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Boosting electrocatalytic activity for CO2 reduction on nitrogen-doped carbon catalysts by co-doping with phosphorus
Chen, Shuo1,2; Liu, Tianfu2; Olanrele, Samson O.2; Lian, Zan2; Si, Chaowei2; Chen, Zhimin1; Li, Bo2
Corresponding AuthorChen, Zhimin(zmchen@hlju.edu.cn) ; Li, Bo(boli@imr.ac.cn)
2021-03-01
Source PublicationJOURNAL OF ENERGY CHEMISTRY
ISSN2095-4956
Volume54Pages:143-150
AbstractElectrochemical reduction of CO2 (CERR) to value-added chemicals is an attractive strategy for greenhouse gas mitigation, and carbon recycles utilization. Conventional metal catalysts suffered from low durability and sluggish kinetics impede the practical application. On the other hand, doped carbon materials recently demonstrate superior catalytic performance in CERR, which shows the potential to diminish the problems of metal catalysts to some extent. Herein, we present the design and fabrication of nitrogen (N), phosphorus (P) co-doped metal-free carbon materials as an efficient and stable electrocatalyst for reduction of CO2 to CO, which exhibits an excellent performance with a high faradaic efficiency of 92% (-0.55 V vs. RHE) and up to 24 h stability. A series of characterizations including TEM and XPS verified that nitrogen and phosphorous are successfully incorporated into the carbon matrix. Moreover, the comparisons between co-doping and single doping catalysts reveal that co-doping can significantly increase CERR performance. The improved catalytic activity is attributed to the synergetic effects between nitrogen and phosphorous dopants, which effectively modulate properties of the active site. The density functional theory (DFT) calculations were also performed to understand the synergy effects of dopants. It is revealed that the phosphorous doping can significantly lower the Gibbs free energy of COOH* formation. Moreover, the introduction of the second dopants phosphorous can reduce the reaction barrier along the reaction path and cause polarization of density of states at the Fermi level. These changes can greatly enhance the activity of the catalysts. From a combined experimental and computational exploration, current work provides valuable insights into the reaction mechanism of CERR on N, P co-doped carbon catalysts, and the influence from synergy effects between dopants, which paves the way for the rational design of novel metal-free catalysts for CO2 electro-reduction. (C) 2020 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
KeywordMetal-free catalyst CO2 reduction Co-doping, DFT
Funding OrganizationNational Natural Science Foundation of China ; Natural Science Foundation of Liao Ning Province ; Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science ; 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)
DOI10.1016/j.jechem.2020.05.006
Indexed BySCI
Language英语
Funding ProjectNational Natural Science Foundation of China[21573255] ; National Natural Science Foundation of China[21573062] ; Natural Science Foundation of Liao Ning Province[20180510014] ; Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science ; 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 AreaChemistry ; Energy & Fuels ; Engineering
WOS SubjectChemistry, Applied ; Chemistry, Physical ; Energy & Fuels ; Engineering, Chemical
WOS IDWOS:000605328400018
PublisherELSEVIER
Citation statistics
Cited Times:10[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/158973
Collection中国科学院金属研究所
Corresponding AuthorChen, Zhimin; Li, Bo
Affiliation1.Heilongjiang Univ, Sch Chem & Mat Sci, Key Lab Funct Inorgan Mat Chem, Minist Educ China, Harbin 150080, Heilongjiang, Peoples R China
2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China
Recommended Citation
GB/T 7714
Chen, Shuo,Liu, Tianfu,Olanrele, Samson O.,et al. Boosting electrocatalytic activity for CO2 reduction on nitrogen-doped carbon catalysts by co-doping with phosphorus[J]. JOURNAL OF ENERGY CHEMISTRY,2021,54:143-150.
APA Chen, Shuo.,Liu, Tianfu.,Olanrele, Samson O..,Lian, Zan.,Si, Chaowei.,...&Li, Bo.(2021).Boosting electrocatalytic activity for CO2 reduction on nitrogen-doped carbon catalysts by co-doping with phosphorus.JOURNAL OF ENERGY CHEMISTRY,54,143-150.
MLA Chen, Shuo,et al."Boosting electrocatalytic activity for CO2 reduction on nitrogen-doped carbon catalysts by co-doping with phosphorus".JOURNAL OF ENERGY CHEMISTRY 54(2021):143-150.
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