Colloidal silver diphosphide (AgP2) nanocrystals as low overpotential catalysts for CO2 reduction to tunable syngas

Li, Hui; Wen, Peng; Itanze, Dominique S.; Hood, Zachary D.; Ma, Xiao; Kim, Michael; Adhikari, Shiba; Lu, Chang; Dun, Chaochao; Chi, Miaofang; Qiu, Yejun; Geyer, Scott M.

doi:10.1038/s41467-019-13388-8

Title: Colloidal silver diphosphide (AgP₂) nanocrystals as low overpotential catalysts for CO₂ reduction to tunable syngas

Journal Article · 16 December 2019 · Nature Communications

DOI: https://doi.org/10.1038/s41467-019-13388-8 · OSTI ID:1624219

Li, Hui ^[1]; Wen, Peng ^[2]; Itanze, Dominique S. ^[1];

^[3];

^[1]; Kim, Michael ^[1]; Adhikari, Shiba ^[4]; Lu, Chang ^[1]; Dun, Chaochao ^[5];

^[6]; Qiu, Yejun ^[2];

^[1]

Wake Forest Univ., Winston-Salem, NC (United States). Dept. of Chemistry
Harbin Inst. of Technology (China). School of Materials Science and Engineering, Shenzhen Engineering Lab of Flexible Transparent Conductive Films
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Univ. of Notre Dame, IN (United States). Dept. of Aerospace and Mechanical Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Production of syngas with tunable CO/H₂ ratio from renewable resources is an ideal way to provide a carbon-neutral feedstock for liquid fuel production. Ag is a benchmark electrocatalysts for CO₂-to-CO conversion but high overpotential limits the efficiency. We synthesize AgP₂ nanocrystals (NCs) with a greater than 3-fold reduction in overpotential for electrochemical CO₂-to-CO reduction compared to Ag and greatly enhanced stability. Density functional theory calculations reveal a significant energy barrier decrease in the formate intermediate formation step. In situ X-ray absorption spectroscopy (XAS) shows that a maximum Faradaic efficiency is achieved at an average silver valence state of +1.08 in AgP₂ NCs. A photocathode consisting of a n⁺p-Si wafer coated with ultrathin Al₂O₃ and AgP₂ NCs achieves an onset potential of 0.2 V vs. RHE for CO production and a partial photocurrent density for CO at –0.11 V vs. RHE (j_{–0.11, CO}) of –3.2 mA cm^–2.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC), Engineering & Technology; Wake Forest University; Shenzhen Bureau of Science, Technology and Innovation Commission

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1624219

Journal Information:: Nature Communications, Vol. 10, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 294 works

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Title: Colloidal silver diphosphide (AgP2) nanocrystals as low overpotential catalysts for CO2 reduction to tunable syngas

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