Constructing single-atom Rh sites for selective hydroformylation of 1,3-butadiene to adipic aldehyde

IF 13.3 1区工程技术 Q1 ENGINEERING, CHEMICAL

Chemical Engineering Journal Pub Date : 2025-01-23 DOI:10.1016/j.cej.2025.159698

Zhaozhan Wang, Zihao Yang, Yifan Liu, Shingo Hasegawa, Ken Motokura, Shaoping Kuang, Yong Yang

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Abstract

To solve the difficulty and high cost in catalyst separation and recovery in the hydroformylation reaction is an ultimate goal from both academia and industry. In this study, we develop a recyclable single-atom Rh catalyst for the challenging hydroformylation of 1,3-butadiene. A unique bidentate phosphite-containing porous organic polymer with large surface area and hierarchical pores was rationally designed and synthesized for dispersing and stabilizing Rh species. Comprehensive characterizations reveal the atomic distribution of Rh species on the polymer surface via coordination with P donors. As a result, the single-atom Rh catalyst exhibits catalytic activity comparable to its homogeneous analogue, achieving complete conversion with selectivity to adipic aldehyde of up to 49.7 %. Remarkably, the single-atom Rh catalyst could be easily separated from the reaction mixture for successive reuses without significant decay in both activity and selectivity. This work represents an advancement towards the rational design of a heterogeneous Rh catalyst for 1,3-butadiene hydroformylation.

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构建1,3-丁二烯选择性氢甲酰化制己二醛的单原子Rh位点

解决氢甲酰化反应中催化剂分离和回收困难且成本高的问题是学术界和工业界的终极目标。在这项研究中，我们开发了一种可回收的单原子Rh催化剂，用于1,3-丁二烯的氢甲酰化。合理设计合成了一种独特的具有大表面积和分层孔结构的双齿状含亚磷酸盐多孔有机聚合物，用于分散和稳定Rh。通过与P给体的配位，揭示了Rh在聚合物表面的原子分布。结果表明，单原子Rh催化剂表现出与其均相类似物相当的催化活性，实现了对己二醛的完全转化，选择性高达49.7%。值得注意的是，单原子Rh催化剂可以很容易地从反应混合物中分离出来，以便连续重复使用，而活性和选择性都没有明显的衰减。这项工作代表了对1,3-丁二烯氢甲酰化的异相Rh催化剂的合理设计的进步。

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来源期刊

Chemical Engineering Journal 工程技术-工程：化工

CiteScore

21.70

自引率

9.30%

发文量

6781

审稿时长

2.4 months

期刊介绍： The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.