Controlled one‐pot synthesis of nickel single atoms embedded in carbon nanotube and graphene supports with high loading

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dc.contributor.authorZhao, Sen_AU
dc.contributor.authorWang, Ten_AU
dc.contributor.authorZhou, Gen_AU
dc.contributor.authorZhang, Len_AU
dc.contributor.authorLin, Cen_AU
dc.contributor.authorVeder, JPen_AU
dc.contributor.authorJohannessen, Ben_AU
dc.contributor.authorSaunders, Men_AU
dc.contributor.authorYin, Len_AU
dc.contributor.authorLiu, Cen_AU
dc.contributor.authorDe Marco, Ren_AU
dc.contributor.authorYang, SZen_AU
dc.contributor.authorZhang, Qen_AU
dc.contributor.authorJiang, SPen_AU
dc.date.accessioned2025-01-09T05:24:06Zen_AU
dc.date.available2025-01-09T05:24:06Zen_AU
dc.date.issued2020-04-09en_AU
dc.date.statistics2024-12-23en_AU
dc.description.abstractSingle‐atom catalysts (SACs) have attracted much attentions due to the advantages of high catalysis efficiency and selectivity. However, the controllable and efficient synthesis of SACs remains a significant challenge. Herein, we report a controlled one‐pot synthesis of nickel single atoms embedded on nitrogen‐doped carbon nanotubes (NiSA−N−CNT) and nitrogen‐doped graphene (NiSA−N−G). The formation of NiSA−N−CNT is due to the solid‐to‐solid rolling up mechanism during the high temperature pyrolysis at 800 °C from the stacked and layered Ni‐doped g‐C3N4, g‐C3N4−Ni structure to a tubular CNT structure. Addition of citric acid introduces an amorphous carbon source on the layered g‐C3N4−Ni and after annealing at the same temperature of 800 °C, instead of formation of NiSA−N−CNT, Ni single atoms embedded in planar graphene type supports, NiSA−N−G were obtained. The density functional theory (DFT) calculation indicates the introduction of amorphous carbon source substantially reduces the structure fluctuation or curvature of layered g‐C3N4‐Ni intermediate products, thus interrupting the solid‐to‐solid rolling process and leading to the formation of planar graphene type supports for Ni single atoms. The as‐synthesized NiSA−N−G with Ni atomic loading of ∼6 wt% catalysts shows a better activity and stability for the CO2 reduction reaction (CO2RR) than NiSA−N−CNT with Ni atomic loading of ∼15 wt% due to the open and exposed Ni single atom active sites in NiSA−N−G. This study demonstrates for the first time the feasibility in the control of the microstructure of carbon supports in the synthesis of SACs. © 1999-2024 John Wiley & Sons, Inc or related companies. All rights reserved.en_AU
dc.description.sponsorshipThis work was supported by the Australian Research Council under Discovery Project Funding Scheme (project number: DP180100568 and DP180100731). This research used resources of the National Energy Research Scientific Computing Center; a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant number ACI-1053575. CL thanks support from the National Natural Science Foundation of China (No. 51521091). The authors acknowledge the facilities, and the scientific and technical assistance of the National Imaging Facility at the Centre for Microscopy, Characterization & Analysis, the University of Western Australia, and the WA X-Ray Surface Analysis Facility, funded by an Australian Research Council LIEF grant (LE120100026). The technical support and scientific advice provided by B. Cowie and L. Thompsen regarding NEXAFS measurements are acknowledged. XAS measurements were performed on the soft X-ray and XAS beamlines of the Australian Synchrotron of ANSTO, Victoria, Australia.en_AU
dc.identifier.articlenumber202000223en_AU
dc.identifier.citationZhao, S., Wang, T., Zhou, G., Zhang, L., Lin, C., Veder, J.-P., Johannessen, B., Saunders, M., Yin, L., Liu, C., De Marco, R., Yang, S.-Z., Zhang, Q., & Jiang, S. P. (2020). Controlled one-pot synthesis of nickel single atoms embedded in carbon nanotube and graphene supports with high loading. ChemNanoMat, 6(7), 1063-1074. doi:10.1002/cnma.202000223en_AU
dc.identifier.issn2199-692Xen_AU
dc.identifier.issue7en_AU
dc.identifier.journaltitleChemNanoMaten_AU
dc.identifier.pagination1063-1074en_AU
dc.identifier.urihttps://doi.org/10.1002/cnma.202000223en_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/15872en_AU
dc.identifier.volume6en_AU
dc.languageEnglishen_AU
dc.language.isoenen_AU
dc.publisherWileyen_AU
dc.subjectSynthesisen_AU
dc.subjectNickelen_AU
dc.subjectAtomsen_AU
dc.subjectCarbon nanotubesen_AU
dc.subjectGrapheneen_AU
dc.subjectNitrogenen_AU
dc.subjectCatalystsen_AU
dc.subjectDoped materialsen_AU
dc.subjectCarbonen_AU
dc.titleControlled one‐pot synthesis of nickel single atoms embedded in carbon nanotube and graphene supports with high loadingen_AU
dc.typeJournal Articleen_AU
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