在原子精确纳米集群中,金属可访问性对二氧化碳电减的作用
Yingwei Li1, Grant J Stec1, Agnes E Thorarinsdottir1
1Department of Chemistry & Chemical Biology, Harvard University 12 Oxford Street Cambridge Massachusetts 02138 USA mason@chemistry.harvard.edu.
Chemical science
|November 16, 2023
概括
具有更容易访问的金属位点的原子精确纳米集群在将二氧化碳 (CO2) 转化为一氧化碳 (CO) 中表现出更高的效率. 这项研究揭示了可访问的地点,而不仅仅是尺寸,是有效的二氧化碳电催化剂的关键.
科学领域:
- 纳米材料科学 科学 纳米材料科学
- 电触媒溶解是一种电触媒.
- 表面化学 表面化学
背景情况:
- 原子精确的纳米集群 (NCs) 对二氧化碳还原反应 (CO2RR) 研究非常有价值.
- 由于大小,表面结构和连接体密度等混因素,在NC中理解结构-属性关系具有挑战性.
- 以前的研究往往侧重于大小依赖的趋势,忽视了影响催化活性的其他关键因素.
研究的目的:
- 调查可访问的金属位点对原子精确纳米集群中CO2RR活动和选择性的影响.
- 建立一种可通用的方法来确定NCs上的CO2可访问站点.
- 为了将表面可访问性与电催化性能相关联,独立于纳米集群大小.
主要方法:
- 合成和表征了一系列金银纳米集群,其配体密度不同,但尺寸相似.
- 开发了一种方法来量化每个纳米集群上可访问的CO2站点的数量.
- 进行了电化学二氧化碳减排反应 (CO2RR) 研究,以测量二氧化碳的法拉达效率 (FECO).
主要成果:
- 具有更多可访问金属位点的纳米集群 ([Au43(CCR) 20和[Au42Ag1(CCR) 20]) 在 -0.57 V 与 RHE.相比,实现了>90%的FECO.
- 具有更少可访问地点的纳米集群显示FECO减少.
- 对更广泛的金-基尼尔NCs的研究证实,FECO与可访问的金属位点相关,无论NC大小如何.
结论:
- 可访问的金属位点的数量是原子精确纳米集群中CO2RR性能的关键决定因素.
- 已经建立了一个基于电催化剂的表面可访问性来评估NC的可泛化的方法.
- 这一发现为设计高效的NC电催化剂用于二氧化碳转化提供了新的视角.
更多相关视频
08:40Synthesis of Metal Nanoparticles Supported on Carbon Nanotube with Doped Co and N Atoms and its Catalytic Applications in Hydrogen Production
Published on: December 6, 2021
3.6K
10:22In Situ SIMS and IR Spectroscopy of Well-defined Surfaces Prepared by Soft Landing of Mass-selected Ions
Published on: June 16, 2014
18.2K
相关概念视频
02:51Metal-Ligand Bonds
20.8K
The hemoglobin in the blood, the chlorophyll in green plants, vitamin B-12, and the catalyst used in the manufacture of polyethylene all contain coordination compounds. Ions of the metals, especially the transition metals, are likely to form complexes.
In these complexes, transition metals form coordinate covalent bonds, a kind of Lewis acid-base interaction in which both of the electrons in the bond are contributed by a donor (Lewis base) to an electron acceptor (Lewis acid). The Lewis acid in...
In these complexes, transition metals form coordinate covalent bonds, a kind of Lewis acid-base interaction in which both of the electrons in the bond are contributed by a donor (Lewis base) to an electron acceptor (Lewis acid). The Lewis acid in...
20.8K
02:58Crystal Field Theory - Octahedral Complexes
26.6K
Crystal Field Theory
To explain the observed behavior of transition metal complexes (such as colors), a model involving electrostatic interactions between the electrons from the ligands and the electrons in the unhybridized d orbitals of the central metal atom has been developed. This electrostatic model is crystal field theory (CFT). It helps to understand, interpret, and predict the colors, magnetic behavior, and some structures of coordination compounds of transition metals.
CFT focuses on...
To explain the observed behavior of transition metal complexes (such as colors), a model involving electrostatic interactions between the electrons from the ligands and the electrons in the unhybridized d orbitals of the central metal atom has been developed. This electrostatic model is crystal field theory (CFT). It helps to understand, interpret, and predict the colors, magnetic behavior, and some structures of coordination compounds of transition metals.
CFT focuses on...
26.6K