Efficient Photoelectrocatalysis of Glycerol to Dihydroxyacetone and Synergistic Hydrogen Generation via Dual Oxidation Pathways Using Co-LDH/Bi2O3/TiO2 Ternary Array

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-01-22 DOI:10.1021/acscatal.4c05193

Lu Niu, Rufeng Tian, Wanggang Zhang, Hongxia Wang, Jian Wang, Yiming Liu

{"title":"Efficient Photoelectrocatalysis of Glycerol to Dihydroxyacetone and Synergistic Hydrogen Generation via Dual Oxidation Pathways Using Co-LDH/Bi2O3/TiO2 Ternary Array","authors":"Lu Niu, Rufeng Tian, Wanggang Zhang, Hongxia Wang, Jian Wang, Yiming Liu","doi":"10.1021/acscatal.4c05193","DOIUrl":null,"url":null,"abstract":"Replacing the oxygen evolution reaction (OER) in photoelectrocatalytic (PEC) water splitting with glycerol oxidation reaction (GOR) not only enhances hydrogen production but also generates high-value glycerol byproducts. In this study, we developed a ternary photoanode, Co-LDH/Bi2O3/TiO2, by loading particulate Bi2O3 and linear Co-LDH onto a TiO2 nanorod for glycerol conversion and hydrogen production. The characterization results confirm the formation of coupled interfaces between Co-LDH and Bi2O3 and TiO2, which improves the visible light utilization and promotes the formation of type II heterojunctions, resulting in a significant suppression of electron–hole recombination and an improvement in the PEC performance. Fourier transform infrared (FT-IR) spectroscopy revealed that the Co-LDH/Bi2O3/TiO2 photoanode exhibited stronger adsorption of glycerol intermediate hydroxyl group and more effective desorption of DHA compared to TiO2 and binary photoanodes (Co-LDH/TiO2 and Bi2O3/TiO2), resulting in high-selectivity glycerol conversion to DHA. Mechanistic studies and density function theory calculations have shown that the binary photoanode Co-LDH/TiO2 oxidizes glycerol mainly through hole oxidation, and the binary photoanode Bi2O3/TiO2 oxidizes glycerol mainly through hydroxyl radical (•OH) oxidation. Therefore, the ternary photoanode constructed (Co-LDH/Bi2O3/TiO2) with a dual heterojunction converts glycerol through the dual pathways of hole oxidation and •OH oxidation. This work demonstrates a promising strategy for developing high-performance photoanodes in PEC systems for glycerol oxidation and hydrogen production, leveraging the synergistic effects of multisemiconductor heterojunctions and multiple oxidation pathways, offering significant potential for practical applications.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"45 1","pages":""},"PeriodicalIF":11.3000,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acscatal.4c05193","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}

引用次数: 0

Abstract

Replacing the oxygen evolution reaction (OER) in photoelectrocatalytic (PEC) water splitting with glycerol oxidation reaction (GOR) not only enhances hydrogen production but also generates high-value glycerol byproducts. In this study, we developed a ternary photoanode, Co-LDH/Bi₂O₃/TiO₂, by loading particulate Bi₂O₃ and linear Co-LDH onto a TiO₂ nanorod for glycerol conversion and hydrogen production. The characterization results confirm the formation of coupled interfaces between Co-LDH and Bi₂O₃ and TiO₂, which improves the visible light utilization and promotes the formation of type II heterojunctions, resulting in a significant suppression of electron–hole recombination and an improvement in the PEC performance. Fourier transform infrared (FT-IR) spectroscopy revealed that the Co-LDH/Bi₂O₃/TiO₂ photoanode exhibited stronger adsorption of glycerol intermediate hydroxyl group and more effective desorption of DHA compared to TiO₂ and binary photoanodes (Co-LDH/TiO₂ and Bi₂O₃/TiO₂), resulting in high-selectivity glycerol conversion to DHA. Mechanistic studies and density function theory calculations have shown that the binary photoanode Co-LDH/TiO₂ oxidizes glycerol mainly through hole oxidation, and the binary photoanode Bi₂O₃/TiO₂ oxidizes glycerol mainly through hydroxyl radical (^•OH) oxidation. Therefore, the ternary photoanode constructed (Co-LDH/Bi₂O₃/TiO₂) with a dual heterojunction converts glycerol through the dual pathways of hole oxidation and ^•OH oxidation. This work demonstrates a promising strategy for developing high-performance photoanodes in PEC systems for glycerol oxidation and hydrogen production, leveraging the synergistic effects of multisemiconductor heterojunctions and multiple oxidation pathways, offering significant potential for practical applications.

Abstract Image

查看原文本刊更多论文

求助全文

约1分钟内获得全文求助全文

来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.