Crystal-Phase-Dependent Catalytic Performance of FeOOH in Aminocarbonylation with CO2

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2025-08-28 DOI:10.1007/s10562-025-05157-8

Dalei Sun, Ying Huang, Hongyu Li, Guoliang Lu

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Abstract

Three FeOOH polymorphs (α-, β-, γ-) were synthesized and evaluated for n-butylamine carbonylation with CO₂. α-FeOOH exhibited relatively high catalytic performance (83.5% conversion, 99.7% selectivity at 160 ℃ under 5.0 MPa) with excellent recyclability. The comprehensive characterization, such as XRD, BET, XPS, EPR, and TG-DSC/ESC, reveals that the catalytic activity is strongly correlated with two key factors: (1) surface hydroxyl concentration and (2) oxygen vacancy density, which are coupled with a balanced Bronsted-Lewis acid-base pair distribution. The superior performance of the α-phase stems from the synergistic effects of its oxygen-deficient surface (which enhances CO₂ activation) and the optimal distribution of acid-base sites (which stabilizes intermediates). This study establishes FeOOH polymorphs as potentially efficient catalysts for C-N coupling reactions and demonstrates that polymorph engineering is an effective strategy for CO₂ utilization.

Graphical Abstract

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FeOOH晶体相依赖性催化CO2氨基羰基化的性能

合成了3个FeOOH多晶体（α-, β-, γ-），并对其进行了CO2羰基化反应。α-FeOOH具有较高的催化性能（转化率83.5%，选择性99.7%,160℃，5.0 MPa）和优良的可回收性。XRD、BET、XPS、EPR和TG-DSC/ESC等综合表征表明，催化剂的催化活性与两个关键因素密切相关：(1)表面羟基浓度和(2)氧空位密度，并伴有平衡的Bronsted-Lewis酸碱对分布。α-相的优异性能源于其缺氧表面的协同作用（增强CO2活化）和酸碱位点的优化分布（稳定中间体）。本研究确立了FeOOH多晶型作为C-N偶联反应的潜在高效催化剂，并证明了多晶型工程是CO2利用的有效策略。图形抽象

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.