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Rice Straw Biochar as an Effective Support for Pd Nanoparticles for Ethanol Electro-Oxidation Reaction in Alkaline Condition 稻草生物炭作为钯纳米颗粒在烷烃条件下乙醇电氧化反应中的有效支持物
IF 2.6 4区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-10 DOI: 10.1002/cnma.202400288
Matthew L. Villanueva, Justienne Rei P. Laxamana, Hannah Grace G. Necesito, Jonyl L. Garcia, Prof. Bernard John V. Tongol

Herein, we report the utilization of biochar derived from rice straw (RSB) as an effective support matrix for Pd nanoparticles and its application as an electrocatalyst for ethanol electro-oxidation (EEO) in an alkaline medium. Rice straw, a common agricultural byproduct, was pyrolyzed at 600 °C, 700 °C, and 800 °C under N2 atmosphere. Pd was loaded onto the RSB via borohydride reduction of Pd2+, with a nominal loading of 20 % Pd. Spectroscopic and morphological characterization revealed the formation of dispersed Pd nanoparticles on the RSB surface. Pyrolysis temperature was observed to influence both the porosity of the resulting RSB and the dispersion and degree of exposure of Pd nanoparticles deposited on the surface. Electrochemical characterization revealed that Pd/RSB could be a potential EEO electrocatalyst for direct ethanol fuel cell applications. Pd/RSB-700 exhibited better performance in terms of EEO forward mass activity (jf) and forward and backward mass activity (jf/jb) ratio relative to Pd/RSB-600 and Pd/RSB-800. Moreover, Pd/RSB was shown to be superior to commercial Pd on carbon black in terms of electrochemical stability. This study opens the potential of rice straw biochar as a sustainable and environmentally friendly carbon-based support matrix for Pd-based EEO electrocatalysts.

在此,我们报告了如何利用从稻草(RSB)中提取的生物炭作为钯纳米粒子的有效支撑基质,并将其用作碱性介质中乙醇电氧化(EEO)的电催化剂。稻草是一种常见的农副产品,在 600 ℃、700 ℃ 和 800 ℃ 的氮气环境下进行热解。钯通过硼氢化还原 Pd2+ 被负载到 RSB 上,钯的名义负载量为 20%。光谱和形态表征显示,在 RSB 表面形成了分散的 Pd 纳米颗粒。据观察,热解温度既影响所得 RSB 的孔隙率,也影响沉积在表面的 Pd 纳米粒子的分散性和暴露程度。电化学特性分析表明,Pd/RSB 可作为一种潜在的 EEO 电催化剂直接用于乙醇燃料电池。与 Pd/RSB-600 和 Pd/RSB-800 相比,Pd/RSB-700 在 EEO 正向质量活性(jf)和正反向质量活性(jf/jb)比方面表现出更好的性能。此外,就电化学稳定性而言,Pd/RSB 还优于炭黑上的商用钯。这项研究揭示了稻草生物炭作为钯基 EEO 电催化剂的可持续和环保型碳基支撑基质的潜力。
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引用次数: 0
Fabrication of ripple structured silicon carbide (SiC) films for nano‐grating and solar cell applications 制作用于纳米光栅和太阳能电池的波纹结构碳化硅 (SiC) 薄膜
IF 3.8 4区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-10 DOI: 10.1002/cnma.202400455
Gupta Divya, Kalpana Chhoker, Usha Rani, Amena Salim, Rahul Singhal, Vishal Sharma, Sanjeev Aggarwal
In the present study, we aim to investigate the self‐organization of unexplored silicon carbide (SiC) film surfaces under 30 keV oblique Ar+ ions irradiation and hence unprecedented tailoring of optical and electrical characteristics with view of their uses in solar cells, gratings and nano‐ to micro‐scale devices. The surface morphology mainly consisted of triangular shaped nanoparticles which evolves into nanoscale ripple structures with an alignment parallel to the projection of ion beam direction. For the first time, we have demonstrated the fabrication of highly‐ordered ripple patterns with wavelength in visible region over SiC films and applicable as nano‐gratings. The underlying mechanism relies on the structural rearrangement due to transition of film microstructure from amorphous to mixed phase (crystalline, nano‐crystalline and amorphous) and lowering of C=C and C‐C vibration modes by the heavier Si atoms. These nanostructured silicon carbide film shows unparalleled optical (energy gap decreases from 4.60±0.4 eV to 3.16±0.2 eV) & electrical characteristics (conductivity increases from 6.6x10‐11 to 1.12x10‐3 S/m with linear I‐V behavior). Thus, we propose that ripple structured SiC films with wide band gap, high refractive index and high electrical conductivity with ohmic behaviour are promising candidates for application as window layer in solar cells and opto‐electronics.
在本研究中,我们旨在研究碳化硅(SiC)薄膜表面在 30 keV Ar+ 离子斜向辐照下的自组织情况,从而对其光学和电学特性进行前所未有的定制,以期将其应用于太阳能电池、光栅和纳米到微米尺度的设备中。表面形态主要由三角形纳米颗粒组成,这些颗粒演变成纳米级波纹结构,其排列方向与离子束投射方向平行。我们首次展示了在碳化硅薄膜上制造出波长在可见光区域的高有序波纹图案,并将其用作纳米支架。其基本机理依赖于薄膜微观结构从非晶态向混合相(晶体、纳米晶体和非晶态)转变所导致的结构重排,以及较重硅原子对 C=C 和 C-C 振动模式的降低。这些纳米结构碳化硅薄膜显示出无与伦比的光学特性(能隙从 4.60±0.4 eV 减小到 3.16±0.2 eV)和电子特性(电导率从 6.6x10-11 增加到 1.12x10-3 S/m,具有线性 I-V 行为)。因此,我们认为具有宽带隙、高折射率和高电导率及欧姆特性的波纹结构碳化硅薄膜有望用作太阳能电池和光电元件的窗口层。
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引用次数: 0
Front Cover: Superhydrophilic Densely-Packed Gecko-Like Structures by Soft-Template Electropolymerization (ChemNanoMat 9/2024) 封面:通过软模板电聚合形成的超亲水致密壁虎状结构(ChemNanoMat 9/2024)
IF 2.6 4区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-09 DOI: 10.1002/cnma.202480901
Pape Diene Dione, Prof. Alioune Diouf, Dr. Abdoulaye Dramé, Dr. François Orange, Prof. Frédéric Guittard, Dr. Thierry Darmanin

Gecko-like structures have been prepared by soft-template electropolymerization in micellar solution. Various monomers were designed from a triphenylamine core but only one monomer gives such structures even if the monomer is not perfectly planar. Extremely long and densely packed-microtubes are obtained at constant potential. However, the surfaces are not both highly hydrophobic and with strong water adhesion as gecko foot but are superhydrophilic. These differences can be explained by a higher surface energy or difference in arrangement structures for our surfaces. More information can be found in the Research Article by Thierry Darmanin and co-workers.

通过在胶束溶液中进行软模板电聚合,制备出了壁虎状结构。以三苯胺为核心设计了多种单体,但只有一种单体能产生这种结构,即使该单体不是完全平面的。在恒定电位下,可获得极长且密集的微管。然而,这些表面并不像壁虎脚那样既高度疏水又有很强的水附着力,而是超亲水性的。这些差异可以用我们的表面具有更高的表面能或排列结构不同来解释。更多信息,请参阅 Thierry Darmanin 及其合作者的研究文章。
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引用次数: 0
The Influence of Halogen Anions on the Color/Fluorescence Dual-Switching Behaviors of 1,10-Phenanthroline-Based Viologen Derivatives 卤素阴离子对 1,10-菲罗啉基 Viologen 衍生物颜色/荧光双切换行为的影响
IF 2.6 4区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-09 DOI: 10.1002/cnma.202400418
Dr. Yanling Zhuang, Qidong Zhang, Xiaquan Lin

Stimuli-responsive color/fluorescence dual-switchable materials have garnered significant attention in displays, sensors, and anti-counterfeiting. However, current material systems are hampered by the single stimulus-response and unregulated fluorescence. Viologen derivatives featuring fluorophore as N-substituent and halogen anions as counteranions not only exhibit responsiveness to both electric and light stimuli but also enable adjustable emission. In this work, we explored the influence of halogen anions on the color/fluorescence dual-switching behaviors of 1,10-phenanthroline-based viologen derivatives. The energy level gaps for phen-Vio[2Cl] (2.93 eV), phen-Vio[2Br] (2.67 eV), and phen-Vio[2I] (2.34 eV) decreased with the decrease of electron affinity of halogen anions (Cl>Br>I), which leads to a sequential improvement in their electrochromic/electrofluorochromic and photochromic/photofluorochromic properties. This work has important guidance for the design and development of smart materials and their optoelectronic devices.

刺激响应式色彩/荧光双开关材料在显示器、传感器和防伪领域备受关注。然而,目前的材料系统受到单一刺激响应和不规则荧光的阻碍。以荧光团为 N 取代基、卤素阴离子为反阴离子的 Viologen 衍生物不仅能对电刺激和光刺激做出响应,还能实现可调节的发射。在这项工作中,我们探讨了卤素阴离子对 1,10-菲罗啉基紫罗兰衍生物的颜色/荧光双切换行为的影响。随着卤素阴离子(Cl- > Br- > I-)电子亲和力的减小,phen-Vio[2Cl-](2.93 eV)、phen-Vio[2Br-](2.67 eV)和phen-Vio[2I-](2.34 eV)的能级间隙也随之减小,从而使它们的电致变色/电致荧光变色和光致变色/光致荧光变色性能相继得到改善。这项工作对设计和开发智能材料及其光电器件具有重要指导意义。
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引用次数: 0
Polyoxometalate derived materials as laccase‐mimic nanozyme and reduction catalyst for p‐nitrophenol remediation in water 聚氧化金属酸盐衍生材料作为模仿漆酶的纳米酶和对硝基苯酚水污染修复还原催化剂
IF 3.8 4区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-09 DOI: 10.1002/cnma.202400336
Ping Sun, Xinxin Xu, Jin Chen
p‐Nitrophenol (PNP), a highly toxic water pollutant, poses significant risks to human health and the environment. For detecting PNP, a colorimetric method utilizing a nanozyme that mimics laccase activity presents a viable approach. In this study, PV14@MIL‐88A, a robust nanozyme with superior laccase‐mimic capabilities, was synthesized by incorporating Na7H2[PV14O42] (PV14) into MIL‐88A, a metal‐organic framework (MOF). This nanozyme demonstrates optimal laccase‐mimicking activity, enabling effective PNP detection via colorimetry and digital image colorimetry using smartphones. Theoretical analyses suggest that the outstanding laccase‐mimic activity of PV14@MIL‐88A is derived from the optimized d‐band center in PV14. Upon calcination with dicyandiamide (DCDA), PV14@MIL‐88A transforms into Fe2O3/VO2@NCNF. In the presence of NaBH4, Fe2O3/VO2@NCNF facilitates the conversion of PNP to p‐aminophenol (PAP), an essential precursor in paracetamol synthesis. The interaction between Fe2O3 and VO2 in Fe2O3/VO2@NCNF enhances adsorption and subsequent reduction of PNP. The saturation magnetization of Fe2O3/VO2@NCNF reaches 25 emu·g‐1, which supports efficient magnetic separation in the reduction process. This study not only advances an effective method for PNP detection but also facilitates its transformation from a hazardous pollutant into a valuable chemical precursor.
对硝基苯酚(PNP)是一种剧毒水污染物,对人类健康和环境构成重大风险。利用模仿漆酶活性的纳米酶比色法检测 PNP 是一种可行的方法。在本研究中,通过将 Na7H2[PV14O42] (PV14) 加入金属有机框架 (MOF) MIL-88A 中,合成了具有卓越漆酶模拟能力的 PV14@MIL-88A。这种纳米酶具有最佳的裂解酶模拟活性,可通过智能手机的比色法和数字图像比色法有效检测 PNP。理论分析表明,PV14@MIL-88A 杰出的长效酶模拟活性源自 PV14 中优化的 d 波段中心。用双氰胺(DCDA)煅烧后,PV14@MIL-88A 转化为 Fe2O3/VO2@NCNF。在 NaBH4 的存在下,Fe2O3/VO2@NCNF 可促进 PNP 向对氨基苯酚(PAP)的转化,对氨基苯酚是对乙酰氨基酚合成过程中必不可少的前体。Fe2O3/VO2@NCNF 中的 Fe2O3 和 VO2 之间的相互作用增强了对 PNP 的吸附和随后的还原。Fe2O3/VO2@NCNF 的饱和磁化率达到 25 emu-g-1,这为还原过程中的高效磁分离提供了支持。这项研究不仅推进了一种检测 PNP 的有效方法,还促进了 PNP 从一种有害污染物转变为一种有价值的化学前体。
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引用次数: 0
An Oxygen-Self-Produced Nanoplatform Based on MnO2 for Relieving Hypoxia 基于二氧化锰的自产氧纳米平台用于缓解缺氧症状
IF 2.6 4区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-08 DOI: 10.1002/cnma.202400157
Guohua Pan, Hanxiao Bao, Jinguo Zhang, Jue Hou, Jun Zhou, Hongzhen Bai, Guping Tang

Manganese dioxide (MnO2) nanoparticles are increasingly recognized for their potential in biomedical applications, particularly in the realm of hypoxic cancer therapy, due to their unique physicochemical characteristics. This investigation introduces a novel, template-free synthesis strategy. The reducing groups inherent in bovine serum albumin (BSA) facilitate a redox reaction with potassium permanganate (KMnO4), while the abundance of functional groups in BSA is instrumental in the formation of MnO2. The transmission electron microscopy (TEM) analysis has characterized the synthesized MnO2 nanoparticles, termed BM NPs, as spherical particles with a mean diameter of 210 nm and zeta potential of −40.1 mV measured by dynamic light scattering (DLS). The Fourier transform infrared (FT-IR) spectrum of BM NPs exhibits the characteristic peak of MnO2 at 1113 cm−1 and 620 cm−1. Furthermore, the elemental composition of BM NPs has been ascertained through energy-dispersive X-ray (EDX) elemental mapping analysis. Though concentration of BM NPs up to 200 μg/mL, the survival rate of 4T1 cells remained approximately 75 %. Given that BM NPs at a concentration of 100 μg/mL significantly alleviate cellular hypoxia, the high oxygen-generating capacity of these nanoparticles is proved, suggesting their suitability as a drug delivery system, especially in the context of hypoxic tumor microenvironments.

二氧化锰(MnO2)纳米粒子因其独特的物理化学特性,在生物医学应用,尤其是缺氧性癌症治疗领域的潜力日益得到认可。本研究介绍了一种新颖的无模板合成策略。牛血清白蛋白(BSA)中固有的还原基团促进了与高锰酸钾(KMnO4)的氧化还原反应,而 BSA 中丰富的官能团则有助于 MnO2 的形成。透射电子显微镜(TEM)分析表明,合成的 MnO2 纳米颗粒(称为 BM NPs)为球形颗粒,平均直径为 210 nm,动态光散射(DLS)测量的 Zeta 电位为 -40.1 mV。BM NPs 的傅立叶变换红外光谱(FT-IR)在 1113 cm-1 和 620 cm-1 处显示出 MnO2 的特征峰。此外,还通过能量色散 X 射线(EDX)元素图谱分析确定了 BM NPs 的元素组成。尽管 BM NPs 的浓度高达 200 微克/毫升,但 4T1 细胞的存活率仍保持在 75% 左右。鉴于浓度为100微克/毫升的BM NPs能显著缓解细胞缺氧,证明了这些纳米颗粒的高产氧能力,表明它们适合作为药物输送系统,尤其是在缺氧的肿瘤微环境中。
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引用次数: 0
Rifampicin-Loaded Nano-in-Microparticles (Trojan Particles) as a Pulmonary Delivery System for Tuberculosis Treatment 作为肺部给药系统治疗肺结核的利福平纳米微粒(特洛伊微粒
IF 2.6 4区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-07 DOI: 10.1002/cnma.202400296
Dinh-Duy Pham, Van-Thin Luong, Truc Thanh Ngoc Huynh, Duyen Thi My Huynh, Duy Toan Pham

The oral rifampicin (RIF) dosage forms possess various side effects and limited efficacy for tuberculosis treatment. Thus, this work developed the nano-in-microparticles containing RIF (trojan nRIF) as a novel pulmonary delivery system. The RIF-loaded nanoparticles (nRIF) were prepared by self-assembly polyelectrolyte complexation between lecithin and chitosan, whereas the trojan nRIF were formulated by spray-drying method of nRIF and mannitol/maltodextrin. The nRIF had a spherical shape with sizes of 86–126 nm, zeta potentials of 24–39 mV, entrapment efficiencies of 44–80 %, and drug loading capacities of 13–42 %. The RIF release from nRIF occurred in two stages, the initially rapid release stage and the controlled release stage upto 96 h, followed the Higuchi model. The trojan nRIF possessed the mass median aerodynamic diameter of 3.7–4.6 μm, fine particle fraction of 34–40 %, and alveolar fraction of 17–21 %. Compared to mannitol, maltodextrin was a superior carrier for nRIF, which yielded better aerodynamic properties and RIF was mainly stayed in the amorphous form. Moreover, using the scanning electron microscopy, the nano-in-microparticles were clearly observed with hollow structure. Finally, the trojan nRIF could preserve the physical properties of the encapsulated nRIF. In summary, the trojan nRIF could become a potential inhalation anti-tuberculosis product.

口服利福平(RIF)剂型具有各种副作用,对结核病的治疗效果有限。因此,本研究开发了含有 RIF 的纳米微粒(trojan nRIF),作为一种新型肺部给药系统。负载 RIF 的纳米颗粒(nRIF)是通过卵磷脂和壳聚糖的自组装聚电解质复合物制备的,而木马 nRIF 则是通过 nRIF 和甘露醇/麦芽糊精的喷雾干燥法制备的。nRIF 呈球形,大小为 86-126 nm,zeta 电位为 24-39 mV,夹带效率为 44-80%,载药量为 13-42%。按照樋口模型,RIF 从 nRIF 中的释放分为两个阶段,即最初的快速释放阶段和直到 96 小时的控制释放阶段。特洛伊nRIF的质量中值空气动力学直径为3.7-4.6微米,细颗粒部分占34-40%,肺泡部分占17-21%。与甘露醇相比,麦芽糊精是一种更好的 nRIF 载体,它具有更好的空气动力学特性,而且 RIF 主要以无定形形式存在。此外,利用扫描电子显微镜可以清楚地观察到纳米微粒具有中空结构。最后,特洛伊 nRIF 还能保持封装 nRIF 的物理特性。总之,特洛伊 nRIF 有可能成为一种潜在的吸入式抗结核产品。
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引用次数: 0
Molecular Aggregation to and from Disaggregation of an Organic Emitter for Strategic Emission Modulation 有机发射器的分子聚合与分解,实现战略性发射调制
IF 3.8 4区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-07 DOI: 10.1002/cnma.202400474
Arabinda Mallick, Provakar Paul, Saikat Samanta, Arunavo Chatterjee, Bibhas Mondal, Ujjal Kanti Roy, Tapas Majumdar
“Aggregation‐caused fluorescence quenching” is a well‐established phenomenon by now. The procedure from aggregation to disaggregation usually causes a revival of emission signals, and thus affords an interesting new path to design “turn‐on” optical probes. For this purpose, the photophysics, energetics and dynamics of supra‐molecular encapsulation induced disaggregation of a self‐assembled bis‐indole derivative, 3,3’‐bisindolyl(phenyl)methane (BIPM), and its further reaggregation are reported herein. Compared to disaggregation strategies, its reverse process, reaggregation, has received much less attention so far. The gamma‐cyclodextrin (γ‐CD) molecules were found to be effective in disaggregating the BIPM associations and emission enhancement, whereas, the incorporation of guanidine hydrochloride (Gnd‐HCl) into the aqueous solution of disaggregated BIPM monomers in γ‐CD environment resulted in probe reaggregation leading to quenching of the restored emission. Here, γ‐CD and Gnd‐HCl can be considered as the molecular modulators of BIPM fluorescence based on the disaggregation–reaggregation mechanisms. The spectroscopic and thermodynamic findings associated with the disaggregation‐reaggregation processes might be insightful in reversible controlling of molecular aggregation and the associated optical properties for diverse applications.
"聚集引起的荧光淬灭 "现已成为一种公认的现象。从聚集到分解的过程通常会导致发射信号的恢复,从而为设计 "开启 "光学探针提供了一条有趣的新途径。为此,本文报告了一种自组装双吲哚衍生物--3,3'-双吲哚基(苯基)甲烷(BIPM)的超分子封装诱导分解及其进一步再聚集的光物理、能量学和动力学。与分解策略相比,其逆向过程--再聚合迄今为止受到的关注要少得多。研究发现,γ-环糊精(γ-CD)分子能有效地分解 BIPM 团聚并增强发射,而在γ-CD 环境中,将盐酸胍(Gnd-HCl)加入分解的 BIPM 单体的水溶液中会导致探针重新聚集,从而淬灭恢复的发射。根据分解-重组机制,γ-CD 和 Gnd-HCl 可被视为 BIPM 荧光的分子调节剂。与解聚-重组过程相关的光谱学和热力学发现可能有助于可逆地控制分子的聚集和相关的光学特性,从而实现多种应用。
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引用次数: 0
Single Source Precursor Path to 2D Materials: A Case Study of Solution-Processed Molybdenum-Rich MoSe2-x Ultrathin Nanosheets 通向二维材料的单源前驱体之路:溶液加工富钼 MoSe2-x 超薄纳米片的案例研究
IF 2.6 4区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-06 DOI: 10.1002/cnma.202400357
Shashank Mishra, Erwann Jeanneau, Sweta Gahlot, Nidal Raydan, Laurence Burel, Thibault Cornier, Anne Bonhomme, Pascal Bargiela

Two-dimensional Molybdenum diselenide is a versatile and promising material used for a wide range of applications and its synthesis in high quality and yield is currently the subject of intense research. Low temperature solution phase synthesis of nanomaterials using designed molecular precursors enjoys tremendous advantages over traditional high-temperature solid-state synthesis. However, molecular precursor chemistry of molybdenum selenide nanomaterials is almost non-existent. We report here synthesis and structural characterization of new molybdenum molecular precursors with selenoether and selenourea ligands, which due to their easy synthesis, desired Mo/Se composition and moderate processing properties, are highly promising as single source precursors for the scale-up production of 2D molybdenum diselenide materials. This is demonstrated by the solution-phase decomposition of the Mo-selenourea precursor which produced Mo-rich MoSe2-x ultrathin nanosheets (NSs) in good yield. These NSs were characterized by Inductively Coupled Plasma Optical Emission Spectroscopy (ICP-OES), Powder X-ray diffraction (XRD), Raman spectroscopy, Fourier Transform Infrared Spectroscopy (FT-IR), Thermogravimetric analysis (TGA), Transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) studies.

二维二硒化钼是一种用途广泛、前景广阔的材料,高质量、高产量地合成二维二硒化钼是目前研究的热点。与传统的高温固态合成相比,利用设计的分子前驱体低温溶液相合成纳米材料具有巨大的优势。然而,硒化钼纳米材料的分子前驱体化学几乎不存在。我们在此报告了带有硒醚和硒脲配体的新型钼分子前驱体的合成和结构表征,由于它们易于合成、具有理想的钼/硒成分和适中的加工性能,因此极有希望作为单源前驱体用于二维二硒化钼材料的放大生产。通过对钼-硒脲前驱体进行溶液相分解,生产出了富钼的 MoSe2-x 超薄纳米片(NSs),并取得了良好的收率。通过电感耦合等离子体光学发射光谱 (ICP-OES)、粉末 X 射线衍射 (XRD)、拉曼光谱、傅立叶变换红外光谱 (FT-IR)、热重分析 (TGA)、透射电子显微镜 (TEM) 和 X 射线光电子能谱 (XPS) 研究对这些纳米片进行了表征。
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引用次数: 0
Bifunctional Electrocatalyst Enhanced Synergistically by MoS2/Ni3S2 Heterojunctions and Au Nanoparticles for Large-Current-Density Overall Water Splitting 通过 MoS2/Ni3S2 异质结和金纳米粒子协同增强的双功能电催化剂用于大电流密度整体水分离
IF 2.6 4区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-09-02 DOI: 10.1002/cnma.202400430
Peizhi Liu, Dechuan Peng, Bin Zhang, Bing Hao, Yongqing Shen, Yanhui Song, Haojie Liang, Min Zhao, Haixia Zhang, Bingshe Xu, Junjie Guo

Developing transition metal based overall water splitting (OWS) electrocatalysts with high efficiency, low-cost, large current density, and long-term stability is crucial for industrial electrolysis of water, but remains a major challenge. In this study, a hierarchical electrocatalyst with MoS2/Ni3S2 heterojunctions and a tiny amount of Au nanoparticles grown on nickel foam (MoS2/Ni3S2-Au@NF) has been developed by a one-step hydrothermal method. The heterojunctions and Au nanoparticle decoration induce the electron-rich interfaces in the catalyst, which facilitate the synergistic adsorption of both OER and HER intermediates. As a result, MoS2/Ni3S2-Au@NF possesses an excellent bifunctional electrocatalytic performance in 1 M KOH with low HER overpotential (78 mV@10 mA cm−2, 253 mV@500 mA cm−2), low OER overpotential (261 mV@50 mA cm−2, 435 mV@500 mA cm−2), and outstanding cyclical stability and continuous stability, which are superior than typical benchmarks of Pt/C and RuO2. An electrolyzer assembled with the self-supported MoS2/Ni3S2-Au@NF electrode also displays excellent OWS activity and stability with a current density beyond 100 mA cm−2. This experiment is responding a potential alternative non-precious metal electrocatalyst for OWS at industrial settings, and thus promotes the real-world application of hydrogen energy conversions.

开发高效、低成本、大电流密度和长期稳定的过渡金属基整体水分离(OWS)电催化剂对于工业电解水至关重要,但仍是一项重大挑战。本研究采用一步水热法开发了一种在泡沫镍上生长有 MoS2/Ni3S2 异质结和微量金纳米粒子的分层电催化剂(MoS2/Ni3S2-Au@NF)。异质结和金纳米粒子装饰在催化剂中形成了富电子界面,从而促进了 OER 和 HER 中间产物的协同吸附。因此,MoS2/Ni3S2-Au@NF 在 1M KOH 中具有优异的双功能电催化性能,具有较低的 HER 过电位(78 mV@10 mA cm-2,253 mV@500 mA cm-2)、较低的 OER 过电位(261 mV@50 mA cm-2,435 mV@500 mA cm-2),以及出色的周期稳定性和连续稳定性,优于 Pt/C 和 RuO2 的典型基准。使用自支撑 MoS2/Ni3S2-Au@NF 电极组装的电解槽在电流密度超过 100 mA cm-2 时也显示出卓越的 OWS 活性和稳定性。该实验为工业环境下的 OWS 提供了一种潜在的非贵金属电催化剂替代品,从而促进了氢能转换的实际应用。
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