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Nitrogen-doped carbon black supported synergistic palladium single atoms and nanoparticles for electrocatalytic oxidation of methanol

Zhuang, Lei1,2; Jia, Zhijun1; Wang, Yi1; Zhang, Xiaoming3; Wang, Suli3; Song, Jing1,2; Tian, Liangliang4; Qi, Tao1
2022-06-15
Source PublicationCHEMICAL ENGINEERING JOURNAL
ISSN1385-8947
Volume438Pages:12
AbstractFor commercially viable direct methanol fuel cells, electrocatalysts play a crucial role in motivating the sluggish methanol oxidation reaction (MOR) over anode. Unfortunately, the large-scale applications of current MOR catalysts are hampered by their poor tolerance to poisoning and fast activity degradation. Herein, a unique composite catalyst comprised of partial Pd nanoparticles and partial Pd single atoms (Pd-NPs/Pd-N-x@C) is developed. The as-fabricated catalyst exhibits remarkable activity of 9.45 mA.cm(-2) towards MOR in alkaline solution, which is 7.05 and 3.92 times that of commercial Pd/C and nanoparticle type (Pd-NPs@C) electro-catalysts, respectively. Impressively, the Pd-NPs/Pd-N-x@C shows the highest long-time stability with 90.38% and 89.8% of the initial activity retained after 3600 s chronoamperometry (CA) test and 2000 cycles of cyclic voltammetry (CV) measurements with accelerated durability test (ADT), respectively. Combined with high-angle annular darkfield scanning transmission electron microscopy (HAADF-STEM), X-ray adsorption fine structure (XAFS) spectra and X-ray photoelectron spectroscopy (XPS) analyses, the superior performance of Pd-NPs/Pd-N-x@C can be ascribed to the synergistic effect from the Pd single atoms, N-doped carbon supports and Pd nanoparticles. Notably, the embedded Pd single atoms are liable to transfer electrons to the substrate due to the electronic metal-support interactions (EMSI) and the charge transfer between Pd nanoparticles and carbon supports is suppressed, inducing a weak adsorption strength of poisonous carbonous intermediate species on active Pd nanoparticles and improved poisoning tolerance in MOR process, which is verified by density functional theory (DFT) calculations as well as CO-stripping voltammetry experiments. This work not only con-tributes the first example of a synergistic catalyst between nanoparticles and single atoms for MOR but also deepens the knowledge on the metal-support interaction.
KeywordElectrocatalyst Palladium single atom Palladium nanoparticle Methanol oxidation reaction Electronic structure regulation
DOI10.1016/j.cej.2022.135585
Language英语
WOS KeywordELECTROOXIDATION ; CATALYSTS ; GRAPHENE
Funding ProjectNational Key Research and Development Program of China[2020YFC1909001] ; Strategic Priority Research Program of Chinese Academy of Sciences[XDA21070302] ; National Natural Science Foundation of China[51804291] ; Beijing Natural Science Foundation[2184127] ; Chinese Academy of Sciences[HZ2021013]
WOS Research AreaEngineering
WOS SubjectEngineering, Environmental ; Engineering, Chemical
Funding OrganizationNational Key Research and Development Program of China ; Strategic Priority Research Program of Chinese Academy of Sciences ; National Natural Science Foundation of China ; Beijing Natural Science Foundation ; Chinese Academy of Sciences
WOS IDWOS:000779697700002
PublisherELSEVIER SCIENCE SA
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/52827
Collection中国科学院过程工程研究所
Corresponding AuthorWang, Yi; Zhang, Xiaoming; Qi, Tao
Affiliation1.Chinese Acad Sci, Natl Engn Res Ctr Green Recycling Strateg Met Res, Inst Proc Engn, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, Div Fuel Cell & Battery, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
4.Chongqing Univ Arts & Sci, Sch Elect Informat & Elect Engn, Chongqing 400000, Peoples R China
Recommended Citation
GB/T 7714
Zhuang, Lei,Jia, Zhijun,Wang, Yi,et al.

Nitrogen-doped carbon black supported synergistic palladium single atoms and nanoparticles for electrocatalytic oxidation of methanol

[J]. CHEMICAL ENGINEERING JOURNAL,2022,438:12.
APA Zhuang, Lei.,Jia, Zhijun.,Wang, Yi.,Zhang, Xiaoming.,Wang, Suli.,...&Qi, Tao.(2022).

Nitrogen-doped carbon black supported synergistic palladium single atoms and nanoparticles for electrocatalytic oxidation of methanol

.CHEMICAL ENGINEERING JOURNAL,438,12.
MLA Zhuang, Lei,et al."

Nitrogen-doped carbon black supported synergistic palladium single atoms and nanoparticles for electrocatalytic oxidation of methanol

".CHEMICAL ENGINEERING JOURNAL 438(2022):12.
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