C60 富勒烯诱导的金属离子还原:具有高电催化氢气进化性能的 C60-金属簇异质结构的合成。

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Wenhao Yang, Qi Huang, Yingying Yan, Yaozhou Li, Tingting Xu, Ao Yu, Yihang Zhao, Ping Peng, Ying Wang, Luis Echegoyen, Fang-Fang Li
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引用次数: 0

摘要

金属簇由于尺寸小,表面原子比例高,因此与块状金属簇和纳米颗粒相比,催化活性显著提高。缺陷碳和改性碳支持物能有效稳定金属簇,然而,孤立金属簇的合成仍然需要多个步骤和苛刻的条件。在此,我们开发了一种 C60 富勒烯驱动的自发金属沉积工艺,其中 C60 既是还原剂又是锚,无需在 C60 上添加任何缺陷或官能团,即可获得均匀的金属(Rh、Ir、Pt、Pd、Au 和 Ru)团簇。密度泛函理论计算显示,C60 具有多个强金属吸附位点,这有利于金属原子的稳定和均匀沉积。此外,由于 C60 的吸电子特性,金属团簇的电子结构得到了有效调节,不仅优化了反应中间产物的吸附行为,还加速了氢进化反应的动力学过程。合成的 Ru/C60-300 在碱性条件下的氢气进化中表现出卓越的性能。本研究展示了一种简便高效的方法,无需任何预处理和额外的还原剂即可合成有效的富勒烯支撑金属簇催化剂。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

C60 Fullerene-Induced Reduction of Metal Ions: Synthesis of C60-Metal Cluster Heterostructures with High Electrocatalytic Hydrogen-Evolution Performance

C60 Fullerene-Induced Reduction of Metal Ions: Synthesis of C60-Metal Cluster Heterostructures with High Electrocatalytic Hydrogen-Evolution Performance

Metal clusters, due to their small dimensions, contain a high proportion of surface atoms, thus possessing a significantly improved catalytic activity compared with their bulk counterparts and nanoparticles. Defective and modified carbon supports are effective in stabilizing metal clusters, however, the synthesis of isolated metal clusters still requires multiple steps and harsh conditions. Herein, we develop a C60 fullerene-driven spontaneous metal deposition process, where C60 serves as both a reductant and an anchor, to achieve uniform metal (Rh, Ir, Pt, Pd, Au and Ru) clusters without the need for any defects or functional groups on C60. Density functional theory calculations reveal that C60 possesses multiple strong metal adsorption sites, which favors stable and uniform deposition of metal atoms. In addition, owing to the electron-withdrawing properties of C60, the electronic structures of metal clusters are effectively regulated, not only optimizing the adsorption behavior of reaction intermediates but also accelerating the kinetics of hydrogen evolution reaction. The synthesized Ru/C60-300 exhibits remarkable performance for hydrogen evolution in an alkaline condition. This study demonstrates a facile and efficient method for synthesizing effective fullerene-supported metal cluster catalysts without any pretreatment and additional reducing agent.

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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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