在平面内和平面间铜双单原子催化剂中的散装类碳化物用于级联CO2光降解
Xiaoyang Yue1, Lei Cheng1, Chen Guan1
1State Key Laboratory of Electronic Thin Film and Integrated Devices, School of Electronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu, 610054, P. R. China.
Small (Weinheim an der Bergstrasse, Germany)
|November 10, 2023
概括
双重单原子催化剂 (DSACs) 在散装类碳化物中具有内平面Pd和间平面Cu,可显著提高CO产量. 这种双原子设计优化了催化活性,提高了二氧化碳的转化.
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.
- 纳米技术纳米技术
背景情况:
- 双单原子催化剂 (DSAC) 提供了超越传统单原子催化剂 (SAC) 的协同效应.
- 精确的合成和DSAC的功能化仍然是催化研究的一个重大挑战.
研究的目的:
- 开发精确合成的DSAC,具有不同的原子位点,以提高催化性能.
- 研究二氧化碳转化中的双单原子催化剂的协同效应和反应机制.
主要方法:
- 将双单原子 (Pd和Cu) 纳入层叠的散装类碳化物 (b-CN) 框架.
- 使用femtosecond时间解析的短暂吸收 (fs-TA) 谱学的表征.
- 通过密度函数理论 (DFT) 模拟进行理论分析.
主要成果:
- 一种新的DSAC,Pd1-Cu1/b-CN,用平面内三坐标Pd和平面间四坐标Cu位点合成.
- fs-TA光谱检测显示,与平面间Cu (3.07ps) 相比,平面内Pd (95.6ps) 的电荷衰变寿命显著更长.
- Pd1-Cu1/b-CN催化剂的碳排放量增加了3.47倍,表现优于b-CN,Pd1/b-CN和Cu1/b-CN.
结论:
- 精确定义的Pd1-Cu1/b-CN双功能级联系统提高了CO2-CO转换效率.
- 在平面内Pd作为有利的电子捐赠活性位点,对催化过程至关重要.
- 在二氧化碳吸附和化过程中,DFT的计算证实了在二氧化碳吸附和化过程中具有独特的s-p合与d-p混合机制,有利于二氧化碳的产生.
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