Vapor-Fed Electrolyzers for Carbon Dioxide Reduction Using Tandem Electrocatalysts: Cuprous Oxide Coupled with Nickel-Coordinated Nitrogen-Doped Carbon

Yi-Rung Lin; Dong Un Lee; Shunquan TanDavid M. KoshyTiras Y. LinLei WangDaniel CorralJaime E. Aviles AcostaJose A. Zamora ZeledonVictor A. BeckSarah E. BakerEric B. DuossChristopher HahnThomas F. Jaramillo

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Vapor-Fed Electrolyzers for Carbon Dioxide Reduction Using Tandem Electrocatalysts: Cuprous Oxide Coupled with Nickel-Coordinated Nitrogen-Doped Carbon

机译：Vapor-Fed Electrolyzers for Carbon Dioxide Reduction Using Tandem Electrocatalysts: Cuprous Oxide Coupled with Nickel-Coordinated Nitrogen-Doped Carbon

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Ethylene is particularly attractive due to its major importance as a feedstockfor various applications including the polymer industry. As such, catalyst andelectrolyzer developments are crucial to achieve industrially relevant ethyleneproduction and efficiency levels. Here, a tandem electrocatalyst composed ofcopper nanocubes and nickel-coordinated nitrogen-doped carbon (NiNC) ispresented, which is integrated into gas diffusion electrodes (GDEs) for directconversion of vapor-fed CO_2 into ethylene. Evaluation of tandem GDEs in thevapor-fed flow electrolyzer shows significantly increased ethylene selectivityin terms of faradaic efficiency and C_2H_4/CO ratio compared to a non-tandemcopper GDE. The enhancements are attributed to the increased local COavailability near the copper surface via effective CO_2 to CO conversion onneighboring NiNC. The experimental results are validated by 3D resolvedcontinuum simulations, which show increased flux of higher-order productswith the added CO flux from NiNC. The practical viability of Cu/NiNCcatalyst is further evaluated in a membrane electrode assembly electrolyzer,achieving 40 FE toward ethylene at 150 mA cm~(?2) and 3.2 V. These findingshighlight the high selectivity and formation rate of ethylene achievedby successful device integration of the Cu/NiNC catalyst, demonstrating thepotential for implementation in large-scale sustainable CO_2 electrolyzers.

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《Advanced functional materials》 |2022年第28期|2113252.1-2113252.10|共10页
作者
Yi-Rung Lin; Dong Un Lee; Shunquan TanDavid M. KoshyTiras Y. LinLei WangDaniel CorralJaime E. Aviles AcostaJose A. Zamora ZeledonVictor A. BeckSarah E. BakerEric B. DuossChristopher HahnThomas F. Jaramillo;
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Materials Science DivisionLawrence Livermore National LaboratoryLivermore, CA 94550, USA;

Materials Engineering DivisionLawrence Livermore National LaboratoryLivermore, CA 94550, USA;

Materials Science DivisionLawrence Livermore National LaboratoryLivermore, CA 94550, USA, SUNCAT Center for Interface Science and CatalysisSLAC National Accelerator LaboratoryMenlo Park, CA 94025, USASUNCAT Center for Interface Science and CatalysisDepartment of Chemical EngineeringStanford UniversityStanford, CA 94305, USA, SUNCAT Center for Interface Science and CatalysisSLAC National Accelerator LaboratoryMenlo Park, CA 94025, USASUNCAT Center for Interface Science and CatalysisDepartment of Chemical EngineeringStanford UniversityStanford, CA 94305, USAComputational Engineering DivisionLawrence Livermore National LaboratoryLivermore, CA 94550, USA;

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CO_2 reduction; electrocatalysis; ethylene; membrane electrode assemblies (MEA); selectivity; tandem catalysis;

Vapor-Fed Electrolyzers for Carbon Dioxide Reduction Using Tandem Electrocatalysts: Cuprous Oxide Coupled with Nickel-Coordinated Nitrogen-Doped Carbon

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