Atomically Precise Silver Nanocluster Riveted by Uneven Charged Traps toward Enhancing Electrocatalytic Activity for the Oxygen Reduction Reaction.

IF 4.3 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Zhao-Di Wang,Wen-Yan Sun,Wen-Yan Li,Ya-Kun Lv,Ying-Ying Wang,Peng Peng
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Abstract

Metal nanoclusters (MNCs) possessed promising potentials for catalytic applications but were hindered by the intrinsic charge-carrier mobility and the exposure of active sites. To this point, our work developed the uneven charged traps strategy to realize the homogeneous dispersion and immobilization of atomically precise silver nanoclusters (Ag6) and obtained an Ag cluster-based oxygen reduction reaction (ORR) electrocatalyst with enhanced performance. As expected, the uneven charged traps derived by graphitized nitrogen-doped carbon (NDC) extended the effective catalytic active area, tuned the electrical environment, and facilitated the binding between ORR intermediates and the active sites. Compared with pure Ag6 nanoclusters, Ag6@NDC possessed nearly 160 times higher electrochemical surface area (ECSA) and dramatically decreased electrochemical impedance spectroscopy (EIS). In alkaline media, the overall catalytic performance of Ag6@NDC with only 3.64 wt % Ag was even superior to commercial 20 wt % Pt/C. This work not only offered a successful showcase to enhance the catalytic performance of atomically precise MNCs but also provided highly efficient alternatives for both electrocatalytic applications and mechanism studies.
不均匀电荷阱铆接原子精密银纳米团簇提高氧还原反应电催化活性。
金属纳米团簇(MNCs)具有良好的催化应用前景,但其固有的载流子迁移率和活性位点的暴露阻碍了其催化应用。为此,我们开发了不均匀带电陷阱策略,以实现原子精密银纳米团簇(Ag6)的均匀分散和固定化,并获得了性能增强的Ag团簇基氧还原反应(ORR)电催化剂。正如预期的那样,石墨化氮掺杂碳(NDC)产生的不均匀带电陷阱扩大了有效催化活性区域,调节了电环境,促进了ORR中间体与活性位点之间的结合。与纯Ag6纳米团簇相比,Ag6@NDC具有近160倍的电化学表面积(ECSA)和显著降低的电化学阻抗谱(EIS)。在碱性介质中,Ag6@NDC的整体催化性能仅为3.64 wt % Ag,甚至优于20 wt % Pt/C。这项工作不仅为提高原子精密MNCs的催化性能提供了成功的展示,而且为电催化应用和机理研究提供了高效的替代方案。
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来源期刊
Inorganic Chemistry
Inorganic Chemistry 化学-无机化学与核化学
CiteScore
7.60
自引率
13.00%
发文量
1960
审稿时长
1.9 months
期刊介绍: Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.
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