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基于合成烯的[FeFe]-酶活性位点的生物启发模型,用于电催化进化
Afridi Zamader1,2, Bertrand Reuillard1, Julien Pérard1
1Univ Grenoble Alpes, CNRS, CEA, IRIG, Laboratoire de Chimie et Biologie des Métaux 17 rue des Martyrs 38000 Grenoble France bertrand.reuillard@cea.fr.
Sustainable energy & fuels
|November 28, 2023
概括
这项研究将仿生催化剂集成到聚合物支架中,以提高太阳能燃料生产. 由此产生的金属聚合物与孤立催化剂相比,显著提高了的生产速度和稳定性.
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.
- 能源转换 能源转换
背景情况:
- 在聚合物支架中集成的分子催化剂为催化应用提供了增强的稳定性和类似酶的特性.
- 这种方法对于推进太阳能燃料研究和化学能源转换,提高反应速度和能源效率至关重要.
- 当前系统性能需要进一步提高电流密度和稳定性,这些都受到内置的分子催化剂的影响.
研究的目的:
- 合成和表征含有仿生 [2Fe2S] 活性位点的金属聚合物,以[FeFe] 化酶为灵感.
- 研究这些金属聚合物在中性水性介质中的电化学生产活性.
- 优化催化剂性能,通过变化烯含量和固定金属聚合物在多壁碳纳米管 (MWNT) 上.
主要方法:
- 使用自由基聚合,将生物仿真{Fe2(μ-adt) ((CO) 6}活性部位整合到合成聚合物支架中.
- 由此产生的金属聚合物, [2Fe2S]adt[DMAEMA][PyBMA],具有水溶性 (DMAEMA) 和疏水性 (PyBMA) 单体的不同比例的特征.
- 进行了电化学生产,并将最活跃的金属聚合物固定在MWNT上进行进一步测试.
主要成果:
- 合成的金属聚合物在中性水性介质中对电化学 (H2) 生产具有活性.
- 在MWNT上固定并优化烯含量 (∼2.3 mol%) 显著提高了性能.
- 优化的金属聚合物在20小时的时间内,在0.49V的超电位下,实现了生产的周转率 (TONH) ∼0.4 × 10^5,比孤立的催化剂高两倍.
结论:
- 该研究提出了一种可行的合成方法,用于将具有第二协调球功能组的催化单元纳入聚合物矩阵.
- 在聚合物矩阵内封闭显然有利于催化性能,从而提高生产的活性和稳定性.
- 这项工作有助于开发用于高效太阳能燃料生产和化学能源转换的先进材料.
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