Phosphorus-doped onion-like carbon for CO2 electrochemical reduction: the decisive role of the bonding configuration of phosphorus | |
Liu, TianFu1,2; Ali, Sajjad1,3; Lian, Zan1,2; Si, ChaoWei1,2; Su, Dang Sheng1; Li, Bo1 | |
Corresponding Author | Su, Dang Sheng(dssu@imr.ac.cn) ; Li, Bo(boli@imr.ac.cn) |
2018-11-07 | |
Source Publication | JOURNAL OF MATERIALS CHEMISTRY A
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ISSN | 2050-7488 |
Volume | 6Issue:41Pages:8 |
Abstract | Doping with heteroatoms, such as nitrogen and boron, is crucial for the good performance of metal-free carbon cathode catalysts in the CO2 electrochemical reduction reaction (CERR). In this report, for the first time phosphorus is used to fabricate carbon catalysts and it is found that the bonding configuration of phosphorus has a key effect on the performance of the CERR. Two different phosphorus doped onion-like carbon (P-OLC) catalysts are synthesized with P-O bonding or P-C bonding as the major phosphorus bonding configuration, respectively. Compared to P-OLC with P-O bonding, P-OLC with P-C bonding exhibits a much better CERR performance, with a partial current density of 4.9 mA cm(-2), 81% faradaic efficiency, and excellent durability (27 h) at low potential (-0.90 V vs. SHE). Density functional theory calculations show that the binding energy of the key intermediate COOH* in P-C bonding is much higher than that of its counterpart in P-O bonding, which is beneficial for lowering the energy barrier of the rate-limiting step. The better reactivity of the P-C bonding site is also verified by aromaticity analysis. Moreover, ultraviolet photoelectron spectroscopy (UPS) and partial density of state (PDOS) analysis suggest that the electron transfer capability of P-C bonding is stronger than that of P-O bonding. The current study demonstrates that phosphorus doping is an effective strategy for fabricating carbon CERR catalysts and reveals the pivotal role of the phosphorus bonding configuration. |
Funding Organization | NSFC ; Institute of Metal Research ; State Key Laboratory of Catalytic Materials and Reaction Engineering (RIPP, SINOPEC) ; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund (the second phase) |
DOI | 10.1039/c8ta06649c |
Indexed By | SCI |
Language | 英语 |
Funding Project | NSFC[21573255] ; NSFC[51521091] ; Institute of Metal Research[Y3NBA211A1] ; State Key Laboratory of Catalytic Materials and Reaction Engineering (RIPP, SINOPEC) ; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund (the second phase)[U1501501] |
WOS Research Area | Chemistry ; Energy & Fuels ; Materials Science |
WOS Subject | Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary |
WOS ID | WOS:000448412700012 |
Publisher | ROYAL SOC CHEMISTRY |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.imr.ac.cn/handle/321006/130067 |
Collection | 中国科学院金属研究所 |
Corresponding Author | Su, Dang Sheng; Li, Bo |
Affiliation | 1.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Liaoning, Peoples R China 2.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Liaoning, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China |
Recommended Citation GB/T 7714 | Liu, TianFu,Ali, Sajjad,Lian, Zan,et al. Phosphorus-doped onion-like carbon for CO2 electrochemical reduction: the decisive role of the bonding configuration of phosphorus[J]. JOURNAL OF MATERIALS CHEMISTRY A,2018,6(41):8. |
APA | Liu, TianFu,Ali, Sajjad,Lian, Zan,Si, ChaoWei,Su, Dang Sheng,&Li, Bo.(2018).Phosphorus-doped onion-like carbon for CO2 electrochemical reduction: the decisive role of the bonding configuration of phosphorus.JOURNAL OF MATERIALS CHEMISTRY A,6(41),8. |
MLA | Liu, TianFu,et al."Phosphorus-doped onion-like carbon for CO2 electrochemical reduction: the decisive role of the bonding configuration of phosphorus".JOURNAL OF MATERIALS CHEMISTRY A 6.41(2018):8. |
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