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Jeong, Hu Young
UCRF Electron Microscopy group
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Synthetic multiscale design of nanostructured Ni single atom catalyst for superior CO2 electroreduction

Author(s)
Jeong, Gyoung HwaTan, Ying ChuanSong, Jun TaeLee, Gil-YongLee, Ho JinLim, JaewoongJeong, Hu YoungWon, SomiOh, JihunKim, Sang Ouk
Issued Date
2021-12
DOI
10.1016/j.cej.2021.131063
URI
https://scholarworks.unist.ac.kr/handle/201301/58455
Citation
CHEMICAL ENGINEERING JOURNAL, v.426, pp.131063
Abstract
Rational design of nanoscale structures can greatly strengthen heterogeneous catalysis with the maximal utilization of active sites. Single atom catalysts (SACs) are recently emerging but a systematic design of nanostructured SAC has rarely been demonstrated yet. Here, distinct architectural structure-dependence of electrochemical CO2 reduction (CO2RR) on Ni-based SACs is presented. Starting from Ni-imidazolate coordination polymers (Ni-Im) and their supported counterparts with a carbon nanotube (CNT) and a zeolite imidazolate framework (ZIF-8), the respective derivatives, i.e. Ni-SAC, Ni-SAC-CNT, and Ni-SAC-ZIF8, are obtained after pyrolysis. The presence of substrates ultimately results in large surface porous N-doped carbon nanostructures, which facilitate the diffusion of etchants to remove undesired Ni nanoparticles effectively. The dense Ni single atomic sites contained within the nanostructure are easily accessible to CO2 reactants during CO2RR, thus promoting high utilization of active sites even at large current densities. Electro-conductive CNT substrates mediate fluent charge transfer and stimulates the intrinsic activity of catalytic sites. Consequently, operating at 400 mA cm−2, Ni-SAC-CNT attains a high faradaic efficiency of 99% toward CO at a low overpotential of 0.24 V, equivalent to a record cathodic energetic efficiency and turnover frequency of 83.4% and 439,000 h−1, respectively.
Publisher
ELSEVIER SCIENCE SA
ISSN
1385-8947
Keyword (Author)
Single atom catalystCO2 reductionCarbon nanostructureElectrochemistry
Keyword
METAL-ORGANIC FRAMEWORKSELECTROCHEMICAL REDUCTIONEFFICIENT CO2ELECTROLYSISCONVERSIONGASALKALINITYSITES

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