Synthetic Multiscale Design of Nanostructured Ni Single Atom Catalyst for Superior CO2 Electroreduction

Synthetic Multiscale Design of Nanostructured Ni Single Atom Catalyst for Superior CO2 Electroreduction

Chemical Engineering Journal

10.1016/j.cej.2021.131063

http://dx.doi.org/10.1016/j.cej.2021.131063

Gyoung Hwa Jeong, Ying Chuan Tan, Jun Tae Song, Gil-Yong Lee, Ho Jin Lee, Jaewoong Lim, Hu Young Jeong, Somi Won, Jihun Oh, Sang Ouk Kim

Industrial and Manufacturing Engineering, General Chemistry, General Chemical Engineering, Environmental Chemistry

03 July 2021

Jeong, G.H., Tan, Y.C., Song, J.T., Lee, G.-Y., Lee, H.J., Lim, J., … Ouk Kim, S. (2021). Synthetic Multiscale Design of Nanostructured Ni Single Atom Catalyst for Superior CO2 Electroreduction. Chemical Engineering Journal, 131063. doi:10.1016/j.cej.2021.131063

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

Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0)

This research / project is supported by the Korean Government (Ministry of Science and ICT), National Research Foundation - Creative Materials Discovery Program
Grant Reference no. : NRF-2017M3D1A1040692

This research / project is supported by the Korean Government (Ministry of Science and ICT), National Research Foundation - Carbon to X Project
Grant Reference no. : NRF-2020M3H7A1096388

National Creative Research Initiative (CRI) Center for Multi-Dimensional Directed Nanoscale Assembly - Grant No 2015R1A3A2033061

https://oar.a-star.edu.sg/communities-collections/articles/17805

1385-8947

Institute of Materials Research and Engineering