Electron shuttle in the MOF derived TiO2/CuO heterojunction boosts light driven hydrogen evolution

Zhang, Yunbo; Hu, Wenhui; Wang, Denan; Reinhart, Benjamin J.; Huang, Jier

doi:10.1039/d0ta12220c

Title: Electron shuttle in the MOF derived TiO₂/CuO heterojunction boosts light driven hydrogen evolution

Abstract

Metal organic frameworks (MOFs) have emerged as a novel template to develop porous photocatalytic materials for solar fuel conversion. In this work, we report the synthesis, charge separation dynamics, and photocatalytic performance of the TiO₂/CuO heterostructure derived from mixed-phase MOFs based on Ti and Cu metal nodes, which demonstrates significantly enhanced catalytic activity for the hydrogen evolution reaction (HER) compared to metal oxides derived from single node MOFs. More importantly, using transient absorption spectroscopy, we identified the specific role each component in the heterostructure plays and unravelled the key intermediate species that is responsible for the exceptional photocatalytic activity of the heterostructure. We found that the HER is initiated with ultrafast electron transfer (<150 fs) from the molecular photosensitizer to the conduction band of TiO₂, where TiO₂ acts as an electron mediator and shuttles the electron to the CuO cocatalyst, facilitating charge separation and ultimately boosting the HER efficiency. Overall, these results not only demonstrate the great potential of using mixed-phase MOFs as templates to synthesize mesoporous heterostructure photocatalysts but also provide important insight into the HER mechanism.

Authors:

Zhang, Yunbo ^[1]; Hu, Wenhui ^[2];

^[2]; Reinhart, Benjamin J. ^[3];

^[2]

Wuyi Univ., Jiangmen (China); Marquette Univ., Milwaukee, WI (United States)
Marquette Univ., Milwaukee, WI (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Publication Date:: Wed Jan 27 00:00:00 EST 2021

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

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

OSTI Identifier:: 1780720

Grant/Contract Number:: AC02-06CH11357; CBET-1706971

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Materials Chemistry. A

Additional Journal Information:: Journal Volume: 9; Journal Issue: 10; Journal ID: ISSN 2050-7488

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; MOF; Metal organic frameworks; hydrogen evolution

Citation Formats


                    Zhang, Yunbo, Hu, Wenhui, Wang, Denan, Reinhart, Benjamin J., and Huang, Jier. Electron shuttle in the MOF derived TiO2/CuO heterojunction boosts light driven hydrogen evolution.  United States: N. p., 2021. 
Web.  doi:10.1039/d0ta12220c.

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                    Zhang, Yunbo, Hu, Wenhui, Wang, Denan, Reinhart, Benjamin J., & Huang, Jier. Electron shuttle in the MOF derived TiO2/CuO heterojunction boosts light driven hydrogen evolution.  United States.  https://doi.org/10.1039/d0ta12220c

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                    Zhang, Yunbo, Hu, Wenhui, Wang, Denan, Reinhart, Benjamin J., and Huang, Jier. Wed .  
"Electron shuttle in the MOF derived TiO2/CuO heterojunction boosts light driven hydrogen evolution".  United States.  https://doi.org/10.1039/d0ta12220c.  https://www.osti.gov/servlets/purl/1780720.

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@article{osti_1780720,

  title        = {Electron shuttle in the MOF derived TiO2/CuO heterojunction boosts light driven hydrogen evolution},

  author       = {Zhang, Yunbo and Hu, Wenhui and Wang, Denan and Reinhart, Benjamin J. and Huang, Jier},

  abstractNote = {Metal organic frameworks (MOFs) have emerged as a novel template to develop porous photocatalytic materials for solar fuel conversion. In this work, we report the synthesis, charge separation dynamics, and photocatalytic performance of the TiO2/CuO heterostructure derived from mixed-phase MOFs based on Ti and Cu metal nodes, which demonstrates significantly enhanced catalytic activity for the hydrogen evolution reaction (HER) compared to metal oxides derived from single node MOFs. More importantly, using transient absorption spectroscopy, we identified the specific role each component in the heterostructure plays and unravelled the key intermediate species that is responsible for the exceptional photocatalytic activity of the heterostructure. We found that the HER is initiated with ultrafast electron transfer (<150 fs) from the molecular photosensitizer to the conduction band of TiO2, where TiO2 acts as an electron mediator and shuttles the electron to the CuO cocatalyst, facilitating charge separation and ultimately boosting the HER efficiency. Overall, these results not only demonstrate the great potential of using mixed-phase MOFs as templates to synthesize mesoporous heterostructure photocatalysts but also provide important insight into the HER mechanism.},

  doi          = {10.1039/d0ta12220c},

  journal      = {Journal of Materials Chemistry. A},

  number       = 10,

  volume       = 9,

  place        = {United States},

  year         = {Wed Jan 27 00:00:00 EST 2021},

  month        = {Wed Jan 27 00:00:00 EST 2021}

}

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Abstract

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Synthesis of Amino-Functionalized Ti-MOF Derived Yolk–Shell and Hollow Heterostructures for Enhanced Photocatalytic Hydrogen Production under Visible Light journal, December 2018

Synthesis and photocatalytic activities of a CuO/TiO 2 composite catalyst using aquatic plants with accumulated copper as a template journal, January 2019

Pd-grafted open metal site copper-benzene-1,4-dicarboxylate metal organic frameworks (Cu-BDC MOF’s) as promising interfacial catalysts for sustainable Suzuki coupling journal, May 2016

Site-Selective Probes of Mixed-Node Metal Organic Frameworks for Photocatalytic Hydrogen Generation journal, December 2019

Binary metal (Ti, Cu) oxyhydroxy–organic (terephthalate) framework: An interface model nanocatalyst for hydrogen purification journal, December 2015

A new family of carbon materials: synthesis of MOF-derived nanoporous carbons and their promising applications journal, January 2013

Metal-Organic-Framework-Derived Hollow N-Doped Porous Carbon with Ultrahigh Concentrations of Single Zn Atoms for Efficient Carbon Dioxide Conversion journal, January 2019

Photochemistry of Ru(bpy)2(dcbpy)2+ on Al2O3 and TiO2 Surfaces. An Insight into the Mechanism of Photosensitization journal, July 1995

Metal–Organic Frameworks in Solid–Gas Phase Catalysis journal, November 2018

Ultrafast Hole Trapping and Relaxation Dynamics in p-Type CuS Nanodisks journal, June 2015

Mesoporous TiO 2 Embedded with a Uniform Distribution of CuO Exhibit Enhanced Charge Separation and Photocatalytic Efficiency journal, December 2017

Quinoxaline synthesis via oxidative cyclization reaction using metal–organic framework Cu(BDC) as an efficient heterogeneous catalyst journal, February 2015

Influence of Hydrothermal Pressure during Crystallization on the Structure and Electron-Conveying Ability of TiO 2 Colloids for Dye-Sensitized Solar Cells journal, August 2010

Dual-Emitting MOF⊃Dye Composite for Ratiometric Temperature Sensing journal, January 2015

Metal-Organic Framework (MOF)-Based Drug/Cargo Delivery and Cancer Therapy journal, March 2017

Mesoporous Cu–Cu 2 O@TiO 2 heterojunction photocatalysts derived from metal–organic frameworks journal, January 2020

Mechanistic Probes of Zeolitic Imidazolate Framework for Photocatalytic Application journal, November 2017

Unravelling the Correlation of Electronic Structure and Carrier Dynamics in CuInS 2 Nanoparticles journal, December 2017

Two-dimensional porous cuprous oxide nanoplatelets derived from metal–organic frameworks (MOFs) for efficient photocatalytic dye degradation under visible light journal, January 2018

From Molecules to Crystal Engineering: Supramolecular Isomerism and Polymorphism in Network Solids journal, June 2001

Metal–Organic Frameworks for Photocatalysis and Photothermal Catalysis journal, December 2018

Single Molecule Photocatalysis on TiO 2 Surfaces: Focus Review journal, September 2019

Incorporation of a [Ru(dcbpy)(bpy) 2 ] 2+ photosensitizer and a Pt(dcbpy)Cl 2 catalyst into metal–organic frameworks for photocatalytic hydrogen evolution from aqueous solution journal, January 2015

MOF-derived nitrogen-doped nanoporous carbon for electroreduction of CO 2 to CO: the calcining temperature effect and the mechanism journal, January 2019

Synthesis and Hydrogen Sorption Properties of Carborane Based Metal−Organic Framework Materials journal, October 2007

MOF Crystal Chemistry Paving the Way to Gas Storage Needs: Aluminum-Based soc -MOF for CH 4 , O 2 , and CO 2 Storage journal, October 2015

Noble-Metal-Free CdS Decorated Porous Ni x Co 1– x O Skeleton Derived from Metal–Organic Framework for Efficient Visible-Light H 2 Production journal, December 2019

Fabrication of functional hollow microspheres constructed from MOF shells: Promising drug delivery systems with high loading capacity and targeted transport journal, November 2016

Functional Porous Coordination Polymers journal, April 2004

Transient Absorption Spectroscopy of Ruthenium and Osmium Polypyridyl Complexes Adsorbed onto Nanocrystalline TiO 2 Photoelectrodes journal, September 2002

Metal–Organic Frameworks as A Tunable Platform for Designing Functional Molecular Materials journal, August 2013

Reaction Mechanism and Activity of WO 3 -Catalyzed Photodegradation of Organic Substances Promoted by a CuO Cocatalyst journal, March 2009

Title: Electron shuttle in the MOF derived TiO₂/CuO heterojunction boosts light driven hydrogen evolution

Double-slit photoelectron interference in strong-field ionization of the neon dimer
journal, January 2019

Dual Cocatalysts in TiO ₂ Photocatalysis
journal, May 2019

Ti and O K edges for titanium oxides by multiple scattering calculations: Comparison to XAS and EELS spectra
journal, April 1997

Precise fabrication of single-atom alloy co-catalyst with optimal charge state for enhanced photocatalysis
journal, September 2020

Synthesis and Structure Characterization of Copper Terephthalate Metal-Organic Frameworks
journal, June 2009

Mesoporous Anatase TiO ₂ Films: Use of Ti K XANES for the Quantification of the Nanocrystalline Character and Substrate Effects in the Photocatalysis Behavior
journal, July 2007

XAS study of TiO 2 -based nanomaterials
journal, July 2015

Photoactive Zeolitic Imidazolate Framework as Intrinsic Heterogeneous Catalysts for Light-Driven Hydrogen Generation
journal, December 2016

Development of MOF-Derived Carbon-Based Nanomaterials for Efficient Catalysis
journal, August 2016

MOF-74 derived porous hybrid metal oxide hollow nanowires for high-performance electrochemical energy storage
journal, January 2018

A New Photoactive Crystalline Highly Porous Titanium(IV) Dicarboxylate
journal, July 2009

Photocatalytic CO2 reduction over metal-organic framework-based materials
journal, June 2020

Atomically Dispersed Metal Sites in MOF-Based Materials for Electrocatalytic and Photocatalytic Energy Conversion
journal, June 2018

Metal–Organic Frameworks and Self-Assembled Supramolecular Coordination Complexes: Comparing and Contrasting the Design, Synthesis, and Functionality of Metal–Organic Materials
journal, November 2012

Metal–organic framework (MOF): a novel sensing platform for biomolecules
journal, January 2013

MOF-derived C-doped ZnO prepared via a two-step calcination for efficient photocatalysis
journal, July 2016

Synergistic Effects of Water and SO ₂ on Degradation of MIL-125 in the Presence of Acid Gases
journal, November 2016

Self-Healing of Molecular Catalyst and Photosensitizer on Metal–Organic Framework: Robust Molecular System for Photocatalytic H ₂ Evolution from Water
journal, July 2016

Introduction to Metal–Organic Frameworks
journal, September 2011

Fundamentals of TiO ₂ Photocatalysis: Concepts, Mechanisms, and Challenges
journal, July 2019

Removal of Ammonia Emissions via Reversible Structural Transformation in M(BDC) (M = Cu, Zn, Cd) Metal–Organic Frameworks
journal, February 2020

Structural and Electronic Properties of Sol−Gel Titanium Oxides Studied by X-ray Absorption Spectroscopy
journal, December 1998

Hydrogen Storage in Microporous Metal-Organic Frameworks
journal, May 2003

Synthesis of Amino-Functionalized Ti-MOF Derived Yolk–Shell and Hollow Heterostructures for Enhanced Photocatalytic Hydrogen Production under Visible Light
journal, December 2018

Synthesis and photocatalytic activities of a CuO/TiO ₂ composite catalyst using aquatic plants with accumulated copper as a template
journal, January 2019

Pd-grafted open metal site copper-benzene-1,4-dicarboxylate metal organic frameworks (Cu-BDC MOF’s) as promising interfacial catalysts for sustainable Suzuki coupling
journal, May 2016

Site-Selective Probes of Mixed-Node Metal Organic Frameworks for Photocatalytic Hydrogen Generation
journal, December 2019

Binary metal (Ti, Cu) oxyhydroxy–organic (terephthalate) framework: An interface model nanocatalyst for hydrogen purification
journal, December 2015

A new family of carbon materials: synthesis of MOF-derived nanoporous carbons and their promising applications
journal, January 2013

Metal-Organic-Framework-Derived Hollow N-Doped Porous Carbon with Ultrahigh Concentrations of Single Zn Atoms for Efficient Carbon Dioxide Conversion
journal, January 2019

Photochemistry of Ru(bpy)2(dcbpy)2+ on Al2O3 and TiO2 Surfaces. An Insight into the Mechanism of Photosensitization
journal, July 1995

Metal–Organic Frameworks in Solid–Gas Phase Catalysis
journal, November 2018

Ultrafast Hole Trapping and Relaxation Dynamics in p-Type CuS Nanodisks
journal, June 2015

Mesoporous TiO ₂ Embedded with a Uniform Distribution of CuO Exhibit Enhanced Charge Separation and Photocatalytic Efficiency
journal, December 2017

Quinoxaline synthesis via oxidative cyclization reaction using metal–organic framework Cu(BDC) as an efficient heterogeneous catalyst
journal, February 2015

Influence of Hydrothermal Pressure during Crystallization on the Structure and Electron-Conveying Ability of TiO ₂ Colloids for Dye-Sensitized Solar Cells
journal, August 2010

Dual-Emitting MOF⊃Dye Composite for Ratiometric Temperature Sensing
journal, January 2015

Metal-Organic Framework (MOF)-Based Drug/Cargo Delivery and Cancer Therapy
journal, March 2017

Mesoporous Cu–Cu ₂ O@TiO ₂ heterojunction photocatalysts derived from metal–organic frameworks
journal, January 2020

Mechanistic Probes of Zeolitic Imidazolate Framework for Photocatalytic Application
journal, November 2017

Unravelling the Correlation of Electronic Structure and Carrier Dynamics in CuInS 2 Nanoparticles
journal, December 2017

Two-dimensional porous cuprous oxide nanoplatelets derived from metal–organic frameworks (MOFs) for efficient photocatalytic dye degradation under visible light
journal, January 2018

From Molecules to Crystal Engineering: Supramolecular Isomerism and Polymorphism in Network Solids
journal, June 2001

Metal–Organic Frameworks for Photocatalysis and Photothermal Catalysis
journal, December 2018

Single Molecule Photocatalysis on TiO ₂ Surfaces: Focus Review
journal, September 2019

Incorporation of a [Ru(dcbpy)(bpy) ₂ ] ²⁺ photosensitizer and a Pt(dcbpy)Cl ₂ catalyst into metal–organic frameworks for photocatalytic hydrogen evolution from aqueous solution
journal, January 2015

MOF-derived nitrogen-doped nanoporous carbon for electroreduction of CO ₂ to CO: the calcining temperature effect and the mechanism
journal, January 2019

Synthesis and Hydrogen Sorption Properties of Carborane Based Metal−Organic Framework Materials
journal, October 2007

MOF Crystal Chemistry Paving the Way to Gas Storage Needs: Aluminum-Based soc -MOF for CH ₄ , O ₂ , and CO ₂ Storage
journal, October 2015

Noble-Metal-Free CdS Decorated Porous Ni _x Co _{1– x} O Skeleton Derived from Metal–Organic Framework for Efficient Visible-Light H ₂ Production
journal, December 2019

Fabrication of functional hollow microspheres constructed from MOF shells: Promising drug delivery systems with high loading capacity and targeted transport
journal, November 2016

Functional Porous Coordination Polymers
journal, April 2004

Transient Absorption Spectroscopy of Ruthenium and Osmium Polypyridyl Complexes Adsorbed onto Nanocrystalline TiO ₂ Photoelectrodes
journal, September 2002

Metal–Organic Frameworks as A Tunable Platform for Designing Functional Molecular Materials
journal, August 2013

Reaction Mechanism and Activity of WO ₃ -Catalyzed Photodegradation of Organic Substances Promoted by a CuO Cocatalyst
journal, March 2009