Electroreduction of carbon dioxide into selective hydrocarbon using isomorphic atomic substitution in stable copper oxide

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dc.contributor.author Nellaiappan, Subramanian
dc.contributor.author Kumar, Ritesh
dc.contributor.author Shivakumara, C.
dc.contributor.author Irusta, Silvia
dc.contributor.author Hachtel, Jordan A.
dc.contributor.author Idrobo, Juan-Carlos
dc.contributor.author Singh, Abhishek Kumar
dc.contributor.author Tiwary, Chandra Sekhar
dc.contributor.author Sharma, Sudhanshu
dc.date.accessioned 2019-12-30T10:09:24Z
dc.date.available 2019-12-30T10:09:24Z
dc.date.issued 2019-11
dc.identifier.citation Nellaiappan, Subramanian; Kumar, Ritesh; Shivakumara, C.; Irusta, Silvia; Hachtel, Jordan A.; Idrobo, Juan-Carlos; Singh, Abhishek Kumar; Tiwary, Chandra Sekhar and Sharma, Sudhanshu, "Electroreduction of carbon dioxide into selective hydrocarbon using isomorphic atomic substitution in stable copper oxide", ACS Sustainable Chemistry & Engineering, DOI: 10.1021/acssuschemeng.9b05087, Nov. 2019. en_US
dc.identifier.issn 2168-0485
dc.identifier.uri https://doi.org/10.1021/acssuschemeng.9b05087
dc.identifier.uri https://repository.iitgn.ac.in/handle/123456789/5049
dc.description.abstract The conversion of carbon dioxide into selective hydrocarbons is vital for green energy generation. Due to the chemical instability and lower activity, environmentally stable transition metal oxides (e.g., CuO) are unpopular for CO2 electroreduction catalysis. Here, we demonstrate substitution of Cu with an isomorphic atom, i.e., Ni, in CuO and utilize it for improving the hydrocarbon selectivity by 4 times as compared to that of pristine CuO. Hydrocarbon formation is achieved at the lowest possible applied potential (?0.2 V, reversible hydrogen electrode). This gives the overpotential of about 0.37 V for methane and 0.28 V for ethylene, the lowest ever reported. Employing the ionic interaction between Ni and Cu, this catalyst suppresses the hydrogen evolution reaction to improve the hydrocarbon selectivity prominently. It is observed that current normalized by the Brunauer�Emmett�Teller surface area gives 15�20 times enhancement in the case of Ni-substituted CuO compared to undoped CuO. The in situ experiments indicate that Ni-doped CuO prefers CO pathways compared to formate, resulting into high hydrocarbon selectivity. The experimental observation is further supported by density functional theory studies, which reveal that the Ni-doped CuO catalyst has a higher limiting potential for CO2 electroreduction to CH4 due to the stabilization of the CH2O intermediate on the Cu0.9375Ni0.0625O surface rather than the CHO intermediate, in comparison to the pristine CuO surface.
dc.description.statementofresponsibility by Subramanian Nellaiappan, Ritesh Kumar, C. Shivakumara, Silvia Irusta, Jordan A. Hachtel, Juan-Carlos Idrobo, Abhishek Kumar Singh, Chandra Sekhar Tiwary and Sudhanshu Sharma
dc.language.iso en_US en_US
dc.publisher American Chemical Society en_US
dc.subject redox-active catalyst en_US
dc.subject isomorphic atomic substitution en_US
dc.subject nickel-substituted copper oxide en_US
dc.subject CO2 electroreduction en_US
dc.subject FTIR en_US
dc.subject DFT studies en_US
dc.title Electroreduction of carbon dioxide into selective hydrocarbon using isomorphic atomic substitution in stable copper oxide en_US
dc.type Article en_US
dc.relation.journal ACS Sustainable Chemistry & Engineering


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