通过氧气空隙介导的选择性C-N合以实现电催化尿素合成
Xiaoxiao Wei1,2, Xiaojian Wen2, Yingying Liu1
1State Key Laboratory of Chemo/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Advanced Catalytic Engineering Research Center of the Ministry of Education, Hunan University, Changsha, Hunan 410082, P. R. China.
Journal of the American Chemical Society
|June 24, 2022
概括
在二氧化 (CeO2) 中的氧气空位通过稳定关键中间体使得高效的,单阶段的电催化尿素合成成为可能. 这种方法提高了C-N合的选择性,为传统的尿素生产方法提供了有希望的替代方案.
科学领域:
- 电化学
- 材料科学
- 催化剂
背景情况:
- 传统的尿素合成是能源密集的,涉及多个步骤.
- 电催化C-N合为尿素生产提供了更可持续的替代方案.
- 介质化通常会限制电催化尿素合成的效率.
研究的目的:
- 在环境条件下开发一级尿素合成的高效电催化剂.
- 研究氧气空缺在增强C-N合选择性的作用.
- 提高电催化尿素生产的产量.
主要方法:
- 电催化
- 氧气空位丰富的二氧化 (CeO2) 的合成
- 现场总频率生成光谱用于机械研究
主要成果:
- 富含氧气空位的CeO2有效地稳定了关键的*NO中间体.
- 稳定中间体更喜欢C-N合而不是质子,增强选择性.
- 获得了943.6毫克h-1g-1的高尿素产率,超过了一些贵金属催化剂.
结论:
- 氧气空缺对于设计高效的尿素合成电催化剂至关重要.
- 具有量身定制的氧空位的CeO2为选择性C-N合提供了一条新途径.
- 这一战略促进了改善尿素生产系统的催化剂设计.
相关概念视频
Catalysis
27.5K
The presence of a catalyst affects the rate of a chemical reaction. A catalyst is a substance that can increase the reaction rate without being consumed during the process. A basic comprehension of a catalysts’ role during chemical reactions can be understood from the concept of reaction mechanisms and energy diagrams.
27.5K
Urea Cycle
45.7K
The urea cycle describes how liver cells convert ammonia to urea. Ammonia is a toxic waste product of protein catabolism. Land animals must convert ammonia into the less toxic urea which can be safely eliminated by the kidneys through urine. Marine animals excrete ammonia directly, and the surrounding water dilutes the ammonia to safe levels.
45.7K
Thermal and Photochemical Electrocyclic Reactions: Overview
2.4K
Electrocyclic reactions are reversible reactions. They involve an intramolecular cyclization or ring-opening of a conjugated polyene. Shown below are two examples of electrocyclic reactions. In the first reaction, the formation of the cyclic product is favored. In contrast, in the second reaction, ring-opening is favored due to the high ring strain associated with cyclobutene formation.
2.4K
Oxidative Cleavage of Alkenes: Ozonolysis
11.1K
In ozonolysis, ozone is used to cleave a carbon–carbon double bond to form aldehydes and ketones, or carboxylic acids, depending on the work-up.
Ozone is a symmetrical bent molecule stabilized by a resonance structure.
Ozone is a symmetrical bent molecule stabilized by a resonance structure.
11.1K
Preparation of 1° Amines: Hofmann and Curtius Rearrangement Mechanism
3.6K
The Hofmann and Curtius rearrangement reactions can be applied to synthesize primary amines from carboxylic acid derivatives such as amides and acyl azides. In the Hofmann rearrangement, a primary amide undergoes deprotonation in the presence of a base, followed by halogenation to generate an N-haloamide. A second proton abstraction produces a stabilized anionic species, which rearranges to an isocyanate intermediate via an alkyl group migration from the carbonyl carbon to the neighboring...
3.6K
Aldehydes and Ketones with HCN: Cyanohydrin Formation Mechanism
3.4K
Cyanohydrins are formed when cyanide nucleophiles and carbonyl compounds like aldehydes and ketones react. A strong base, the cyanide ion, catalyzes cyanohydrin formation. The ions are generated from HCN under aqueous conditions. Once the cyanide ions are generated, the first step involves the nucleophilic attack of the cyanide ions on the electrophilic carbonyl carbon. This attack shifts the π electrons from the C=O to the oxygen atom forming the alkoxide ion intermediate. The alkoxide anion...
3.4K

![Protein Film Infrared Electrochemistry Demonstrated for Study of H2 Oxidation by a [NiFe] Hydrogenase](/_next/image?url=https%3A%2F%2Fcloudfront.jove.com%2FCDNSource%2Fteasers%2F55858.jpg&w=3840&q=50)
