化学链燃烧
等离子体
环境科学
材料科学
化学工程
化学
环境化学
废物管理
工程类
物理化学
物理
燃烧
量子力学
作者
Yanhui Long,Xingzi Wang,Hai Zhang,Kaiyi Wang,Wee‐Liat Ong,Annemie Bogaerts,Kongzhai Li,Chunqiang Lu,Xiaodong Li,Jianhua Yan,Xin Tu,Hao Zhang
出处
期刊:JACS Au
[American Chemical Society]
日期:2024-05-08
卷期号:4 (7): 2462-2473
被引量:40
标识
DOI:10.1021/jacsau.4c00153
摘要
High Resolution Image Download MS PowerPoint Slide We propose a plasma chemical looping CO 2 splitting (PCLCS) approach that enables highly efficient CO 2 conversion into O 2 -free CO at mild temperatures. PCLCS achieves an impressive 84% CO 2 conversion and a 1.3 mmol g –1 CO yield, with no O 2 detected. Crucially, this strategy significantly lowers the temperature required for conventional chemical looping processes from 650 to 1000 °C to only 320 °C, demonstrating a robust synergy between plasma and the Ce 0.7 Zr 0.3 O 2 oxygen carrier (OC). Systematic experiments and density functional theory (DFT) calculations unveil the pivotal role of plasma in activating and partially decomposing CO 2, yielding a mixture of CO, O 2 /O, and electronically/vibrationally excited CO 2 *. Notably, these excited CO 2 * species then efficiently decompose over the oxygen vacancies of the OCs, with a substantially reduced activation barrier (0.86 eV) compared to ground-state CO 2 (1.63 eV), contributing to the synergy. This work offers a promising and energy-efficient pathway for producing O 2 -free CO from inert CO 2 through the tailored interplay of plasma and OCs.
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