Synergizing Electron and Heat Flows in Photocatalyst for Direct Conversion of Captured CO2

Choi, Chungseok; Zhao, Fengyi; Hart, James L.; Gao, Yuanzuo; Menges, Fabian; Rooney, Conor L.; Harmon, Nia J.; Shang, Bo; Xu, Zihao; Suo, Sa; Sam, Quynh; Cha, Judy J.; Lian, Tianquan; Wang, Hailiang

doi:10.1002/anie.202302152

Synergizing Electron and Heat Flows in Photocatalyst for Direct Conversion of Captured CO₂

Journal Article · Mon Mar 27 04:00:00 EDT 2023 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202302152· OSTI ID:2421786

Choi, Chungseok ^[1]; Zhao, Fengyi ^[2]; Hart, James L. ^[3]; Gao, Yuanzuo ^[4]; Menges, Fabian ^[5]; Rooney, Conor L. ^[4]; Harmon, Nia J. ^[4]; Shang, Bo ^[4]; Xu, Zihao ^[2]; Suo, Sa ^[2]; Sam, Quynh ^[3]; Cha, Judy J. ^[3]; Lian, Tianquan ^[2]; ^[4]

Yale University, New Haven, CT (United States); Yale University, West Haven, CT (United States); OSTI
Emory University, Atlanta, GA (United States)
Cornell University, Ithaca, NY (United States)
Yale University, New Haven, CT (United States); Yale University, West Haven, CT (United States)
Yale University, New Haven, CT (United States)

We report a ternary hybrid photocatalyst architecture with tailored interfaces that boost the utilization of solar energy for photochemical CO₂ reduction by synergizing electron and heat flows in the photocatalyst. The photocatalyst comprises cobalt phthalocyanine (CoPc) molecules assembled on multiwalled carbon nanotubes (CNTs) that are decorated with nearly monodispersed cadmium sulfide quantum dots (CdS QDs). The CdS QDs absorb visible light and generate electron-hole pairs. The CNTs rapidly transfer the photogenerated electrons from CdS to CoPc. The CoPc molecules then selectively reduce CO₂ to CO. Here, the interfacial dynamics and catalytic behavior are clearly revealed by time-resolved and in situ vibrational spectroscopies. In addition to serving as electron highways, the black body property of the CNT component can create local photothermal heating to activate amine-captured CO₂, namely carbamates, for direct photochemical conversion without additional energy input.

View Accepted Manuscript (DOE)

Research Organization:: University of North Carolina, Chapel Hill, NC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); U.S. National Science Foundation (NSF)

Grant/Contract Number:: SC0021173

OSTI ID:: 2421786

Alternate ID(s):: OSTI ID: 1975158

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 23 Vol. 62; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (39)

Visible-Light-Induced Selective CO ₂ Reduction Utilizing a Ruthenium Complex Electrocatalyst Linked to a p-Type Nitrogen-Doped Ta ₂ O ₅ Semiconductor Sato, Shunsuke; Morikawa, Takeshi; Saeki, Shu Angewandte Chemie International Edition, Vol. 49, Issue 30 https://doi.org/10.1002/anie.201000613	journal	June 2010
Visible-Light-Driven CO ₂ Reduction with Carbon Nitride: Enhancing the Activity of Ruthenium Catalysts Kuriki, Ryo; Sekizawa, Keita; Ishitani, Osamu Angewandte Chemie International Edition, Vol. 54, Issue 8 https://doi.org/10.1002/anie.201411170	journal	January 2015
Across the Board: Rui Cao on Electrocatalytic CO ₂ Reduction Cao, Rui ChemSusChem, Vol. 15, Issue 21 https://doi.org/10.1002/cssc.202201788	journal	October 2022
Random walk models of charge transfer and transport in dye sensitized systems Nelson, Jenny; Chandler, Rosemary E. Coordination Chemistry Reviews, Vol. 248, Issue 13-14 https://doi.org/10.1016/j.ccr.2004.04.001	journal	July 2004
Recent advances in CdS-based photocatalysts for CO2 photocatalytic conversion Yang, Kaihua; Yang, Zhongzhu; Zhang, Chang Chemical Engineering Journal, Vol. 418 https://doi.org/10.1016/j.cej.2021.129344	journal	August 2021
Synthesis, characterization and electrochemical properties of tetra 7-oxy-3-biphenylcoumarin substituted metal-free, zinc(II), cobalt(II) and indium(III) phthalocyanines Gök, Asiye; Orman, Efe Baturhan; Salan, Ümit Dyes and Pigments, Vol. 133 https://doi.org/10.1016/j.dyepig.2016.06.002	journal	October 2016
Electrochemical, spectroelectrochemical, and dielectric properties of metallophthalocyanines bearing redox active cobalt and manganese metal centres Uzunmehmetoğlu, Hilal Zengin; Yenilmez, H. Yasemin; Kaya, Kerem Inorganica Chimica Acta, Vol. 459 https://doi.org/10.1016/j.ica.2017.01.017	journal	April 2017
Heterogeneous Molecular Catalysts of Metal Phthalocyanines for Electrochemical CO₂ Reduction Reactions Wu, Yueshen; Liang, Yongye; Wang, Hailiang Accounts of Chemical Research, Vol. 54, Issue 16 https://doi.org/10.1021/acs.accounts.1c00200	journal	August 2021
Quantum Efficiency of Charge Transfer Competing against Nonexponential Processes: The Case of Electron Transfer from CdS Nanorods to Hydrogenase Utterback, James K.; Wilker, Molly B.; Mulder, David W. The Journal of Physical Chemistry C, Vol. 123, Issue 1 https://doi.org/10.1021/acs.jpcc.8b09916	journal	December 2018
Investigation of Cobalt Phthalocyanine at the Solid/Liquid Interface by Electrochemical Tip-Enhanced Raman Spectroscopy Jiang, Song; Chen, Zhu; Chen, Xu The Journal of Physical Chemistry C, Vol. 123, Issue 15 https://doi.org/10.1021/acs.jpcc.9b00513	journal	March 2019
Stand-Alone CdS Nanocrystals for Photocatalytic CO₂ Reduction with High Efficiency and Selectivity Feng, You-Xiang; Wang, Hong-Juan; Wang, Jia-Wei ACS Applied Materials & Interfaces, Vol. 13, Issue 22 https://doi.org/10.1021/acsami.1c03606	journal	May 2021
Boron Carbon Nitride Semiconductors Decorated with CdS Nanoparticles for Photocatalytic Reduction of CO ₂ Zhou, Min; Wang, Sibo; Yang, Pengju ACS Catalysis, Vol. 8, Issue 6 https://doi.org/10.1021/acscatal.8b00104	journal	April 2018
Monolayer Molecular Functionalization Enabled by Acid–Base Interaction for High-Performance Photochemical CO₂ Reduction Shang, Bo; Zhao, Fengyi; Choi, Chungseok ACS Energy Letters, Vol. 7, Issue 7 https://doi.org/10.1021/acsenergylett.2c01147	journal	June 2022
Electrochemical Capture and Release of Carbon Dioxide Rheinhardt, Joseph H.; Singh, Poonam; Tarakeshwar, Pilarisetty ACS Energy Letters, Vol. 2, Issue 2 https://doi.org/10.1021/acsenergylett.6b00608	journal	January 2017
High-Performance Electrochemical CO ₂ Reduction Cells Based on Non-noble Metal Catalysts Lu, Xu; Wu, Yueshen; Yuan, Xiaolei ACS Energy Letters, Vol. 3, Issue 10 https://doi.org/10.1021/acsenergylett.8b01681	journal	September 2018
Ultrafast Charge Separation and Long-Lived Charge Separated State in Photocatalytic CdS–Pt Nanorod Heterostructures Wu, Kaifeng; Zhu, Haiming; Liu, Zheng Journal of the American Chemical Society, Vol. 134, Issue 25 https://doi.org/10.1021/ja303306u	journal	June 2012
Strongly Coupled Inorganic/Nanocarbon Hybrid Materials for Advanced Electrocatalysis Liang, Yongye; Li, Yanguang; Wang, Hailiang Journal of the American Chemical Society, Vol. 135, Issue 6 https://doi.org/10.1021/ja3089923	journal	January 2013
Photoinduced Ultrafast Electron Transfer from CdSe Quantum Dots to Re-bipyridyl Complexes Huang, Jier; Stockwell, Dave; Huang, Zhuangqun Journal of the American Chemical Society, Vol. 130, Issue 17 https://doi.org/10.1021/ja8003683	journal	April 2008
Selective Photocatalytic CO ₂ Reduction in Water through Anchoring of a Molecular Ni Catalyst on CdS Nanocrystals Kuehnel, Moritz F.; Orchard, Katherine L.; Dalle, Kristian E. Journal of the American Chemical Society, Vol. 139, Issue 21 https://doi.org/10.1021/jacs.7b00369	journal	May 2017
Dual Cocatalysts Loaded Type I CdS/ZnS Core/Shell Nanocrystals as Effective and Stable Photocatalysts for H₂ Evolution Huang, Lei; Wang, Xiuli; Yang, Jinhui The Journal of Physical Chemistry C, Vol. 117, Issue 22 https://doi.org/10.1021/jp400010z	journal	May 2013
Exciton Annihilation and Dissociation Dynamics in Group II–V Cd ₃ P ₂ Quantum Dots Wu, Kaifeng; Liu, Zheng; Zhu, Haiming The Journal of Physical Chemistry A, Vol. 117, Issue 29 https://doi.org/10.1021/jp402511m	journal	May 2013
Transient Absorption Spectroscopy of Excitons in an Individual Suspended Metallic Carbon Nanotube Gao, Bo; Hartland, Gregory V.; Huang, Libai The Journal of Physical Chemistry Letters, Vol. 4, Issue 18 https://doi.org/10.1021/jz401497n	journal	August 2013
Highly selective and active CO2 reduction electrocatalysts based on cobalt phthalocyanine/carbon nanotube hybrid structures Zhang, Xing; Wu, Zishan; Zhang, Xiao Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14675	journal	March 2017
Electrochemical upgrade of CO2 from amine capture solution Lee, Geonhui; Li, Yuguang C.; Kim, Ji-Yong Nature Energy, Vol. 6, Issue 1 https://doi.org/10.1038/s41560-020-00735-z	journal	December 2020
Nanoparticle surfactants for kinetically arrested photoactive assemblies to track light-induced electron transfer Sokołowski, Kamil; Huang, Junyang; Földes, Tamás Nature Nanotechnology, Vol. 16, Issue 10 https://doi.org/10.1038/s41565-021-00949-6	journal	September 2021
Reaction mechanisms of aqueous monoethanolamine with carbon dioxide: a combined quantum chemical and molecular dynamics study Hwang, Gyeong S.; Stowe, Haley M.; Paek, Eunsu Physical Chemistry Chemical Physics, Vol. 17, Issue 2 https://doi.org/10.1039/C4CP04518A	journal	January 2015
Photocatalytic and photoelectrocatalytic reduction of CO ₂ using heterogeneous catalysts with controlled nanostructures Xie, Shunji; Zhang, Qinghong; Liu, Guodong Chemical Communications, Vol. 52, Issue 1 https://doi.org/10.1039/C5CC07613G	journal	January 2016
CdS-Based photocatalysts Cheng, Lei; Xiang, Quanjun; Liao, Yulong Energy & Environmental Science, Vol. 11, Issue 6 https://doi.org/10.1039/C7EE03640J	journal	January 2018
Porphyrin-based frameworks for oxygen electrocatalysis and catalytic reduction of carbon dioxide Liang, Zuozhong; Wang, Hong-Yan; Zheng, Haoquan Chemical Society Reviews, Vol. 50, Issue 4 https://doi.org/10.1039/D0CS01482F	journal	January 2021
Strongly coupled inorganic–nano-carbon hybrid materials for energy storage Wang, Hailiang; Dai, Hongjie Chemical Society Reviews, Vol. 42, Issue 7 https://doi.org/10.1039/c2cs35307e	journal	January 2013
A black body absorber from vertically aligned single-walled carbon nanotubes Mizuno, K.; Ishii, J.; Kishida, H. Proceedings of the National Academy of Sciences, Vol. 106, Issue 15 https://doi.org/10.1073/pnas.0900155106	journal	April 2009
Stretched exponential relaxation in molecular and electronic glasses Phillips, J. C. Reports on Progress in Physics, Vol. 59, Issue 9 https://doi.org/10.1088/0034-4885/59/9/003	journal	September 1996
Trap-limited recombination in dye-sensitized nanocrystalline metal oxide electrodes Nelson, Jenny; Haque, Saif A.; Klug, David R. Physical Review B, Vol. 63, Issue 20 https://doi.org/10.1103/PhysRevB.63.205321	journal	May 2001
Ultrafast dynamics in metallic and semiconducting carbon nanotubes Lüer, Larry; Lanzani, Guglielmo; Crochet, Jared Physical Review B, Vol. 80, Issue 20 https://doi.org/10.1103/PhysRevB.80.205411	journal	November 2009
Ultrafast luminescence kinetics of metallic single-walled carbon nanotubes: Possible evidence for excitonic luminescence Koyama, Takeshi; Shimizu, Satoru; Saito, Takeshi Physical Review B, Vol. 85, Issue 4 https://doi.org/10.1103/PhysRevB.85.045428	journal	January 2012
Ultrafast Relaxation of Excited Dirac Fermions in Epitaxial Graphene Using Optical Differential Transmission Spectroscopy Sun, Dong; Wu, Zong-Kwei; Divin, Charles Physical Review Letters, Vol. 101, Issue 15 https://doi.org/10.1103/PhysRevLett.101.157402	journal	October 2008
In Vivo Imaging of Quantum Dots Encapsulated in Phospholipid Micelles Dubertret, B. Science, Vol. 298, Issue 5599 https://doi.org/10.1126/science.1077194	journal	November 2002
Carbon Capture and Storage: How Green Can Black Be? Haszeldine, R. S. Science, Vol. 325, Issue 5948 https://doi.org/10.1126/science.1172246	journal	September 2009
Amine Scrubbing for CO2 Capture Rochelle, G. T. Science, Vol. 325, Issue 5948 https://doi.org/10.1126/science.1176731	journal	September 2009

Similar Records

Synergizing Electron and Heat Flows in Photocatalyst for Direct Conversion of Captured CO ₂

Journal Article · Wed Apr 26 00:00:00 EDT 2023 · Angewandte Chemie · OSTI ID:1975297

Strain enhances the activity of molecular electrocatalysts via carbon nanotube supports

Journal Article · Mon Aug 14 00:00:00 EDT 2023 · Nature Catalysis · OSTI ID:2421863

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Chemistry

Synergizing Electron and Heat Flows in Photocatalyst for Direct Conversion of Captured CO2

Citation Formats

References (39)

Similar Records

Related Subjects

Synergizing Electron and Heat Flows in Photocatalyst for Direct Conversion of Captured CO₂