An unexpected case of instability of metal nanoclusters

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-06-22 DOI:10.1016/j.jcat.2024.115618
Alexander S. Lisitsyn, Evgenii Y. Gerasimov, Nina I. Kuznetsova
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Abstract

It is known that Pt clusters on the surface of chlorinated alumina are highly stable against sintering in reducing or inert environments and easily disintegrate into single atoms upon heat treatments under O. However, this study reveals that partially oxidized nanoclusters tend to grow in size and reconstruct upon further annealing in an inert gas (conventionally prepared 0.25 ÷ 1 %Pt/γ-AlO-Cl samples). Even more surprisingly, the sintering takes place at rather mild conditions (He/Ar, 400–500 °C) but stops soon after it commences (within minutes). The lower the temperature of O-pretreatment (500 → 20 °C), the sharper the further drop in metal dispersion, and one to a few cycles of the consecutive treatments could be sufficient for the unique properties of Pt clusters to be lost. Possible reasons, contributing factors, and implications of the results for different catalytic systems are discussed.

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金属纳米团簇不稳定的意外情况
众所周知,氯化铝表面的铂团簇在还原或惰性环境中对烧结非常稳定,在 O 下进行热处理时很容易分解为单个原子。然而,本研究发现,部分氧化的纳米团簇在惰性气体中进一步退火后(传统制备的 0.25 ÷ 1 %Pt/γ-AlO-Cl 样品),其尺寸往往会增大并发生重构。更令人惊讶的是,烧结是在相当温和的条件下进行的(He/Ar,400-500 °C),但烧结开始后很快就停止了(几分钟内)。O 预处理的温度越低(500 → 20 °C),金属分散度进一步下降的幅度就越大,连续处理一到几个周期就足以使铂簇失去其独特的性质。本文讨论了这一结果的可能原因、促成因素和对不同催化体系的影响。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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