O,N协调介导单原子催化剂,用于高效生成H2O2
Bin Yue1, Liang Lin1, Ying Lei1
1College of Chemical Engineering, Sichuan University of Science and Engineering, Zigong 643000, PR China.
我们开发了一种新型的催化剂,在氧化碳黑上使用单个原子,以有效地在现场生产过氧化 (H2O2). 这种催化剂在电化学氧降解方面表现出高选择性和稳定性,为分散的H2O2生成铺平了道路.
科学领域:
- 电化学 电化学 电化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 过氧化 (H2O2) 的电化学生产为现场发电提供了一个可持续的途径.
- 开发高度选择性和稳定的催化剂对于通过两电子氧降解反应有效合成H2O2至关重要.
研究的目的:
- 合成和描述一种用于选择性电化学H2O2生产的新型单原子催化剂.
- 研究用于分散生成H2O2的开发材料的催化性能和稳定性.
主要方法:
- 在氧化碳黑 (OCB) 上通过协调复合物的热解合成由和氧 (Ni-N1O3) 协调的Ni单原子位.
- 使用偏差校正扫描传输电子显微镜 (AC-STEM) 和X射线吸收光谱 (XAS) 进行表征.
- 在H细胞中进行H2O2生产的电化学评估,包括动力学研究和稳定性测试. 用密度函数理论 (DFT) 的计算来理解反应机制.
主要成果:
- 成功合成了OCB (Ni-SACs@OCB) 上由N和O协调的Ni单原子位点.
- 在0.65V时达到高的H2O2选择性 (95%),动力电流密度为2.8mA cm-2和质量活性为24A gcat.-1,在0.65V时达到高的H2O2选择性.
- 证明了高的H2O2生产率98.5 mmolgcat.-1 h-1在H细胞中具有很好的稳定性.
- DFT计算表明,N,O介导的协调增强了氧吸附和对中间体的反应性,有利于H2O2的选择性.
结论:
- 新型N,O介导的四坐标单原子催化剂 (Ni-SACs@OCB) 对于选择性的电化学H2O2生产非常有效.
- 催化剂对实际的,分散的H2O2产生表现出有希望的性能和稳定性.
- 这项工作为设计高效电化学合成的单原子催化剂提供了新的途径.
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