Phosphorus-doped onion-like carbon for CO2 electrochemical reduction: the decisive role of the bonding configuration of phosphorus

doi:10.1039/c8ta06649c

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	Phosphorus-doped onion-like carbon for CO2 electrochemical reduction: the decisive role of the bonding configuration of phosphorus
	Liu, TianFu 1,2; Ali, Sajjad 1,3; Lian, Zan 1,2; Si, ChaoWei 1,2; Su, Dang Sheng 1; Li, Bo 1
刊名	JOURNAL OF MATERIALS CHEMISTRY A
	2018-11-07
卷号	6 期号:41 页码:8
ISSN号	2050-7488
DOI	10.1039/c8ta06649c
通讯作者	Su, Dang Sheng(dssu@imr.ac.cn) ; Li, Bo(boli@imr.ac.cn)
英文摘要	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.
资助项目	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研究方向	Chemistry ; Energy & Fuels ; Materials Science
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000448412700012
资助机构	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)
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/130066]
专题	金属研究所_中国科学院金属研究所
通讯作者	Su, Dang Sheng; Li, Bo
作者单位	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
推荐引用方式 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.