基激进使工业水平的氧气电还原到过氧化
Song Xue1, Xiaohui Li1,2, Yuanyuan Sun2
1Research Center on Advanced Chemical Engineering and Energy Materials, China University of Petroleum (East China), Changjiang West Road 66, 266580, Qingdao, P. R. China.
Angewandte Chemie (International ed. in English)
|November 21, 2024
概括
这项研究表明,局部质子的可用性是高效的电化学过氧化 (H2O2) 合成的关键. 一个新的在氧化碳纳米管电极上增强了反应动力学和选择性,以实现可持续的H2O2生产.
科学领域:
- 电化学 电化学 电化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 使用可再生电力的过氧化 (H2O2) 的电化学合成为能源密集的工业自氧化过程提供了一个可持续的替代方案.
- 两电子氧降解反应 (2e-ORR) 机制,特别是局部质子的作用,仍然不完全理解,阻碍了优化.
- 开发高效的电催化剂对于推动可持续的H2O2生产至关重要.
研究的目的:
- 研究当地的质子可用性对2e-ORR的动力学和选择性的影响.
- 阐明相关中间体在2e-ORR机制中的作用.
- 设计和评估一种合作电极材料,用于增强H2O2合成.
主要方法:
- 合理设计了一种合作电极材料:嵌入氧化碳纳米管复合材料 (Co-OCNT) 的 (II) 集群.
- 通过使用可再生电力供电的电化学合成研究了2e-ORR.
- 使用Co-OCNT材料分析了反应动力学,选择性和中间路径.
主要成果:
- 证实了一种涉及基转移的2e-ORR过程,其中局部质子可用性决定了反应性能.
- Co-OCNT 电极表现出卓越的动力学和选择性,实现了约40.6 mol gcat−1 h−1 的 H2O2 生产速率和在 300 mA cm−2.2. 的 90% 的法拉达效率.
- 氧化碳纳米管站点促进了质子生产,而站点促进了ORR中间体的形成,展示了合作的双活性站点.
结论:
- 在Co-OCNT材料中的高局部质子可用性和合作双活性位点显著提高了H2O2合成的2e-ORR性能.
- 开发的材料显示了可持续和高效的电化学H2O2生产的前景.
- 使用电-芬顿工艺对2e-ORR进行级联处理,显示出高选择性 (97%) 对于从乙烯糖醇价值化中产生酸的产生.
相关概念视频
Radical Autoxidation
2.1K
The oxidation of an organic compound in the presence of air or oxygen is called autoxidation. For example, cumene reacts with oxygen to form hydroperoxide. Autoxidation involves initiation, propagation, and termination steps. Many organic compounds are susceptible to autoxidation—especially ethers in the presence of oxygen, which form hydroperoxides. Even though this reaction is slow, old ether bottles contain small amounts of peroxide, which leads to laboratory explosions during ether...
2.1K
Radical Formation: Abstraction
3.5K
The electron of an atom can be abstracted from a compound by a relatively unstable radical to generate a new radical of relatively greater stability. For example, an initiator which forms radicals by homolysis can abstract a suitable species like a hydrogen atom or a halogen atom from a compound to generate a new radical. This ability of radicals to propagate by abstraction is a crucial feature of radical chain reactions.
Even though homolysis produces radicals, it is different from radical...
Even though homolysis produces radicals, it is different from radical...
3.5K
Radical Formation: Homolysis
3.5K
A bond is formed between two atoms by sharing two electrons. When this bond is broken by supplying sufficient energy, either two electrons can be taken up by one atom forming ions by the cleavage called heterolysis, or the two electrons are shared by two atoms, with one each creating radicals by the cleavage called homolysis.
3.5K
Radical Anti-Markovnikov Addition to Alkenes: Mechanism
3.7K
The reaction of hydrogen bromide with alkenes in the presence of hydroperoxides or peroxides proceeds via anti-Markovnikov addition. The radical chain reaction comprises initiation, propagation, and termination steps.
The mechanism starts with chain initiation, which involves two steps. In the first chain initiation step, a weak peroxide bond is homolytically cleaved upon mild heating to form two alkoxy radicals. In the second initiation step, a hydrogen atom is abstracted by the alkoxy...
The mechanism starts with chain initiation, which involves two steps. In the first chain initiation step, a weak peroxide bond is homolytically cleaved upon mild heating to form two alkoxy radicals. In the second initiation step, a hydrogen atom is abstracted by the alkoxy...
3.7K
Reduction of Alkenes: Catalytic Hydrogenation
11.8K
Alkenes undergo reduction by the addition of molecular hydrogen to give alkanes. Because the process generally occurs in the presence of a transition-metal catalyst, the reaction is called catalytic hydrogenation.
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
11.8K
Reduction of Alkenes: Asymmetric Catalytic Hydrogenation
3.2K
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...
3.2K


