利用过醇化反应设计、合成和评估贵金属纳米粒子和原位分解碳支撑纳米粒子电催化剂

IF 7.2 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Chemistry of Materials Pub Date : 2024-10-19 DOI:10.1021/acs.chemmater.4c02091
Nikolaos Chalmpes, Iosif Tantis, Ahmed Wasel Alsmaeil, Athanasios B. Bourlinos, Emmanuel P. Giannelis
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引用次数: 0

摘要

我们首次报道了利用双酚反应在碳上合成金属纳米颗粒和支撑金属纳米颗粒的过程。具体而言,我们报告了使用氢化钠(NaH)作为相应金属盐前体的点火引发剂和还原剂合成贵金属纳米颗粒(Pt、Ag 和 Au)的情况。此外,我们还报告了通过添加蔗糖作为碳源一步原位合成碳支撑的铂纳米粒子。与传统的使用硼氢化钠(NaBH4)在溶液中合成的纳米粒子相比,超醇合成的纳米粒子呈现出椭圆形态,且结晶度更高。在作为电催化剂进行测试时,与传统合成的铂纳米粒子相比,超醇铂纳米粒子的比电化学活性表面积(ECSA)高出 2 倍以上,与可逆氢电极(RHE)相比,半波电位(E1/2)高出 0.94 V。此外,基于原位合成碳的电催化剂在装饰了超醇合成的铂纳米粒子后,其性能优于类似的、最先进的商用铂碳系统。例如,前者的 E1/2 值为 0.94 V,而商用 PtC 为 0.9 V。在碱性环境中进行的加速耐久性测试(ADT)还增加了另一项优势。经过 10,000 次循环后,超醇合成系统的 E1/2 降低幅度较小,降解程度也低于商用 PtC(10 mV,而商用 PtC 为 ∼30 mV)。本文所描述的工作是首次报道利用金属纳米粒子和支撑金属纳米粒子的超醇化反应进行合成。所得电催化剂的特性证明了这种新方法在材料合成方面的多功能性和前景,并为进一步研究电催化剂开辟了新的途径。
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Design, Synthesis, and Evaluation of Noble Metal Nanoparticles and In Situ-Decorated Carbon-Supported Nanoparticle Electrocatalysts Using Hypergolic Reactions
We report the first synthesis of metal nanoparticles and supported metal nanoparticles on carbon by using hypergolic reactions. Specifically, we report the synthesis of noble metal nanoparticles (Pt, Ag, and Au) using sodium hydride (NaH) as both an ignition trigger and a reducing agent for the corresponding metal salt precursors. In addition, we report the one-step, in situ synthesis of Pt nanoparticles supported on carbon by adding sucrose as the carbon source. The hypergolically synthesized nanoparticles display elliptical morphology and are more crystalline compared with those conventionally synthesized in solution using sodium borohydride (NaBH4). When tested as electrocatalysts, the hypergolic Pt nanoparticles exhibit more than 2 times higher specific electrochemical active surface area (ECSA) and a higher half-wave potential (E1/2) of 0.94 V vs the reversible hydrogen electrode (RHE) compared to the conventionally synthesized ones. In addition, the electrocatalyst based on the in situ synthesized carbon that was decorated with the Pt nanoparticles synthesized hypergolically outperforms an analogous, state of the art, commercial PtC system. For example, the former shows an attractive E1/2 (0.94 V) compared with 0.9 V for the commercial PtC. Accelerated durability tests (ADT) in an alkaline environment add another advantage. After 10 000 cycles, the hypergolically synthesized system shows a smaller reduction of E1/2 and less degradation compared to the commercial PtC (10 mV compared to ∼30 mV). The work described here represents the first reported synthesis using hypergolic reactions of metal nanoparticles as well as supported metal nanoparticles. The properties of the resulting electrocatalysts demonstrate the versatility and promise of the new approach in materials synthesis and open new avenues for further investigation as electrocatalysts.
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来源期刊
Chemistry of Materials
Chemistry of Materials 工程技术-材料科学:综合
CiteScore
14.10
自引率
5.80%
发文量
929
审稿时长
1.5 months
期刊介绍: The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.
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