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Titanium dioxide/carbon nitride nanosheet nanocomposites for gas phase CO2 photoreduction under UV-visible irradiation

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TiO2-CN SI 021018_Accepted.docxFile embargoed until 09 October 20196.15 MBMicrosoft Word    Request a copy
TiO2-CN 021018_Accepted.docxFile embargoed until 09 October 201919.2 MBMicrosoft Word    Request a copy
Title: Titanium dioxide/carbon nitride nanosheet nanocomposites for gas phase CO2 photoreduction under UV-visible irradiation
Authors: Crake, A
Christoforidis, K
Godin, R
Moss, B
Kafizas, A
Zafeiratos, S
Durrant, J
Petit, C
Item Type: Journal Article
Abstract: In the field of photocatalysis and particularly that of CO2 photoreduction, the formulation of nanocomposites provids avenues to design a material platform with a unique set of structural, optoelectronic and chemical features thereby addressing shortcomings of single-phase materials and allowing synergistic effects. In this work, inorganic/organic composite photocatalysts for CO2 reduction comprised of titanium dioxide (TiO2) and carbon nitride nanosheets (CNNS) were synthesized using a hydrothermal in-situ growth method. Specifically, pre-formed CNNS were used to synthesize TiO2/CNNS heterostructures with control over the TiO2 facet formation. This synthesis approach improved the catalytic properties by increasing CO2 adsorption capacity and facilitating charge transfer. The materials were characterised by various spectroscopic, imaging, and analytical techniques to investigate their structural (from nano- to macroscale), chemical, and optical properties. TiO2 nanoparticles were efficiently grown on the CNNS. The CO2 adsorption capacity of the composites was measured, and they were tested for CO2 photoreduction under UV-Vis illumination with hydrogen as the reducing agent in a heterogeneous gas-solid system to combine CO2 capture and conversion into a single-step process. Catalytic tests were performed without adding any precious metal co-catalyst. The composites exhibited enhanced CO2 adsorption capacity and photocatalytic CO2 conversion compared to their constituent materials (> ten-fold increase) and outperformed the TiO2 P25 benchmark material. The TiO2/CNNS composite with more {001} TiO2 facets was the most catalytically active. Further investigations using transient absorption spectroscopy (TAS) revealed the control of facet formation improved interfacial transfer at the TiO2/CNNS junction. A photocatalytic mechanism was proposed based on the spectroscopic analyses as well as the CO2 adsorption, and CO2 conversion results.
Issue Date: 1-Mar-2019
Date of Acceptance: 7-Oct-2018
URI: http://hdl.handle.net/10044/1/65303
DOI: https://dx.doi.org/10.1016/j.apcatb.2018.10.023
ISSN: 0926-3373
Publisher: Elsevier
Start Page: 369
End Page: 378
Journal / Book Title: Applied Catalysis B: Environmental
Volume: 242
Copyright Statement: © 2018 Elsevier B.V. All rights reserved. This manuscript is licensed under the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International http://creativecommons.org/licenses/by-nc-nd/4.0/
Sponsor/Funder: Commission of the European Communities
Engineering and Physical Sciences Research Council
Engineering & Physical Science Research Council (EPSRC)
Kaust
The Royal Society
Funder's Grant Number: 291482
EP/N024206/1
CHEDG_P61719
RSG\R1\180434
Keywords: Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Engineering, Environmental
Engineering, Chemical
Chemistry
Engineering
Carbon nitride nanosheets
TiO2
001 facets
CO2 reduction
Heterojunction
GRAPHITIC CARBON NITRIDE
ENHANCED PHOTOCATALYTIC ACTIVITY
METAL-ORGANIC FRAMEWORKS
ANATASE TIO2
001 FACETS
HYDROGEN EVOLUTION
BAND ALIGNMENT
SEMICONDUCTORS
EFFICIENT
REDUCTION
0306 Physical Chemistry (Incl. Structural)
0904 Chemical Engineering
0907 Environmental Engineering
Physical Chemistry
Publication Status: Published
Embargo Date: 2019-10-09
Online Publication Date: 2018-10-09
Appears in Collections:Chemistry
Centre for Environmental Policy
Chemical Engineering
Faculty of Natural Sciences



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