电子移位的Ni活性位点在spinel催化剂中使有效的尿素氧化成为可能
Hui-Jian Zhang1, Zi-Qiang Chen1, Xiao-Tong Ye1
1School of Chemistry and Chemical Engineering/Institute of Clean Energy and Materials/Guangzhou Key Laboratory for Clean Energy and Materials/Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Guangzhou University, Guangzhou Higher Education Mega Center, No. 230 Wai Huan Xi Road, 510006, P. R. China.
调整催化剂的.
科学领域:
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
- 材料科学 材料科学 材料科学
背景情况:
- 尿素氧化反应 (UOR) 是氧化演化反应 (OER) 的一个有前途的替代方案,因为它具有较低的超电位.
- 基于的催化剂对UOR有希望,但选择性和机制仍然不清楚.
- 控制产品选择性和理解尿素解离是关键的挑战.
研究的目的:
- 研究位中的电子脱位如何影响尿素解离和UOR中的产品选择性.
- 使用旋NiCo2O4作为模型催化剂来调整电子属性.
- 澄清管理UOR效率和选择性的基本机制.
主要方法:
- 在NiCo2O4螺旋中使用替代来调整活性位点的电荷移位.
- 进行电化学实验以测量UOR性能,包括电流密度和法拉第效率.
- 使用理论计算来理解尿素解离路径和氧化物结合点.
主要成果:
- 在NiCo2O4中完全替代,显著提高了 (N2) 选择性,达到26.8%,峰值电流密度为300mA·cm-2.2.
- 部分替代实现了高法拉第效率78.1%的液体产品 (NOx-).
- 强大的电荷移位促进了氧化物对尿素的远程攻击,有利于N2选择性和抑制OER.
- 弱移位有利于附近的网站攻击,提高了UOR的效率.
结论:
- 在Ni位点调节电子移位对于控制OH−结合和尿素解离路径至关重要.
- 在NiCo2O4中替代提供了选择性UOR催化的一种可行的策略.
- 了解这些机制可以指导用于尿素氧化的高效电催化剂的设计.
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