在扭曲的CoP4配置上通过酶途径实现光催化总固定
Xin Wang1,2, Yuqi Zhao1,3, Xi Wu1,4
1Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055, China.
Angewandte Chemie (International ed. in English)
|December 23, 2024
概括
研究人员开发了一种新型的单原子催化剂 (SAC),可显著提高光催化固定效率. 这一突破通过优化分子激活和吸附来改善氨生产.
科学领域:
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
- 摄影化学的使用.
背景情况:
- 光催化固化对于氨合成至关重要,但由于效率低而受到限制.
- 微弱的吸附和NN键解离阻碍了基于半导体的催化剂.
研究的目的:
- 为光催化固定设计具有增强 (N2) 吸附和激活的单原子催化剂 (SAC).
- 为了研究C缺陷引起的CoP4扭曲配置对催化性能的影响.
主要方法:
- 使用选择性化策略制造一个单原子催化剂 (Co SAC).
- 利用P-doping和碳缺陷来调整矿场的电子结构.
- 使用实验和理论计算来分析N2吸附和激活机制.
主要成果:
- 扭曲的CoP4配置促进了侧面N2吸附模式,具有高吸附能量 (-1.40 eV) 和延长的N-N键 (1.20 Å).
- 在没有牺牲剂的情况下,达到1249.5μmolh-1g-1的高氨产率.
- 在365nm时显示出3.51%的表面量子产量,表明光催化效率高.
结论:
- 开发的Co SAC通过优化N2吸附和激活,显著提高光催化固定效率.
- 选择性化策略适用于合成其他单原子催化剂 (例如Ni,Fe).
- 这项工作为有效的光催化N2固定提供了对共同调节电子结构的见解.
更多相关视频
相关概念视频
The Z-Scheme of Electron Transport in Photosynthesis
9.9K
The light reactions of photosynthesis assume a linear flow of electrons from water to NADP+. During this process, light energy drives the splitting of water molecules to produce oxygen. However, oxidation of water molecules is a thermodynamically unfavorable reaction and requires a strong oxidizing agent. This is accomplished by the first product of light reactions: oxidized P680 (or P680+), the most powerful oxidizing agent known in biology. The oxidized P680 that acquires an electron from the...
9.9K
Photochemical Electrocyclic Reactions: Stereochemistry
1.8K
The absorption of UV–visible light by conjugated systems causes the promotion of an electron from the ground state to the excited state. Consequently, photochemical electrocyclic reactions proceed via the excited-state HOMO rather than the ground-state HOMO. Since the ground- and excited-state HOMOs have different symmetries, the stereochemical outcome of electrocyclic reactions depends on the mode of activation; i.e., thermal or photochemical.
Selection Rules: Photochemical Activation
Selection Rules: Photochemical Activation
1.8K
Oxygenic Photosynthesis
Oxygenic photosynthesis is a fundamental process in which light energy is harnessed to drive the oxidation of water, leading to the production of molecular oxygen (O₂), adenosine triphosphate (ATP), and nicotinamide adenine dinucleotide phosphate (NADPH). This process is essential for sustaining aerobic life on Earth and is primarily carried out by cyanobacteria, algae, and plants. The core of oxygenic photosynthesis lies in the thylakoid membranes, where chlorophyll pigments facilitate...
Anoxygenic Photosynthesis
Anoxygenic photosynthesis is a phototrophic process that captures light energy to drive carbon fixation without producing molecular oxygen. Unlike oxygenic photosynthesis, which utilizes water as an electron donor and releases oxygen, anoxygenic phototrophs use alternative electron donors such as hydrogen sulfide (H₂S), elemental sulfur (S⁰), or thiosulfate (S₂O₃²⁻). This process is carried out by diverse groups of bacteria, including purple bacteria, green...
Photosystem I
61.7K
Although structurally similar to photosystem II (PSII), photosystem I (PSI) is has a different electron supplier and electron acceptor.
Both these photosystems work in concert. An excited electron from PSII is relayed to PSI via an electron transport chain in the thylakoid membrane of the chloroplast, which is comprised of the carrier molecule plastoquinone, the dual-protein cytochrome complex, and plastocyanin. As electrons move between PSII and PSI, they lose energy and must be re-energized...
Both these photosystems work in concert. An excited electron from PSII is relayed to PSI via an electron transport chain in the thylakoid membrane of the chloroplast, which is comprised of the carrier molecule plastoquinone, the dual-protein cytochrome complex, and plastocyanin. As electrons move between PSII and PSI, they lose energy and must be re-energized...
61.7K
The Calvin Benson Cycle
4.4K
Ribulose 1,5- bisphosphate carboxylase/oxygenase (RuBisCo) is a critical enzyme that catalyzes carbon dioxide assimilation during photosynthesis. However, it is an inefficient enzyme, having an extremely slow catalytic rate. A typical enzyme can process about a thousand molecules per second; however, RuBisCo fixes only around three-carbon dioxides per second. Photosynthetic cells compensate for this slow rate by synthesizing very high amounts of RuBisCo, making it the most abundant single...
4.4K

![Cercosporin-Photocatalyzed [4+1]- and [4+2]-Annulations of Azoalkenes Under Mild Conditions](/_next/image?url=https%3A%2F%2Fcloudfront.jove.com%2FCDNSource%2Fteasers%2F60786.jpg&w=3840&q=50)
