Zhengyuan Li¹, Peng Wang², Xiang Lyu³, Vamsi Krishna Reddy Kondapalli⁴, Shuting Xiang⁵, Juan D. Jimenez⁶, Lu Ma⁷, Takeshi Ito¹, Tianyu Zhang¹, Jithu Raj¹, Yanbo Fang⁴, Yaocai Bai³, Jianlin Li³, Alexey Serov³, Vesselin Shanov^1,4, Anatoly I. Frenkel^5,6, Sanjaya D. Senanayake⁶, Yang Shize^8*, Thomas Senftle^2*, Jingjie Wu^1*

1 Department of Chemical and Environmental Engineering, University of Cincinnati, Cincinnati, OH 45221, USA

2 Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX 77005, USA

3 Electrification and Energy Infrastructures Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA

4 Department of Mechanical and Materials Engineering, University of Cincinnati, Cincinnati, OH 45221, USA

5 Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, NY 11794, USA

6 Chemistry Division, Brookhaven National Laboratory, Upton, NY 11973, USA

7 National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY 11971, USA

8 Eyring Materials Center, Arizona State University, Tempe, AZ 85287, USA

* Corresponding authors emails: shize.yang@asu.edu, tsenftle@rice.edu, jingjie.wu@uc.edu

DOI10.24435/materialscloud:4b-cf [version v1]

Publication date: Nov 30, 2023

How to cite this record

Zhengyuan Li, Peng Wang, Xiang Lyu, Vamsi Krishna Reddy Kondapalli, Shuting Xiang, Juan D. Jimenez, Lu Ma, Takeshi Ito, Tianyu Zhang, Jithu Raj, Yanbo Fang, Yaocai Bai, Jianlin Li, Alexey Serov, Vesselin Shanov, Anatoly I. Frenkel, Sanjaya D. Senanayake, Yang Shize, Thomas Senftle, Jingjie Wu, Directing CO₂ electroreduction pathways for selective C₂ product formation using single-site doped Cu catalysts, Materials Cloud Archive 2023.186 (2023), https://doi.org/10.24435/materialscloud:4b-cf

Description

This dataset includes all the atomic coordinates of the optimized computational models from electronic structure calculations reported in the manuscript. In this work, we highlight that single-site noble metal dopants on the Cu surface can influence C–O bond dissociation in a key selectivity-determining intermediate (e.g., oxygen-bound *CH₂CHO), which in turn direct the post-C–C coupling pathways to ethylene versus ethanol. Combining theoretical and experimental analyses, we demonstrate that the favorability of C–O bond scission is controlled by the oxygen affinity of the metal dopant on the Cu catalyst. We find that the selectivity ratio of ethylene-to-ethanol displays a volcano relationship with respect to the oxygen binding strength on the doped surfaces.

Materials Cloud sections using this data

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File name	Size	Description
uploads.zip MD5md5:3ce982e3a7c723ae1054b5e2dc3206eb	95.7 KiB	All relaxed structures in format of POSCAR/CONTCAR.

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Keywords

CO2 electroreduction Single-site doped catalysts Selectivity