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

Abstract

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.

Authors:
 [1];  [2];  [1]; ORCiD logo [3]; ORCiD logo [1];  [1];  [4];  [1];  [5]; ORCiD logo [6];  [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Wake Forest Univ., Winston-Salem, NC (United States). Dept. of Chemistry
  2. Harbin Inst. of Technology (China). School of Materials Science and Engineering, Shenzhen Engineering Lab of Flexible Transparent Conductive Films
  3. 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
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  5. Univ. of Notre Dame, IN (United States). Dept. of Aerospace and Mechanical Engineering
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC), Engineering & Technology; Wake Forest University; Shenzhen Bureau of Science, Technology and Innovation Commission
OSTI Identifier:
1624219
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Science & technology - other topics; Carbon capture and storage; Electrocatalysis; Heterogeneous catalysis; Nanoparticles

Citation Formats

Li, Hui, Wen, Peng, Itanze, Dominique S., Hood, Zachary D., Ma, Xiao, Kim, Michael, Adhikari, Shiba, Lu, Chang, Dun, Chaochao, Chi, Miaofang, Qiu, Yejun, and Geyer, Scott M. Colloidal silver diphosphide (AgP2) nanocrystals as low overpotential catalysts for CO2 reduction to tunable syngas. United States: N. p., 2019. Web. doi:10.1038/s41467-019-13388-8.
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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. Colloidal silver diphosphide (AgP2) nanocrystals as low overpotential catalysts for CO2 reduction to tunable syngas. United States. https://doi.org/10.1038/s41467-019-13388-8
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Li, Hui, Wen, Peng, Itanze, Dominique S., Hood, Zachary D., Ma, Xiao, Kim, Michael, Adhikari, Shiba, Lu, Chang, Dun, Chaochao, Chi, Miaofang, Qiu, Yejun, and Geyer, Scott M. Mon . "Colloidal silver diphosphide (AgP2) nanocrystals as low overpotential catalysts for CO2 reduction to tunable syngas". United States. https://doi.org/10.1038/s41467-019-13388-8. https://www.osti.gov/servlets/purl/1624219.
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@article{osti_1624219,
title = {Colloidal silver diphosphide (AgP2) nanocrystals as low overpotential catalysts for CO2 reduction to tunable syngas},
author = {Li, Hui and Wen, Peng and Itanze, Dominique S. and Hood, Zachary D. and Ma, Xiao and Kim, Michael and Adhikari, Shiba and Lu, Chang and Dun, Chaochao and Chi, Miaofang and Qiu, Yejun and Geyer, Scott M.},
abstractNote = {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.},
doi = {10.1038/s41467-019-13388-8},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {12}
}
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Works referenced in this record:

Inherent Size Effects on XANES of Nanometer Metal Clusters: Size-Selected Platinum Clusters on Silica
journal, December 2016

  • Dai, Yang; Gorey, Timothy J.; Anderson, Scott L.
  • The Journal of Physical Chemistry C, Vol. 121, Issue 1
  • DOI: 10.1021/acs.jpcc.6b10167

Tunable Syngas Production from CO 2 and H 2 O in an Aqueous Photoelectrochemical Cell
journal, October 2016

  • Chu, Sheng; Fan, Shizhao; Wang, Yongjie
  • Angewandte Chemie International Edition, Vol. 55, Issue 46
  • DOI: 10.1002/anie.201606424

Role of non-metallic atoms in enhancing the catalytic activity of nickel-based compounds for hydrogen evolution reaction
journal, January 2018

  • Zheng, Xingqun; Peng, Lishan; Li, Li
  • Chemical Science, Vol. 9, Issue 7
  • DOI: 10.1039/C7SC04851C

Nanostructured transition metal dichalcogenide electrocatalysts for CO 2 reduction in ionic liquid
journal, July 2016

Hydrogen-evolution characteristics of Ni–Mo-coated, radial junction, n+p-silicon microwire array photocathodes
journal, January 2012

  • Warren, Emily L.; McKone, James R.; Atwater, Harry A.
  • Energy & Environmental Science, Vol. 5, Issue 11
  • DOI: 10.1039/c2ee23192a

Unraveling Charge Transfer in CoFe Prussian Blue Modified BiVO 4 Photoanodes
journal, December 2018

Low resistance silver contacts to indium phosphide: Electrical and metallurgical considerations
journal, March 1993

  • Weizer, Victor G.; Fatemi, Navid S.
  • Journal of Applied Physics, Vol. 73, Issue 5
  • DOI: 10.1063/1.353113

Carbon Dioxide Electroreduction into Syngas Boosted by a Partially Delocalized Charge in Molybdenum Sulfide Selenide Alloy Monolayers
journal, June 2017

  • Xu, Jiaqi; Li, Xiaodong; Liu, Wei
  • Angewandte Chemie International Edition, Vol. 56, Issue 31
  • DOI: 10.1002/anie.201704928

A p-Si/NiCoSe x core/shell nanopillar array photocathode for enhanced photoelectrochemical hydrogen production
journal, January 2016

  • Zhang, Hongxiu; Ding, Qi; He, Denghong
  • Energy & Environmental Science, Vol. 9, Issue 10
  • DOI: 10.1039/C6EE02215D

Tuning of CO 2 Reduction Selectivity on Metal Electrocatalysts
journal, September 2017

Nanoporous Au Thin Films on Si Photoelectrodes for Selective and Efficient Photoelectrochemical CO 2 Reduction
journal, October 2016

  • Song, Jun Tae; Ryoo, Hyewon; Cho, Minhyung
  • Advanced Energy Materials, Vol. 7, Issue 3
  • DOI: 10.1002/aenm.201601103

Recent Trends and Perspectives in Electrochemical Water Splitting with an Emphasis on Sulfide, Selenide, and Phosphide Catalysts of Fe, Co, and Ni: A Review
journal, November 2016

  • Anantharaj, Sengeni; Ede, Sivasankara Rao; Sakthikumar, Kuppan
  • ACS Catalysis, Vol. 6, Issue 12
  • DOI: 10.1021/acscatal.6b02479

Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts
journal, August 2017

  • Mistry, Hemma; Choi, Yong-Wook; Bagger, Alexander
  • Angewandte Chemie International Edition, Vol. 56, Issue 38
  • DOI: 10.1002/anie.201704613

Insight into Electrochemical CO 2 Reduction on Surface-Molecule-Mediated Ag Nanoparticles
journal, December 2016

  • Kim, Cheonghee; Eom, Taedaehyeong; Jee, Michael Shincheon
  • ACS Catalysis, Vol. 7, Issue 1
  • DOI: 10.1021/acscatal.6b01862

A selective and efficient electrocatalyst for carbon dioxide reduction
journal, January 2014

  • Lu, Qi; Rosen, Jonathan; Zhou, Yang
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4242

Nano-designed semiconductors for electro- and photoelectro-catalytic conversion of carbon dioxide
journal, January 2018

  • Zhang, Lei; Zhao, Zhi-Jian; Wang, Tuo
  • Chemical Society Reviews, Vol. 47, Issue 14
  • DOI: 10.1039/C8CS00016F

Electrochemical reduction of CO 2 to synthesis gas with controlled CO/H 2 ratios
journal, January 2017

  • Sheng, Wenchao; Kattel, Shyam; Yao, Siyu
  • Energy & Environmental Science, Vol. 10, Issue 5
  • DOI: 10.1039/C7EE00071E

Atomic layer-deposited tunnel oxide stabilizes silicon photoanodes for water oxidation
journal, June 2011

  • Chen, Yi Wei; Prange, Jonathan D.; Dühnen, Simon
  • Nature Materials, Vol. 10, Issue 7
  • DOI: 10.1038/nmat3047

Ag–Sn Bimetallic Catalyst with a Core–Shell Structure for CO 2 Reduction
journal, January 2017

  • Luc, Wesley; Collins, Charles; Wang, Siwen
  • Journal of the American Chemical Society, Vol. 139, Issue 5
  • DOI: 10.1021/jacs.6b10435

Increasing carbon utilization in Fischer–Tropsch synthesis using H2-deficient or CO2-rich syngas feeds
journal, February 2010

Amorphous TiO2 coatings stabilize Si, GaAs, and GaP photoanodes for efficient water oxidation
journal, May 2014

Nanoscaled Metal Borides and Phosphides: Recent Developments and Perspectives
journal, June 2013

  • Carenco, Sophie; Portehault, David; Boissière, Cédric
  • Chemical Reviews, Vol. 113, Issue 10, p. 7981-8065
  • DOI: 10.1021/cr400020d

A Co3O4-CDots-C3N4 three component electrocatalyst design concept for efficient and tunable CO2 reduction to syngas
journal, November 2017

Ultrafast Studies of Photoexcited Electron Dynamics in γ- and α-Fe 2 O 3 Semiconductor Nanoparticles
journal, January 1998

  • Cherepy, Nerine J.; Liston, Dorion B.; Lovejoy, Jennifer A.
  • The Journal of Physical Chemistry B, Vol. 102, Issue 5
  • DOI: 10.1021/jp973149e

Understanding Selectivity for the Electrochemical Reduction of Carbon Dioxide to Formic Acid and Carbon Monoxide on Metal Electrodes
journal, June 2017

Metal-Free Artificial Photosynthesis of Carbon Monoxide Using N-Doped ZnTe Nanorod Photocathode Decorated with N-Doped Carbon Electrocatalyst Layer
journal, April 2018

  • Jang, Youn Jeong; Bhatt, Mahesh Datt; Lee, Jaehyuk
  • Advanced Energy Materials, Vol. 8, Issue 20
  • DOI: 10.1002/aenm.201702636

Synthesis, Characterization, and Properties of Metal Phosphide Catalysts for the Hydrogen-Evolution Reaction
journal, August 2016

Aqueous-Solution Route to Zinc Telluride Films for Application to CO 2 Reduction
journal, April 2014

  • Jang, Ji-Wook; Cho, Seungho; Magesh, Ganesan
  • Angewandte Chemie International Edition, Vol. 53, Issue 23
  • DOI: 10.1002/anie.201310461

Engineering Cobalt Phosphide (CoP) Thin Film Catalysts for Enhanced Hydrogen Evolution Activity on Silicon Photocathodes
journal, December 2015

  • Hellstern, Thomas R.; Benck, Jesse D.; Kibsgaard, Jakob
  • Advanced Energy Materials, Vol. 6, Issue 4
  • DOI: 10.1002/aenm.201501758

Photosynthesis of formate from CO 2 and water at 1% energy efficiency via copper iron oxide catalysis
journal, January 2015

  • Kang, Unseock; Choi, Sung Kyu; Ham, Dong Jin
  • Energy & Environmental Science, Vol. 8, Issue 9
  • DOI: 10.1039/C5EE01410G

Time-Resolved Spectroscopy of ZnTe Photocathodes for Solar Fuel Production
journal, September 2017

  • Xiong, Xianqiang; Forster, Mark; Major, Jonathan D.
  • The Journal of Physical Chemistry C, Vol. 121, Issue 40
  • DOI: 10.1021/acs.jpcc.7b06304

Localized dielectric breakdown and antireflection coating in metal–oxide–semiconductor photoelectrodes
journal, November 2016

  • Ji, Li; Hsu, Hsien-Yi; Li, Xiaohan
  • Nature Materials, Vol. 16, Issue 1
  • DOI: 10.1038/nmat4801

Cathodic shift in onset potential of solar oxygen evolution on hematite by 13-group oxide overlayers
journal, January 2011

  • Hisatomi, Takashi; Le Formal, Florian; Cornuz, Maurin
  • Energy & Environmental Science, Vol. 4, Issue 7
  • DOI: 10.1039/c1ee01194d

Sungas Instead of Syngas: Efficient Coproduction of CO and H 2 with a Single Beam of Sunlight
journal, October 2015

Converting Metals into Phosphides  A General Strategy for the Synthesis of Metal Phosphide Nanocrystals
journal, February 2007

  • Henkes, Amanda E.; Vasquez, Yolanda; Schaak, Raymond E.
  • Journal of the American Chemical Society, Vol. 129, Issue 7, p. 1896-1897
  • DOI: 10.1021/ja068502l

Thermodynamic Aspects of Electrocatalytic CO 2 Reduction in Acetonitrile and with an Ionic Liquid as Solvent or Electrolyte
journal, October 2015

Tunable Cu Enrichment Enables Designer Syngas Electrosynthesis from CO 2
journal, June 2017

  • Ross, Michael B.; Dinh, Cao Thang; Li, Yifan
  • Journal of the American Chemical Society, Vol. 139, Issue 27
  • DOI: 10.1021/jacs.7b04892

Electron transfer dynamics in fuel producing photosystems
journal, April 2017

Janus dendrimersomes coassembled from fluorinated, hydrogenated, and hybrid Janus dendrimers as models for cell fusion and fission
journal, August 2017

  • Xiao, Qi; Sherman, Samuel E.; Wilner, Samantha E.
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 34
  • DOI: 10.1073/pnas.1708380114

Computational Screening of Near-Surface Alloys for CO 2 Electroreduction
journal, March 2018

Interfacial engineering of metal-insulator-semiconductor junctions for efficient and stable photoelectrochemical water oxidation
journal, June 2017

  • Digdaya, Ibadillah A.; Adhyaksa, Gede W. P.; Trześniewski, Bartek J.
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15968

Design principles for maximizing photovoltage in metal-oxide-protected water-splitting photoanodes
journal, October 2015

  • Scheuermann, Andrew G.; Lawrence, John P.; Kemp, Kyle W.
  • Nature Materials, Vol. 15, Issue 1
  • DOI: 10.1038/nmat4451

Selective CO production by Au coupled ZnTe/ZnO in the photoelectrochemical CO 2 reduction system
journal, January 2015

  • Jang, Youn Jeong; Jang, Ji-Wook; Lee, Jaehyuk
  • Energy & Environmental Science, Vol. 8, Issue 12
  • DOI: 10.1039/C5EE01445J

Hot Hole Collection and Photoelectrochemical CO 2 Reduction with Plasmonic Au/p-GaN Photocathodes
journal, March 2018

XPS and Ag L3-edge XANES characterization of silver and silver–gold sulfoselenides
journal, May 2018

  • Mikhlin, Yuri L.; Pal'yanova, Galina A.; Tomashevich, Yevgeny V.
  • Journal of Physics and Chemistry of Solids, Vol. 116
  • DOI: 10.1016/j.jpcs.2018.01.047

Recycling of carbon dioxide to methanol and derived products – closing the loop
journal, January 2014

  • Goeppert, Alain; Czaun, Miklos; Jones, John-Paul
  • Chem. Soc. Rev., Vol. 43, Issue 23
  • DOI: 10.1039/C4CS00122B

H2 evolution at Si-based metal–insulator–semiconductor photoelectrodes enhanced by inversion channel charge collection and H spillover
journal, May 2013

  • Esposito, Daniel V.; Levin, Igor; Moffat, Thomas P.
  • Nature Materials, Vol. 12, Issue 6
  • DOI: 10.1038/nmat3626

Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons
journal, July 2018

Enabling Silicon for Solar-Fuel Production
journal, January 2014

  • Sun, Ke; Shen, Shaohua; Liang, Yongqi
  • Chemical Reviews, Vol. 114, Issue 17
  • DOI: 10.1021/cr300459q

Sub-4 nm PtZn Intermetallic Nanoparticles for Enhanced Mass and Specific Activities in Catalytic Electrooxidation Reaction
journal, March 2017

  • Qi, Zhiyuan; Xiao, Chaoxian; Liu, Cong
  • Journal of the American Chemical Society, Vol. 139, Issue 13
  • DOI: 10.1021/jacs.6b12780

Shape-Dependent Electrocatalytic Reduction of CO 2 to CO on Triangular Silver Nanoplates
journal, February 2017

  • Liu, Subiao; Tao, Hongbiao; Zeng, Li
  • Journal of the American Chemical Society, Vol. 139, Issue 6
  • DOI: 10.1021/jacs.6b12103

Photoelectrochemical Hydrogen Evolution Using Si Microwire Arrays
journal, January 2011

  • Boettcher, Shannon W.; Warren, Emily L.; Putnam, Morgan C.
  • Journal of the American Chemical Society, Vol. 133, Issue 5, p. 1216-1219
  • DOI: 10.1021/ja108801m

Directed Assembly of Nanoparticle Catalysts on Nanowire Photoelectrodes for Photoelectrochemical CO 2 Reduction
journal, August 2016

Atomic Structure of Pt 3 Ni Nanoframe Electrocatalysts by in Situ X-ray Absorption Spectroscopy
journal, December 2015

  • Becknell, Nigel; Kang, Yijin; Chen, Chen
  • Journal of the American Chemical Society, Vol. 137, Issue 50
  • DOI: 10.1021/jacs.5b09639

Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide
journal, September 2015

  • Kortlever, Ruud; Shen, Jing; Schouten, Klaas Jan P.
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 20
  • DOI: 10.1021/acs.jpclett.5b01559

Achieving Selective and Efficient Electrocatalytic Activity for CO 2 Reduction Using Immobilized Silver Nanoparticles
journal, October 2015

  • Kim, Cheonghee; Jeon, Hyo Sang; Eom, Taedaehyeong
  • Journal of the American Chemical Society, Vol. 137, Issue 43
  • DOI: 10.1021/jacs.5b06568

Effects of catalyst material and atomic layer deposited TiO2 oxide thickness on the water oxidation performance of metal–insulator–silicon anodes
journal, January 2013

  • Scheuermann, Andrew G.; Prange, Jonathan D.; Gunji, Marika
  • Energy & Environmental Science, Vol. 6, Issue 8
  • DOI: 10.1039/c3ee41178h

Aqueous-Solution Route to Zinc Telluride Films for Application to CO 2 Reduction
journal, April 2014

  • Jang, Ji-Wook; Cho, Seungho; Magesh, Ganesan
  • Angewandte Chemie, Vol. 126, Issue 23
  • DOI: 10.1002/ange.201310461

Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts
journal, August 2017

  • Mistry, Hemma; Choi, Yong-Wook; Bagger, Alexander
  • Angewandte Chemie, Vol. 129, Issue 38
  • DOI: 10.1002/ange.201704613

Converting Metals into Phosphides: A General Strategy for the Synthesis of Metal Phosphide Nanocrystals.
journal, May 2007

  • Henkes, Amanda E.; Vasquez, Yolanda; Schaak, Raymond E.
  • ChemInform, Vol. 38, Issue 18
  • DOI: 10.1002/chin.200718203
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