竞争协调构造的异质核Pt1-Fe1双单原子站点,用于选择性氧化合醇
Mingyue Zhao1, Mengnan Ma1, Fanyu Meng1
1State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao, 266580, China.
Angewandte Chemie (International ed. in English)
|November 3, 2025
概括
一种新方法可以创建用于选择性酒精氧化的双单原子催化剂 (DSAC). 这种HAP上的Pt-Fe催化剂表现出高效率和化物选择性,性能优于单原子催化剂.
科学领域:
- 不同质的催化剂.
- 材料科学 材料科学 材料科学
- 纳米技术纳米技术
背景情况:
- 双单原子催化剂 (DSAC) 提供高原子效率和协同效应.
- 在复杂反应中DSACs的精确合成和应用方面仍然存在挑战.
研究的目的:
- 为异核DSACs开发精确的合成方法.
- 研究一种新型DSAC在选择性醇氧化中的应用.
主要方法:
- 使用竞争性协调策略,制造-铁 (Pt-Fe) 双单原子催化剂,支持酸 (HAP).
- 催化剂结构的描述,包括原子分离和电子特性.
- 在醇氧化过程中催化性能的评估.
主要成果:
- 一个异质核的Pt1-Fe1/HAP催化剂在受控的原子分离 (~2.7 Å) 过程中成功合成.
- 轨道杂交诱导了Fe的旋转状态过渡,增强了O2的激活.
- Pt1-Fe1/HAP催化剂实现了92%的化物选择性和12,090.8h-1的周转频率,显著优于Pt1/HAP.
结论:
- 热力学驱动的竞争性协调策略对于构建高性能异质核DSAC是有效的.
- 在DSAC中设计的电子协同作用可以显著提高催化活性和选择性.
- 这种方法为工业应用中先进的催化剂设计提供了一个通用策略.
相关概念视频
Radical Oxidation of Allylic and Benzylic Alcohols
2.8K
Activated manganese(IV) oxide can selectively oxidize allylic and benzylic alcohols via a radical intermediate mechanism. Primary allylic alcohols are oxidized to aldehydes, while secondary allylic alcohols yield ketones. The redox reaction of potassium permanganate with an Mn(II) salt such as manganese sulfate (under either alkaline or acidic conditions), followed by thorough drying, yields the oxidizing agent: activated MnO2. While MnO2 is insoluble in the solvents used for the reaction, the...
2.8K
Oxidation of Alkenes: Syn Dihydroxylation with Osmium Tetraoxide
12.5K
Alkenes are converted to 1,2-diols or glycols through a process called dihydroxylation. It involves the addition of two hydroxyl groups across the double bond with two different stereochemical approaches, namely anti and syn. Dihydroxylation using osmium tetroxide progresses with syn stereochemistry.
12.5K
Reduction of Alkenes: Asymmetric Catalytic Hydrogenation
3.8K
Catalytic hydrogenation of alkenes is a transition-metal catalyzed reduction of the double bond using molecular hydrogen to give alkanes. The mode of hydrogen addition follows syn stereochemistry.
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
3.8K
Oxidation of Alcohols
15.6K
In this lesson, the oxidation of alcohols is discussed in depth. The various reagents used for oxidation of primary and secondary alcohols are detailed, and their mechanism of action is provided.
The process of oxidation in a chemical reaction is observed in any of the three forms:
The process of oxidation in a chemical reaction is observed in any of the three forms:
15.6K
Oxidation of Alkenes: Syn Dihydroxylation with Potassium Permanganate
16.3K
Alkenes can be dihydroxylated using potassium permanganate. The method encompasses the reaction of an alkene with a cold, dilute solution of potassium permanganate under basic conditions to form a cis-diol along with a brown precipitate of manganese dioxide.
16.3K
Alkynes to Aldehydes and Ketones: Hydroboration-Oxidation
20.6K
Introduction
One of the convenient methods for the preparation of aldehydes and ketones is via hydration of alkynes. Hydroboration-oxidation of alkynes is an indirect hydration reaction in which an alkyne is treated with borane followed by oxidation with alkaline peroxide to form an enol that rapidly converts into an aldehyde or a ketone. Terminal alkynes form aldehydes, whereas internal alkynes give ketones as the final product.
One of the convenient methods for the preparation of aldehydes and ketones is via hydration of alkynes. Hydroboration-oxidation of alkynes is an indirect hydration reaction in which an alkyne is treated with borane followed by oxidation with alkaline peroxide to form an enol that rapidly converts into an aldehyde or a ketone. Terminal alkynes form aldehydes, whereas internal alkynes give ketones as the final product.
20.6K


