由电荷转移驱动的氧进化反应从Cr复合物转移到含有多氧金属酸盐的多孔离子晶体
Yuto Shimoyama1, Naoki Ogiwara1, Zhewei Weng1
1Department of Basic Science, School of Arts and Sciences, The University of Tokyo, Komaba, Meguro-ku, Tokyo 153-8902, Japan.
Journal of the American Chemical Society
|January 18, 2022
概括
具有多氧金属酸盐 (Co-POM) 的多孔离子晶体 (PIC) 显示出高效的氧化演化反应 (OER) 催化. 这项研究澄清了协同机制,揭示了组件之间的电荷转移在非基本条件下增强了催化活性.
科学领域:
- 电化学
- 材料科学
- 催化剂
背景情况:
- 过渡金属氧化物对于氧化演化反应 (OER) 催化是至关重要的.
- 含有的多氧金属酸盐 (Co-POM) 是有前途的开放式化学反应催化剂.
- 由于其复杂的结构,了解Co-POM纳米复合材料的协同效应具有挑战性.
研究的目的:
- 建立基于Co-POM的催化剂的组成结构功能关系.
- 阐明OER的多孔离子晶体 (PIC) 中协同催化的起源.
- 在非基本条件下使用专门设计的PIC进行OER调查.
主要方法:
- 使用Keggin型[α-CoW12O40]6−和Cr复合物的多孔离子晶体 (PIC) 的合成.
- 电化学特征包括线性扫描电压测量和动态同位素效应研究.
- 探测电荷转移和反应中间体的光谱分析.
主要成果:
- 合成的PIC具有高效和持续的OER催化活性,而单个构件则不活跃.
- 塔菲尔斜率和动态同位素效应表明限制速度的步骤涉及单个电子和质子转移.
- 协同催化源于Cr复合体向[α-CoW12O40]6−的电荷转移,增强其电子密度和催化性能.
结论:
- PIC为基于POM的催化剂提供了一个明确的组成-结构-功能关系的平台.
- 这种PIC的协同效应通过促进电子和质子转移来增强OER活动.
- 这项工作提供了基于POM的高效和稳定的OER催化剂设计的见解.
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