在多功能二维Pt/Ni-Fe-MOF纳米片上实现了高效的光引发一锅合成苯并咪唑

IF 6 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2025-07-01 Epub Date: 2025-03-31 DOI:10.1016/j.jcat.2025.116119
Hurunqing Liu, Siyang Wu, Zhaohui Li
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引用次数: 0

摘要

成功制备了尺寸约为2 nm的Pt/Ni-Fe-MOF纳米片(NSs),并将其作为多功能催化剂用于邻苯二胺和醇在可见光下的一锅反应生成苯并咪唑。在苯甲醇/甲苯(v/v, 2/1)的混合溶剂中,通过调节反应介质和催化剂的组成来调节单个反应步骤,获得了4 wt% Pt/Ni-Fe-MOF NSs的最佳反应活性,2-苯基苯并咪唑的收率为92.0 %。与块状纳米粒子相比,在二维Pt/Ni-Fe-MOF纳米粒子上观察到的优越活性可归因于光生载流子的重组减少,因为它们的输运路径较短。这项研究首先证明,除了需要不同的催化位点外,可以调节一锅串联/级联反应中涉及的单个反应步骤,以实现有效的整个反应。通过对反应介质和多功能催化剂组分的调节,可以在一定程度上实现对单个反应步骤速率的调节。该研究也为利用二维MOF构建光引发单锅串联/级联反应的多功能催化剂提供了巨大的潜力。
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Enabling an efficient light initiated one-pot synthesis of benzimidazoles over multifunctional 2D Pt/Ni-Fe-MOF nanosheets
Pt/Ni-Fe-MOF nanosheets (NSs), with small sized Pt nanoparticles of ca. 2 nm deposited on 2D Ni-Fe-MOF NSs of ca. 5.5 nm, were successfully fabricated and was used as a multifunctional catalyst for one-pot reaction between o-phenylenediamines and alcohols to produce benzimidazoles under visible light. By modulation on the reaction medium and the composition of the catalyst to regulate the individual reaction step involved, an optimum activity was achieved over 4 wt% Pt/Ni-Fe-MOF NSs in a mixed solvent of benzyl alcohol/toluene (v/v, 2/1), which showed a superior yield of 92.0 % to 2-phenylbenzimidazole. In comparison with its bulk counterpart, the superior activity observed over 2D Pt/Ni-Fe-MOF NSs can be attributed to a reduced recombination of the photogenerated charge carriers due to their short transportation path. This study first demonstrated that in addition to the different catalytic sites required, the individual reaction step involved in a one-pot tandem/cascade reaction can be regulated to enable an efficient whole reaction. Such a regulation of the rate of the individual reaction step can, to a certain degree, be achieved by modulation on the reaction medium and the component of the multifunctional catalyst. This study also provides the great potential of using 2D MOF for the construction of multifunctional catalysts for light initiated one-pot tandem/cascade reaction.
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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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