仅限于外层的单原子催化剂,通过修改的自上而下的策略实现高效的CO2减排
Dong Wei1, Aihao Xu2, Xiangyu Chen1
1Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology, School of Chemistry and Chemical Engineering, Guangxi University, Nanning 530004, China.
一种新方法通过原子化硫化纳米粒子来合成高性能单原子催化剂 (SAC). 这种方法提高了原子利用率,并提高了减少二氧化碳的催化活性,实现了近100%的效率.
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.
- 电化学 电化学 电化学
背景情况:
- 高温热解是一种合成单原子催化剂 (SAC) 的常用方法.
- 这种方法往往导致由于金属原子迁移而导致低原子利用.
- 为SACs开发高效的合成策略对于催化是至关重要的.
研究的目的:
- 为高性能单原子催化剂开发一种新的自上而下的合成策略.
- 为了实现 in situ 原子化和单个原子在支结构中的封闭.
- 为了提高减少二氧化碳的催化性能.
主要方法:
- 合成了表面化硫化 (NiS2) 纳米粒子.
- 采用了自上而下的原子化策略来产生单个Ni原子.
- 电化学CO2减排是在一个流动细胞中进行的.
- 用理论计算来研究反应机制.
主要成果:
- 新的合成策略成功地将NiS2纳米颗粒原子化为单个Ni原子,限制在外层内.
- 单个Ni原子主要分布在支表面上,提高了活跃站点的可访问性.
- 理论计算显示,第二个协调中的S原子减少了二氧化碳减排的激活能量.
- 单原子催化剂在一个广泛的潜能范围 (-0.5到-1.3V与RHE) 上实现了近100%的法拉代效率 (FE_CO).
- 在-1.6V与RHE相比,CO的最大部分电流密度为709mA cm-2在-1.6V与RHE相比,得到了最大部分电流密度.
结论:
- 开发的自上而下的合成策略为生产高效的单原子催化剂提供了一个有前途的途径.
- 单个Ni原子的封闭和表面分布显著提高了催化性能.
- S原子的存在在增强二氧化碳还原反应动力学方面起着至关重要的作用.
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