{"title":"金属有机框架中通过氮配位稳定的钙单原子作为高效固体碱催化剂。","authors":"","doi":"10.1016/j.jcis.2024.09.019","DOIUrl":null,"url":null,"abstract":"<div><p>Considerable attention has been paid to the preparation of single-atom solid base catalysts (SASBCs) owing to their high activity and maximized utilization of basic sites. At present, the reported fabrication methods of SASBCs, such as two-step reduction strategy and sublimation capture strategy, require high temperature. Such a high activation temperature is easy to cause the sublimation loss of alkali or alkaline earth metal atoms and destructive to the support structure. Herein, a new SASBC, Ca<sub>1</sub>/UiO-67-BPY, is fabricated, in which the alkaline earth metal Ca sites are immobilized onto N-rich metal–organic framework UiO-67-BPY at room temperature. The results show that the atomic configuration of Ca single atoms is coordinated by two N atoms in the framework. The obtained Ca SASBC possesses ordered structure and exhibits high product yield of 87.2% in the Knoevenagel reaction between benzaldehyde and malononitrile. Furthermore, thanks to the Ca single atoms sites anchored on UiO-67-BPY, the Ca<sub>1</sub>/UiO-67-BPY catalyst also shows good stability during cycles. This work might offer new insight in designing SASBCs for different base-catalyzed reactions.</p></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4000,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Calcium single atoms stabilized by nitrogen coordination in metal–organic frameworks as efficient solid base catalysts\",\"authors\":\"\",\"doi\":\"10.1016/j.jcis.2024.09.019\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Considerable attention has been paid to the preparation of single-atom solid base catalysts (SASBCs) owing to their high activity and maximized utilization of basic sites. At present, the reported fabrication methods of SASBCs, such as two-step reduction strategy and sublimation capture strategy, require high temperature. Such a high activation temperature is easy to cause the sublimation loss of alkali or alkaline earth metal atoms and destructive to the support structure. Herein, a new SASBC, Ca<sub>1</sub>/UiO-67-BPY, is fabricated, in which the alkaline earth metal Ca sites are immobilized onto N-rich metal–organic framework UiO-67-BPY at room temperature. The results show that the atomic configuration of Ca single atoms is coordinated by two N atoms in the framework. The obtained Ca SASBC possesses ordered structure and exhibits high product yield of 87.2% in the Knoevenagel reaction between benzaldehyde and malononitrile. Furthermore, thanks to the Ca single atoms sites anchored on UiO-67-BPY, the Ca<sub>1</sub>/UiO-67-BPY catalyst also shows good stability during cycles. This work might offer new insight in designing SASBCs for different base-catalyzed reactions.</p></div>\",\"PeriodicalId\":351,\"journal\":{\"name\":\"Journal of Colloid and Interface Science\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":9.4000,\"publicationDate\":\"2024-09-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Colloid and Interface Science\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021979724020770\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Colloid and Interface Science","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021979724020770","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
由于单原子固体基催化剂(SASBC)具有高活性并能最大限度地利用碱性位点,因此其制备受到了广泛关注。目前,已报道的 SASBC 制备方法,如两步还原策略和升华捕获策略,都需要较高的温度。如此高的活化温度容易造成碱金属或碱土金属原子的升华损失,并对支撑结构造成破坏。本文制备了一种新型 SASBC--Ca1/UiO-67-BPY,在室温下将碱土金属 Ca 位点固定在富 N 金属有机框架 UiO-67-BPY 上。结果表明,Ca 单原子的原子构型在框架中由两个 N 原子配位。所获得的 Ca SASBC 具有有序结构,在苯甲醛和丙二腈的 Knoevenagel 反应中表现出 87.2% 的高产率。此外,由于 Ca 单原子位点锚定在 UiO-67-BPY 上,Ca1/UiO-67-BPY 催化剂在循环过程中也表现出良好的稳定性。这项工作可能会为设计用于不同碱催化反应的 SASBC 提供新的见解。
Calcium single atoms stabilized by nitrogen coordination in metal–organic frameworks as efficient solid base catalysts
Considerable attention has been paid to the preparation of single-atom solid base catalysts (SASBCs) owing to their high activity and maximized utilization of basic sites. At present, the reported fabrication methods of SASBCs, such as two-step reduction strategy and sublimation capture strategy, require high temperature. Such a high activation temperature is easy to cause the sublimation loss of alkali or alkaline earth metal atoms and destructive to the support structure. Herein, a new SASBC, Ca1/UiO-67-BPY, is fabricated, in which the alkaline earth metal Ca sites are immobilized onto N-rich metal–organic framework UiO-67-BPY at room temperature. The results show that the atomic configuration of Ca single atoms is coordinated by two N atoms in the framework. The obtained Ca SASBC possesses ordered structure and exhibits high product yield of 87.2% in the Knoevenagel reaction between benzaldehyde and malononitrile. Furthermore, thanks to the Ca single atoms sites anchored on UiO-67-BPY, the Ca1/UiO-67-BPY catalyst also shows good stability during cycles. This work might offer new insight in designing SASBCs for different base-catalyzed reactions.
期刊介绍:
The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality.
Emphasis:
The journal emphasizes fundamental scientific innovation within the following categories:
A.Colloidal Materials and Nanomaterials
B.Soft Colloidal and Self-Assembly Systems
C.Adsorption, Catalysis, and Electrochemistry
D.Interfacial Processes, Capillarity, and Wetting
E.Biomaterials and Nanomedicine
F.Energy Conversion and Storage, and Environmental Technologies