中文版 | English
Title

Impaired conjugation boosts CO2 electroreduction by Ni(ii) macrocyclic catalysts immobilized on carbon nanotubes

Author
Corresponding AuthorShen, Yong; Wang, Jia-Wei; Ouyang, Gangfeng
Publication Years
2023-02-08
DOI
Source Title
ISSN
2050-7488
EISSN
2050-7496
Volume11Issue:6
Abstract
Metal complexes hybridized with conductive supports are desirable as high-performance catalysts for CO2 electroreduction, while the delicate molecular design to improve both the intrinsic activity of complex and the molecule-support interactions still remains challenging. We here employ a conjugation-tuning strategy by comparison between Ni(ii) octabutoxyphthalocyanine and Ni(ii) octabutoxynaphthalocyanine on multi-walled carbon nanotubes (NiPc-B@CNT and NiNc-B@CNT) in aqueous electrocatalytic CO2 reduction, respectively. In contrast to the conventional promotive effects from extended conjugation, the impaired conjugation in the Ni(ii) macrocycles unusually boosts both activity and molecule-support affinity. These merits can be attributed to the favored electronic effects and the higher flexibility of long alkyl chains both arising from the absent extended benzene ring in NiPc-B. Consequently, NiPc-B@CNT exhibits much higher faradaic efficiencies for CO production (FECO >= 94% among -0.79 to -1.09 V vs. RHE) than NiNc-B@CNT (FECO < 20%) in an H-cell configuration. The use of a gas-diffusion electrode further raises the electrocatalytic performances of NiPc-B@CNT under 1 atm CO2 (FECO asymptotic to 100% at -0.15 A cm(-2)) or simulated flue gas (10% CO2, FECO &asymptotic to 80% at -0.1 A cm(-2)), respectively.
URL[Source Record]
Indexed By
Language
English
SUSTech Authorship
Others
Funding Project
National Natural Science Foundation of China["21737006","22076222","22036003"] ; Natural Science Foundation of Guangdong Province[2021A1515010068] ; Guangdong Basic and Applied Basic Research Foundation["2020A1515110017","2021A1515012033"] ; Ramon y Cajal grant through Instituto de Ciencia de Materiales de Madrid, Consejo Superior de Investigaciones Cientificas[RYC2020-029863-I] ; Spanish Ministerio de Ciencia, Innovacion y Universidades grant[PID2019-111086RA-I00]
WOS Research Area
Chemistry ; Energy & Fuels ; Materials Science
WOS Subject
Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS Accession No
WOS:000922016400001
Publisher
Data Source
Web of Science
Citation statistics
Cited Times [WOS]:3
Document TypeJournal Article
Identifierhttp://kc.sustech.edu.cn/handle/2SGJ60CL/475025
DepartmentDepartment of Chemistry
Affiliation
1.Sun Yat sen Univ, Sch Chem, KLGHEI Environm & Energy Chem, Guangzhou 510275, Peoples R China
2.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
3.Consejo Super Invest Cient CS ICMM, Inst Ciencia Mat Madrid, Sor Juana Ines Cruz 3, Madrid 28049, Spain
4.Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Sch Sci, Dept Chem, 18 Shilongshan Rd, Hangzhou 310024, Peoples R China
5.Barcelona Inst Sci & Technol BIST, Inst Chem Res Catalonia ICIQ, Avinguda Paisos Catalans 16, Tarragona 43007, Spain
6.Tianjin Univ Technol, Sch Mat Sci & Engn, Inst New Energy Mat & Low Carbon Technol, Tianjin 300384, Peoples R China
7.Zhengzhou Univ, Chem Coll, Ctr Adv Anal & Gene Sequencing, Zhengzhou 450001, Peoples R China
8.China Natl Analyt Ctr Guangzhou, Guangdong Inst Anal, Guangdong Prov Key Lab Emergency Test Dangerous Ch, Guangzhou 510070, Peoples R China
Recommended Citation
GB/T 7714
Huang, Yanjun,Dai, Hao,Moonshiram, Dooshaye,et al. Impaired conjugation boosts CO2 electroreduction by Ni(ii) macrocyclic catalysts immobilized on carbon nanotubes[J]. Journal of Materials Chemistry A,2023,11(6).
APA
Huang, Yanjun.,Dai, Hao.,Moonshiram, Dooshaye.,Li, Zhuofeng.,Luo, Zhi-Mei.,...&Ouyang, Gangfeng.(2023).Impaired conjugation boosts CO2 electroreduction by Ni(ii) macrocyclic catalysts immobilized on carbon nanotubes.Journal of Materials Chemistry A,11(6).
MLA
Huang, Yanjun,et al."Impaired conjugation boosts CO2 electroreduction by Ni(ii) macrocyclic catalysts immobilized on carbon nanotubes".Journal of Materials Chemistry A 11.6(2023).
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