{"title":"通过自发交联制备碳支撑 Al2O3 纳米粒子,以提高糠醛的选择性氢化能力","authors":"Weiwei Yu, Xinbao Zhang, Hongyu Chen, Yanan Wang, Shaoguo Li, Fucun Chen, Zhenni Liu, Xiujie Li, Xiangxue Zhu","doi":"10.1016/j.jechem.2024.08.059","DOIUrl":null,"url":null,"abstract":"<div><div>Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C<img>C over C<img>O. Herein, a novel Al<sub>2</sub>O<sub>3</sub>/C-u hybrid catalyst, composed of N-modified dendritic carbon networks supporting Al<sub>2</sub>O<sub>3</sub> nanoparticles, was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate, Al<sup>3+</sup> and urea<sub>.</sub> The obtained carbon-supported Al<sub>2</sub>O<sub>3</sub> hybrid catalyst has a high ratio (31%) of Al species in pentahedral-coordinated state. The introduction of urea enhances the surface N content, the ratio of pyrrolic N, and specific surface area of catalyst, leading to improved adsorption capacity of C<img>O and the accessibility of active sites. In the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor, Al<sub>2</sub>O<sub>3</sub>/C-u catalyst achieved a 90% conversion of furfural with 98.0% selectivity to furfuryl alcohol, outperforming that of commercial γ-Al<sub>2</sub>O<sub>3</sub>. Moreover, Al<sub>2</sub>O<sub>3</sub>/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on Al<sub>2</sub>O<sub>3</sub> nanoparticles. This work provides an innovative and facile strategy for fabrication of carbon-supported Al<sub>2</sub>O<sub>3</sub> hybrid catalysts with rich Al<sup>V</sup> species, serving as a high selective hydrogenation catalyst through MPV reaction route.</div></div>","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":null,"pages":null},"PeriodicalIF":4.1000,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Fabrication of carbon-supported Al2O3 nanoparticles via spontaneous cross-linking to enhance selective hydrogenation of furfural\",\"authors\":\"Weiwei Yu, Xinbao Zhang, Hongyu Chen, Yanan Wang, Shaoguo Li, Fucun Chen, Zhenni Liu, Xiujie Li, Xiangxue Zhu\",\"doi\":\"10.1016/j.jechem.2024.08.059\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C<img>C over C<img>O. Herein, a novel Al<sub>2</sub>O<sub>3</sub>/C-u hybrid catalyst, composed of N-modified dendritic carbon networks supporting Al<sub>2</sub>O<sub>3</sub> nanoparticles, was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate, Al<sup>3+</sup> and urea<sub>.</sub> The obtained carbon-supported Al<sub>2</sub>O<sub>3</sub> hybrid catalyst has a high ratio (31%) of Al species in pentahedral-coordinated state. The introduction of urea enhances the surface N content, the ratio of pyrrolic N, and specific surface area of catalyst, leading to improved adsorption capacity of C<img>O and the accessibility of active sites. In the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor, Al<sub>2</sub>O<sub>3</sub>/C-u catalyst achieved a 90% conversion of furfural with 98.0% selectivity to furfuryl alcohol, outperforming that of commercial γ-Al<sub>2</sub>O<sub>3</sub>. Moreover, Al<sub>2</sub>O<sub>3</sub>/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on Al<sub>2</sub>O<sub>3</sub> nanoparticles. This work provides an innovative and facile strategy for fabrication of carbon-supported Al<sub>2</sub>O<sub>3</sub> hybrid catalysts with rich Al<sup>V</sup> species, serving as a high selective hydrogenation catalyst through MPV reaction route.</div></div>\",\"PeriodicalId\":13,\"journal\":{\"name\":\"ACS Chemical Neuroscience\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.1000,\"publicationDate\":\"2024-09-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Chemical Neuroscience\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2095495624006156\",\"RegionNum\":3,\"RegionCategory\":\"医学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"BIOCHEMISTRY & MOLECULAR BIOLOGY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Chemical Neuroscience","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2095495624006156","RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"BIOCHEMISTRY & MOLECULAR BIOLOGY","Score":null,"Total":0}
引用次数: 0
摘要
由于热力学上 CC 比 CO 优先加氢,因此将糠醛选择性加氢为糠醇是加氢领域的一大挑战。本文通过对海藻酸盐、Al3+ 和尿素自发交联的冻干凝胶进行碳化,成功制备了一种新型 Al2O3/C-u 混合催化剂,该催化剂由支撑 Al2O3 纳米颗粒的 N 改性树枝状碳网络组成。所获得的碳支撑 Al2O3 混合催化剂中,五面体配位状态的 Al 种类比例较高(31%)。尿素的引入提高了催化剂的表面 N 含量、吡咯烷 N 比例和比表面积,从而提高了 CO 的吸附能力和活性位点的可及性。在以异丙醇为供氢体的糠醛加氢反应中,Al2O3/C-u 催化剂的糠醛转化率达到 90%,对糠醇的选择性达到 98.0%,优于商用 γ-Al2O3 催化剂。此外,Al2O3/C-u 在循环测试中表现出优异的催化稳定性,这归功于丰富的弱路易斯酸位点和碳网络对 Al2O3 纳米颗粒的锚定作用的协同效应。这项工作为制备富含 AlV 物种的碳支撑 Al2O3 混合催化剂提供了一种创新而简便的策略,可通过 MPV 反应路线用作高选择性加氢催化剂。
Fabrication of carbon-supported Al2O3 nanoparticles via spontaneous cross-linking to enhance selective hydrogenation of furfural
Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of CC over CO. Herein, a novel Al2O3/C-u hybrid catalyst, composed of N-modified dendritic carbon networks supporting Al2O3 nanoparticles, was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate, Al3+ and urea. The obtained carbon-supported Al2O3 hybrid catalyst has a high ratio (31%) of Al species in pentahedral-coordinated state. The introduction of urea enhances the surface N content, the ratio of pyrrolic N, and specific surface area of catalyst, leading to improved adsorption capacity of CO and the accessibility of active sites. In the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor, Al2O3/C-u catalyst achieved a 90% conversion of furfural with 98.0% selectivity to furfuryl alcohol, outperforming that of commercial γ-Al2O3. Moreover, Al2O3/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on Al2O3 nanoparticles. This work provides an innovative and facile strategy for fabrication of carbon-supported Al2O3 hybrid catalysts with rich AlV species, serving as a high selective hydrogenation catalyst through MPV reaction route.
期刊介绍:
ACS Chemical Neuroscience publishes high-quality research articles and reviews that showcase chemical, quantitative biological, biophysical and bioengineering approaches to the understanding of the nervous system and to the development of new treatments for neurological disorders. Research in the journal focuses on aspects of chemical neurobiology and bio-neurochemistry such as the following:
Neurotransmitters and receptors
Neuropharmaceuticals and therapeutics
Neural development—Plasticity, and degeneration
Chemical, physical, and computational methods in neuroscience
Neuronal diseases—basis, detection, and treatment
Mechanism of aging, learning, memory and behavior
Pain and sensory processing
Neurotoxins
Neuroscience-inspired bioengineering
Development of methods in chemical neurobiology
Neuroimaging agents and technologies
Animal models for central nervous system diseases
Behavioral research