Engineering stable Pt nanoparticles and oxygen vacancies on defective TiO2 via introducing strong electronic metal-support interaction for efficient CO2 photoreduction

Liang Yi Lin; Shalinee Kavadiya; Xiang He; Wei Ning Wang; Bedia Begum Karakocak; Yu Chih Lin; Mikhail Y. Berezin; Pratim Biswas

doi:10.1016/j.cej.2019.123450

Engineering stable Pt nanoparticles and oxygen vacancies on defective TiO₂ via introducing strong electronic metal-support interaction for efficient CO₂ photoreduction

Liang Yi Lin, Shalinee Kavadiya, Xiang He, Wei Ning Wang, Bedia Begum Karakocak, Yu Chih Lin, Mikhail Y. Berezin, Pratim Biswas

Research output: Contribution to journal › Article › peer-review

117 Scopus citations

Abstract

This work for the first time reports the promoting effect of strong electronic metal-support interaction (EMSI) in Pt/TiO₂-V_O (V_O: oxygen vacancy) for gas-phase CO₂ photoreduction. A novel in-situ surface hydrogenation was developed to prepare hydrogenated Pt/TiO₂-V_O in a continuous, high throughput diffusion flame aerosol reactor. The combined results of various characterization techniques confirmed the presence of EMSI between Pt and defective TiO₂-V_O resulted in the enhanced electronic density of Pt nanoparticles. Both the modulated electronic structure of Pt and surface oxygen vacancies simultaneously promoted the activation of surface adsorbed carbon intermediates and facilitated the separation of photogenerated charges, eventually boosting the photocatalytic activity of Pt/TiO₂-V_O. The optimized Pt/TiO₂-V_O demonstrated a high quantum yield of 1.49% with high CH₄ selectivity (81%), which rendered 5.8- and 1.2-fold enhancements over its counterparts of TiO₂-V_O and Pt/TiO₂. More significantly, the EMSI also played a critical role in preserving the surface metallic Pt⁰ and oxygen vacancies, and in sustaining high activity of the Pt/TiO₂-V_O, whereas rapid catalytic deactivation are observed for both TiO₂-V_O and Pt/TiO₂.

Original language	English
Article number	123450
Journal	Chemical Engineering Journal
Volume	389
DOIs	https://doi.org/10.1016/j.cej.2019.123450
State	Published - Jun 1 2020

Keywords

CO reduction
Flame synthesis
Hydrogenation
Pt/TiO
Strong electronic metal-support interaction

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Lin, L. Y., Kavadiya, S., He, X., Wang, W. N., Karakocak, B. B., Lin, Y. C., Berezin, M. Y., & Biswas, P. (2020). Engineering stable Pt nanoparticles and oxygen vacancies on defective TiO₂ via introducing strong electronic metal-support interaction for efficient CO₂ photoreduction. Chemical Engineering Journal, 389, Article 123450. https://doi.org/10.1016/j.cej.2019.123450

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title = "Engineering stable Pt nanoparticles and oxygen vacancies on defective TiO2 via introducing strong electronic metal-support interaction for efficient CO2 photoreduction",

abstract = "This work for the first time reports the promoting effect of strong electronic metal-support interaction (EMSI) in Pt/TiO2-VO (VO: oxygen vacancy) for gas-phase CO2 photoreduction. A novel in-situ surface hydrogenation was developed to prepare hydrogenated Pt/TiO2-VO in a continuous, high throughput diffusion flame aerosol reactor. The combined results of various characterization techniques confirmed the presence of EMSI between Pt and defective TiO2-VO resulted in the enhanced electronic density of Pt nanoparticles. Both the modulated electronic structure of Pt and surface oxygen vacancies simultaneously promoted the activation of surface adsorbed carbon intermediates and facilitated the separation of photogenerated charges, eventually boosting the photocatalytic activity of Pt/TiO2-VO. The optimized Pt/TiO2-VO demonstrated a high quantum yield of 1.49% with high CH4 selectivity (81%), which rendered 5.8- and 1.2-fold enhancements over its counterparts of TiO2-VO and Pt/TiO2. More significantly, the EMSI also played a critical role in preserving the surface metallic Pt0 and oxygen vacancies, and in sustaining high activity of the Pt/TiO2-VO, whereas rapid catalytic deactivation are observed for both TiO2-VO and Pt/TiO2.",

keywords = "CO reduction, Flame synthesis, Hydrogenation, Pt/TiO, Strong electronic metal-support interaction",

author = "Lin, {Liang Yi} and Shalinee Kavadiya and Xiang He and Wang, {Wei Ning} and Karakocak, {Bedia Begum} and Lin, {Yu Chih} and Berezin, {Mikhail Y.} and Pratim Biswas",

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year = "2020",

month = jun,

day = "1",

doi = "10.1016/j.cej.2019.123450",

language = "English",

volume = "389",

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T1 - Engineering stable Pt nanoparticles and oxygen vacancies on defective TiO2 via introducing strong electronic metal-support interaction for efficient CO2 photoreduction

AU - Lin, Liang Yi

AU - Kavadiya, Shalinee

AU - He, Xiang

AU - Wang, Wei Ning

AU - Karakocak, Bedia Begum

AU - Lin, Yu Chih

AU - Berezin, Mikhail Y.

AU - Biswas, Pratim

PY - 2020/6/1

Y1 - 2020/6/1

N2 - This work for the first time reports the promoting effect of strong electronic metal-support interaction (EMSI) in Pt/TiO2-VO (VO: oxygen vacancy) for gas-phase CO2 photoreduction. A novel in-situ surface hydrogenation was developed to prepare hydrogenated Pt/TiO2-VO in a continuous, high throughput diffusion flame aerosol reactor. The combined results of various characterization techniques confirmed the presence of EMSI between Pt and defective TiO2-VO resulted in the enhanced electronic density of Pt nanoparticles. Both the modulated electronic structure of Pt and surface oxygen vacancies simultaneously promoted the activation of surface adsorbed carbon intermediates and facilitated the separation of photogenerated charges, eventually boosting the photocatalytic activity of Pt/TiO2-VO. The optimized Pt/TiO2-VO demonstrated a high quantum yield of 1.49% with high CH4 selectivity (81%), which rendered 5.8- and 1.2-fold enhancements over its counterparts of TiO2-VO and Pt/TiO2. More significantly, the EMSI also played a critical role in preserving the surface metallic Pt0 and oxygen vacancies, and in sustaining high activity of the Pt/TiO2-VO, whereas rapid catalytic deactivation are observed for both TiO2-VO and Pt/TiO2.

AB - This work for the first time reports the promoting effect of strong electronic metal-support interaction (EMSI) in Pt/TiO2-VO (VO: oxygen vacancy) for gas-phase CO2 photoreduction. A novel in-situ surface hydrogenation was developed to prepare hydrogenated Pt/TiO2-VO in a continuous, high throughput diffusion flame aerosol reactor. The combined results of various characterization techniques confirmed the presence of EMSI between Pt and defective TiO2-VO resulted in the enhanced electronic density of Pt nanoparticles. Both the modulated electronic structure of Pt and surface oxygen vacancies simultaneously promoted the activation of surface adsorbed carbon intermediates and facilitated the separation of photogenerated charges, eventually boosting the photocatalytic activity of Pt/TiO2-VO. The optimized Pt/TiO2-VO demonstrated a high quantum yield of 1.49% with high CH4 selectivity (81%), which rendered 5.8- and 1.2-fold enhancements over its counterparts of TiO2-VO and Pt/TiO2. More significantly, the EMSI also played a critical role in preserving the surface metallic Pt0 and oxygen vacancies, and in sustaining high activity of the Pt/TiO2-VO, whereas rapid catalytic deactivation are observed for both TiO2-VO and Pt/TiO2.

KW - CO reduction

KW - Flame synthesis

KW - Hydrogenation

KW - Pt/TiO

KW - Strong electronic metal-support interaction

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Engineering stable Pt nanoparticles and oxygen vacancies on defective TiO₂ via introducing strong electronic metal-support interaction for efficient CO₂ photoreduction

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