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Synergistic effect of Co/La in oxygen vacancy Rich Ternary CoAlLa layered double hydroxide with enhanced reductive sites for selective photoreduction of CO2 to CH4

Developing a convenient ternary layered double hydroxide (LDH) semiconductor for highly active photocatalytic reduction is necessary for solving the energy crisis and environmental pollution. In this work, a highly active ternary CoAlLa-LDH was formed through inducing La3+ to enhance coordinatively...

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Main Authors: Khan, Azmat Ali, Muhammad Tahir, Muhammad Tahir
Format: Article
Published: American Chemical Society 2021
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TP Chemical technology
Online Access:http://eprints.utm.my/id/eprint/95321/
http://dx.doi.org/10.1021/acs.energyfuels.1c00671
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spelling my.utm.953212022-04-29T22:26:28Z http://eprints.utm.my/id/eprint/95321/ Synergistic effect of Co/La in oxygen vacancy Rich Ternary CoAlLa layered double hydroxide with enhanced reductive sites for selective photoreduction of CO2 to CH4 Khan, Azmat Ali Muhammad Tahir, Muhammad Tahir TP Chemical technology Developing a convenient ternary layered double hydroxide (LDH) semiconductor for highly active photocatalytic reduction is necessary for solving the energy crisis and environmental pollution. In this work, a highly active ternary CoAlLa-LDH was formed through inducing La3+ to enhance coordinatively unsaturated metals centers for development of reductive sites that resulted in improvement of photogenerated charge carrier separation. It was demonstrated that the ratio of cations between the Co/Al/La-LDHs greatly determined the LDH structure for photocatalytic activity toward CO2 reduction. The increase of La content resulted in destruction of LDH structure with lower photoactivity for CO2 reduction. The rate of CO and CH4 evolution in Co2Al1-LDH was about 15.3 and 9.2 µmol gcat-1 h-1, much higher than Co3Al1-LDH and Co4Al1-LDH, which indicates that the Co2Al1-LDH among CoAl-LDHs is a promising photocatalyst with high photocatalytic activity in CO2 reduction to CO and CH4. The Co/Al/La molar ratios were optimized to be 2:0.95:0.05 with a production rate of 25.5 µmol gcat-1 h-1 and 21.80 µmol gcat-1 h-1 for CH4 and CO, respectively. A more interesting finding is that the selectivity of CH4 was raised to 53.93% as compared to 46.10% for CO. Besides, good stability was observed due to the presence of the intact hexagonal nanosheet structure, which was sustained in multiple cycles without obvious deactivation. The highest activity was due to the proper weaving of lanthanum into the framework of LDH. This work demonstrates a facile synthetic method of rationally doping La transition-metal to develop new photocatalyst with remarkable performance in CO2 reduction. American Chemical Society 2021 Article PeerReviewed Khan, Azmat Ali and Muhammad Tahir, Muhammad Tahir (2021) Synergistic effect of Co/La in oxygen vacancy Rich Ternary CoAlLa layered double hydroxide with enhanced reductive sites for selective photoreduction of CO2 to CH4. Energy and Fuels, 35 (10). pp. 8922-8943. ISSN 0887-0624 http://dx.doi.org/10.1021/acs.energyfuels.1c00671
institution Universiti Teknologi Malaysia
building UTM Library
collection Institutional Repository
continent Asia
country Malaysia
content_provider Universiti Teknologi Malaysia
content_source UTM Institutional Repository
url_provider http://eprints.utm.my/
topic TP Chemical technology
spellingShingle TP Chemical technology
Khan, Azmat Ali
Muhammad Tahir, Muhammad Tahir
Synergistic effect of Co/La in oxygen vacancy Rich Ternary CoAlLa layered double hydroxide with enhanced reductive sites for selective photoreduction of CO2 to CH4
description Developing a convenient ternary layered double hydroxide (LDH) semiconductor for highly active photocatalytic reduction is necessary for solving the energy crisis and environmental pollution. In this work, a highly active ternary CoAlLa-LDH was formed through inducing La3+ to enhance coordinatively unsaturated metals centers for development of reductive sites that resulted in improvement of photogenerated charge carrier separation. It was demonstrated that the ratio of cations between the Co/Al/La-LDHs greatly determined the LDH structure for photocatalytic activity toward CO2 reduction. The increase of La content resulted in destruction of LDH structure with lower photoactivity for CO2 reduction. The rate of CO and CH4 evolution in Co2Al1-LDH was about 15.3 and 9.2 µmol gcat-1 h-1, much higher than Co3Al1-LDH and Co4Al1-LDH, which indicates that the Co2Al1-LDH among CoAl-LDHs is a promising photocatalyst with high photocatalytic activity in CO2 reduction to CO and CH4. The Co/Al/La molar ratios were optimized to be 2:0.95:0.05 with a production rate of 25.5 µmol gcat-1 h-1 and 21.80 µmol gcat-1 h-1 for CH4 and CO, respectively. A more interesting finding is that the selectivity of CH4 was raised to 53.93% as compared to 46.10% for CO. Besides, good stability was observed due to the presence of the intact hexagonal nanosheet structure, which was sustained in multiple cycles without obvious deactivation. The highest activity was due to the proper weaving of lanthanum into the framework of LDH. This work demonstrates a facile synthetic method of rationally doping La transition-metal to develop new photocatalyst with remarkable performance in CO2 reduction.
format Article
author Khan, Azmat Ali
Muhammad Tahir, Muhammad Tahir
author_facet Khan, Azmat Ali
Muhammad Tahir, Muhammad Tahir
author_sort Khan, Azmat Ali
title Synergistic effect of Co/La in oxygen vacancy Rich Ternary CoAlLa layered double hydroxide with enhanced reductive sites for selective photoreduction of CO2 to CH4
title_short Synergistic effect of Co/La in oxygen vacancy Rich Ternary CoAlLa layered double hydroxide with enhanced reductive sites for selective photoreduction of CO2 to CH4
title_full Synergistic effect of Co/La in oxygen vacancy Rich Ternary CoAlLa layered double hydroxide with enhanced reductive sites for selective photoreduction of CO2 to CH4
title_fullStr Synergistic effect of Co/La in oxygen vacancy Rich Ternary CoAlLa layered double hydroxide with enhanced reductive sites for selective photoreduction of CO2 to CH4
title_full_unstemmed Synergistic effect of Co/La in oxygen vacancy Rich Ternary CoAlLa layered double hydroxide with enhanced reductive sites for selective photoreduction of CO2 to CH4
title_sort synergistic effect of co/la in oxygen vacancy rich ternary coalla layered double hydroxide with enhanced reductive sites for selective photoreduction of co2 to ch4
publisher American Chemical Society
publishDate 2021
url http://eprints.utm.my/id/eprint/95321/
http://dx.doi.org/10.1021/acs.energyfuels.1c00671
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score 13.211869

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