Direct Synthesis of Ammonia from N-2 and H2O on Different Iron Species Supported on Carbon Nanotubes using a Gas-Phase Electrocatalytic Flow Reactor | |
Chen, Shiming1,2; Perathoner, Siglinda1; Ampelli, Claudio1; Wei, Hua1; Abate, Salvatore1; Zhang, Bingsen3; Centi, Gabriele4,5 | |
通讯作者 | Chen, Shiming(chenshiming@dicp.ac.cn) ; Perathoner, Siglinda(perathon@unime.it) ; Centi, Gabriele(centi@unime.it) |
2020-05-13 | |
发表期刊 | CHEMELECTROCHEM
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ISSN | 2196-0216 |
卷号 | 7期号:14页码:11 |
摘要 | Green NH3 production by direct electrocatalytic synthesis from N-2 and H2O is still a challenging reaction, which requires us to better understand the nature of the active materials. We show here that iron oxide (Fe2O3) nanoparticles (supported over carbon nanotubes, CNTs) become more active than the corresponding samples after reduction to form Fe- or Fe2N-supported nanoparticles, both indicated as active species in the thermal catalytic reduction of N-2 to ammonia. Characterization data, however, indicate that even for these Fe- and Fe2N-CNT samples, obtained from Fe2O3-CNT by reduction in H-2 or NH3 at 500 degrees C, the active species responsible for N-2 reduction reaction (NRR) at low applied potential (-0.5 V vs RHE) are the same, that is, small (<1-2 nm) iron oxide nanoparticles that are not detected by XRD, but evidenced by XPS and which amount could be correlated to the rate of ammonia formation. This species is stable for at least 24 h of electrocatalytic flow tests. However, at higher applied potentials, sintering/transformation of this species occurs, with loss of the electrocatalytic activity, and Fe2N nanoparticles may also be reduced in situ, forming ammonia, but with irreversible deactivation. |
关键词 | nitrogen reduction ammonia direct synthesis iron-oxide supported on carbon nanotubes electrocatalysis active species |
资助者 | ERC Synergy SCOPE ; PRIN 2017 MULTI-e project ; SINCHEM Grant ; Erasmus Mundus Action 1 Program |
DOI | 10.1002/celc.202000514 |
收录类别 | SCI |
语种 | 英语 |
资助项目 | ERC Synergy SCOPE[810182] ; PRIN 2017 MULTI-e project[20179337R7] ; SINCHEM Grant ; Erasmus Mundus Action 1 Program[FPA 2013-0037] |
WOS研究方向 | Electrochemistry |
WOS类目 | Electrochemistry |
WOS记录号 | WOS:000531900400001 |
出版者 | WILEY-V C H VERLAG GMBH |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.imr.ac.cn/handle/321006/138819 |
专题 | 中国科学院金属研究所 |
通讯作者 | Chen, Shiming; Perathoner, Siglinda; Centi, Gabriele |
作者单位 | 1.Dept ChimBioFarAm, Vle F Stagno D'Alcontres 31, I-98166 Messina, Italy 2.Chinese Acad Sci, Dalian Inst Chem Phys, 457 Zhongshan Rd, Dalian 116023, Peoples R China 3.Chinese Acad Sci IMR CAS, Inst Met Res, Catalysis & Mat Div, 72 Wenhua Rd, Shenyang 110016, Peoples R China 4.Univ Messina, Dept MIFT Ind Chem, ERIC Aisbl, Vle F Stagno D'Alcontres 31, I-98166 Messina, Italy 5.INSTM CASPE, Vle F Stagno D'Alcontres 31, I-98166 Messina, Italy |
推荐引用方式 GB/T 7714 | Chen, Shiming,Perathoner, Siglinda,Ampelli, Claudio,et al. Direct Synthesis of Ammonia from N-2 and H2O on Different Iron Species Supported on Carbon Nanotubes using a Gas-Phase Electrocatalytic Flow Reactor[J]. CHEMELECTROCHEM,2020,7(14):11. |
APA | Chen, Shiming.,Perathoner, Siglinda.,Ampelli, Claudio.,Wei, Hua.,Abate, Salvatore.,...&Centi, Gabriele.(2020).Direct Synthesis of Ammonia from N-2 and H2O on Different Iron Species Supported on Carbon Nanotubes using a Gas-Phase Electrocatalytic Flow Reactor.CHEMELECTROCHEM,7(14),11. |
MLA | Chen, Shiming,et al."Direct Synthesis of Ammonia from N-2 and H2O on Different Iron Species Supported on Carbon Nanotubes using a Gas-Phase Electrocatalytic Flow Reactor".CHEMELECTROCHEM 7.14(2020):11. |
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