MWCNTs nanocomposite was obtained to be 3480 mAhg-1 after 12 cycles. The higher and excellent discharge capacity of nanocomposite can partially be ascribed to its higher porosity, large specific surface area and the small size of Pt/SnO2/Sb2O4 nanoparticle catalyst.
氢的储存和安全运输是氢能应用中最重要的问题。氢具有为供暖和运输提供清洁燃料的必要潜力,因为氢燃烧的唯一产物是纯水。通过提供高效的储存方法,氢被认为是最可再生的能源之一。通过吸收/解吸机制实现高能量转换效率的电化学方法被认为是实现氢储存的适当策略。因此,我们提出了一种基于高效电极材料和电化学方法的氢储能系统。为了获得高效储氢,我们通过简便的多元醇法合成了嵌入多壁碳纳米管(MWCNTs)的 Pt/SnO2/Sb2O4 纳米粒子催化剂作为活性材料。通过不同的技术对样品结构进行了表征,以确定其晶体结构、表面形貌、元素和孔隙率。此外,还通过计时电位分析法评估了制备的纳米复合材料在碱性介质中的电化学储氢能力和比电容值。XRD 研究表明,Pt/SnO2/Sb2O4 纳米粒子催化剂的平均结晶尺寸约为 7.5 纳米。此外,BET 测量显示,Pt/SnO2/Sb2O4/MWCNTs 纳米复合材料的比表面积、孔体积和孔直径分别为 137.89 m2g-1、0.3379 cm3g-1 和 9.8 nm。电化学结果表明,Pt/SnO2/Sb2O4 纳米颗粒催化剂与 MWCNTs 的结合显示出优异的循环稳定性和高度的电化学可逆性,是电化学储氢的理想活性候选材料。经过 12 次循环后,Pt/ SnO2/Sb2O4 /MWCNTs 纳米复合材料的最大放电容量达到 3480 mAhg-1。纳米复合材料较高且优异的放电容量部分归因于其较高的孔隙率、较大的比表面积和较小尺寸的 Pt/SnO2/Sb2O4 纳米颗粒催化剂。
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引用次数: 0
Metal Ion-Modulated Synthesis of γ-MnO2 Nanosheet for Catalytic Oxidative Degradation of Clomiprazole
IF 4 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2025-03-21 DOI: 10.1039/d5dt00058k
Jinlian Zhang, Yu Xie, Xinli Zhang, Yuanhong Zhong, Ming Sun, Lin Yu
Two-dimensional non-layered oxide nanosheets exhibit exceptional catalytic properties, offering significant potential for environmental applications. In this study, we report the development of a novel Fe-doped γ-MnO₂ material with a hierarchical microsphere morphology, achieved through a metal ion regulation strategy. Unlike conventional sea urchin-like γ-MnO₂, Fe doping induced a transformation to a two-dimensional non-layered structure composed of nanosheets, significantly increasing the specific surface area and exposing more active sites. The Fe-doped γ-MnO₂ catalysts were evaluated for the degradation of chlorimiprazole (CBZ), a persistent pollutant, using a sulfate radical-based advanced oxidation process. Among the synthesized catalysts, NF-0.25Fe exhibited superior performance, achieving 93% CBZ removal within 16 min under near-neutral conditions. This exceptional activity was attributed to the optimized morphology, higher low-valence Mn content, and enhanced surface-active oxygen species. Systematic investigations revealed that the catalyst dosage, PMS concentration, and pH critically influenced the catalytic efficiency. This work demonstrates the potential of metal ion modulation in tailoring the structural and catalytic properties of transition metal oxides. The insights gained here provide a robust foundation for designing advanced nanomaterials for environmental remediation and other catalytic applications.
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引用次数: 0
Dual Emissive Ytterbium (III) Complexes with π-Conjugated BODIPY-Bipyridine Ligands
IF 4 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2025-03-21 DOI: 10.1039/d5dt00354g
Priyangika P. Senevirathne, Hongshan He, Kraig Wheeler, Radu F Semeniuc
Four BODIPY-functionalized bipyridine ligands (B1, B2, B3 and B4) were synthesized for sensitizing the near-infrared emission of Yb (III) ions. In these ligands, a BODIPY moiety was conjugated to 2,2′-bipyridine through an acetylene spacer at its C2 position, whereas its C6 position was substituted by H (B1), iodine (B2), 4-carboxylphenylacetylene (B3) or 4-thiocyanophenylacetylene (B4). The ligands exhibit strong absorption in the visible region and readily form stable complexes with ytterbium (III) trishexafluoroacetylacetonate (hfac-) hydrate in dichloromethane. Single-crystal X-ray diffraction analysis for Yb-B2 showed that the BODIPY unit almost falls into the bipyridine plane with Yb (III) being coordinated by six O from hfac- and two N atoms from bipyridine. All complexes exhibit strong absorption between 530 and 570 nm and can sensitize the ytterbium (III) for its emission at 980 nm under the UV-VIS light illumination. Interestingly, the visible emission from the complex increased when excited at 375 nm, making the complexes dual emissive, which is due to the increased absorption of the complex at 375 nm and inefficient energy transfer from BODIPY moiety to the Yb(III) ion.
合成了四种 BODIPY 功能化双吡啶配体(B1、B2、B3 和 B4),用于敏化镱(III)离子的近红外发射。在这些配体中,BODIPY 分子通过其 C2 位上的乙炔间隔与 2,2′-联吡啶共轭,而其 C6 位则被 H(B1)、碘(B2)、4-羧基苯乙炔(B3)或 4-硫氰基苯乙炔(B4)取代。这些配体在可见光区域表现出强烈的吸收,并很容易在二氯甲烷中与三六氟乙酰丙酮酸镱(III)水合物(hfac-)形成稳定的配合物。Yb-B2 的单晶 X 射线衍射分析表明,BODIPY 单元几乎落在联吡啶平面上,镱(III)与 hfac- 中的六个 O 原子和联吡啶中的两个 N 原子配位。所有配合物在 530 和 570 纳米之间都有很强的吸收,在紫外-可见光的照射下,镱(III)能敏化镱(III),使其在 980 纳米处发射。有趣的是,当在 375 纳米波长处激发时,配合物的可见光发射增加,使配合物具有双重发射性,这是由于配合物在 375 纳米波长处的吸收增加,以及 BODIPY 分子向镱离子的能量转移效率较低。
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引用次数: 0
Correction: Dicopper(i) complexes of a binucleating, dianionic, naphthyridine bis(amide) ligand 更正:双核、二阴离子、萘啶双(酰胺)配体的二氯化铜(I)配合物
IF 3.5 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2025-03-21 DOI: 10.1039/D5DT90059J
Laurent Sévery, T. Alexander Wheeler, Amelie Nicolay, Simon J. Teat and T. Don Tilley

Correction for ‘Dicopper(I) complexes of a binucleating, dianionic, naphthyridine bis(amide) ligand’ by Laurent Sévery et al., Dalton Trans., 2025, https://doi.org/10.1039/d5dt00034c.

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引用次数: 0
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