补充剂通过转化促进协同催化 吸附行为以实现有效的电化学酸盐降解反应
Zhijie Cui1, Honghai Wang1, Chunli Li1
1School of Chemical Engineering and Technology, National-Local Joint Engineering Laboratory for Energy Conservation in Chemical Process Integration and Resources Utilization, Hebei University of Technology, Tianjin 300130, China.
这项研究引入了添加的催化剂,用于高效的电化学降解反应 (NO3RR),使废水处理和氨 (NH3) 合成能够同时进行. 这些新型的双重催化站点显著提高了性能,并提供了能源生产能力.
科学领域:
- 电化学
- 材料科学
- 催化剂
- 环境科学
背景情况:
- 电化学降解反应 (NO3RR) 为处理污染废水和合成氨 (NH3) 提供了双重解决方案.
- 了解NO3RR中的不同脱氧和化步骤对于催化剂设计至关重要,因为活性位点通常表现出类似的吸附行为.
- 开发高效的催化剂是优化NO3RR对环境修复和化学合成的关键.
研究的目的:
- 合成和表征用于增强NO3RR的新型化单原子和原子催化剂 (Co SAAC/INC).
- 阐明异质原子对位电子结构和催化活性的影响机制.
- 调查Zn-NO3电池中的Co SAAC/INC的性能,以同时去除污染物,合成NH3和提供能量.
主要方法:
- 使用温和的蚀刻同步策略,在 doped 碳上合成 doped 改性单个原子 (I-CoN4) 和原子集群 (Co AC).
- 在中性电解质中进行电化学表征,包括测量NH3产率和法拉第效率 (FE).
- 现场电化学里埃红外光谱学,在线微分电化学质谱学,确认实验和密度函数理论 (DFT) 计算来分析反应机制.
- 使用Co SAAC/INC作为阴极的Zn-NO3电池的制造和测试.
主要成果:
- 在中性电解质中,Co SAAC/ INC表现出高的NH3输出率为18.64 mgh-1 mgcat-1 在- 0. 7V与RHE之间,以及97.2%的优异FE.
- 第二层兴奋剂有效调节了CoN4位点的电子结构,促进了H2O/*H相对于NO3-的有利吸附.
- 邻近的Co AC站点促进了H2O解离,为化步骤提供了活性 (Hads),形成了与I-CoN4的联动催化站点.
- -NO3电池表现出高功率密度 (15.41 mW cm-2) 和高效的NH3合成,加上酸盐去除和发电.
结论:
- 这项研究成功地阐明了NO3RR增强的机制,突出了在调节电子结构和吸附性质方面的作用.
- 开发涉及I-CoN4和Co AC的合催化位,对于促进电化学酸盐还原反应至关重要.
- 综合系统展示了可持续的废水处理,氨生产和能源采集的有希望的方法.
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