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DOI | 10.1038/s41467-018-02900-1 |
Heterogeneous Fe-3 single-cluster catalyst for ammonia synthesis via an associative mechanism | |
Liu, Jin-Cheng; Ma, Xue-Lu; Li, Yong; Wang, Yang-Gang; Xiao, Hai; Li, Jun1 | |
2018-04-23 | |
发表期刊 | NATURE COMMUNICATIONS
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ISSN | 2041-1723 |
出版年 | 2018 |
卷号 | 9 |
文章类型 | Article |
语种 | 英语 |
国家 | Peoples R China |
英文摘要 | The current industrial ammonia synthesis relies on Haber-Bosch process that is initiated by the dissociative mechanism, in which the adsorbed N-2 dissociates directly, and thus is limited by Bronsted-Evans-Polanyi (BEP) relation. Here we propose a new strategy that an anchored Fe-3 cluster on the theta-Al2O3(010) surface as a heterogeneous catalyst for ammonia synthesis from first-principles theoretical study and microkinetic analysis. We have studied the whole catalytic mechanism for conversion of N-2 to NH3 on Fe-3/theta-Al2O3(010), and find that an associative mechanism, in which the adsorbed N-2 is first hydrogenated to NNH, dominates over the dissociative mechanism, which we attribute to the large spin polarization, low oxidation state of iron, and multi-step redox capability of Fe-3 cluster. The associative mechanism liberates the turnover frequency (TOF) for ammonia production from the limitation due to the BEP relation, and the calculated TOF on Fe-3/theta-Al2O3(010) is comparable to Ru B5 site. |
领域 | 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000430541900026 |
WOS关键词 | N-2 REDUCTION ; IRON COMPLEXES ; NITROGEN REDUCTION ; AMBIENT CONDITIONS ; ELECTRO-CATALYSTS ; SCALING RELATIONS ; FE-N-2 COMPLEX ; VOLCANO CURVE ; CO OXIDATION ; DINITROGEN |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/203665 |
专题 | 资源环境科学 |
作者单位 | 1.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China; 2.Tsinghua Univ, Minist Educ, Key Lab Organ Optoelect & Mol Engn, Beijing 100084, Peoples R China |
推荐引用方式 GB/T 7714 | Liu, Jin-Cheng,Ma, Xue-Lu,Li, Yong,et al. Heterogeneous Fe-3 single-cluster catalyst for ammonia synthesis via an associative mechanism[J]. NATURE COMMUNICATIONS,2018,9. |
APA | Liu, Jin-Cheng,Ma, Xue-Lu,Li, Yong,Wang, Yang-Gang,Xiao, Hai,&Li, Jun.(2018).Heterogeneous Fe-3 single-cluster catalyst for ammonia synthesis via an associative mechanism.NATURE COMMUNICATIONS,9. |
MLA | Liu, Jin-Cheng,et al."Heterogeneous Fe-3 single-cluster catalyst for ammonia synthesis via an associative mechanism".NATURE COMMUNICATIONS 9(2018). |
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