4.8 Article

In Situ Monitoring Charge Transfer on Topotactic Epitaxial Heterointerface for Tetracycline Degradation at the Single-Particle Level

Journal

ACS CATALYSIS
Volume 12, Issue 15, Pages 9114-9124

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c02447

Keywords

epitaxial heterojunction; single-particle spectroscopy; charge transfer; FLIM; crystal facet

Funding

  1. National Natural Science Foundation of China [22072072]
  2. National Key Research and Development Program of China [2020YFA0710301]
  3. Natural Science Foundation of Shandong Province [ZR2021JQ06]
  4. Shandong University Multidisciplinary Research and Innovation Team of Young Scholars [2020QNQT11, 2020QNQT012]
  5. Qilu Young Scholars and Outstanding Young Scholars Projects of Shandong University

Ask authors/readers for more resources

This study presents a strategy for synthesizing SrTiO3/TiO2 epitaxial heterojunctions and investigates the charge transfer process using single-particle spectroscopy. The results demonstrate that the epitaxial heterointerface promotes charge separation and suppresses photoluminescence lifetime decay. This research provides a new strategy for rational designing heterojunction photocatalysts and in-depth monitoring of the structure-activity relationship at the single-particle level.
Selectively constructing heterojunctions on specific crystal facets enable directional electron-hole migration and favorable charge separation. Meanwhile, in-depth monitoring and investigating charge-transfer process on specific crystal facets of individual single crystal are particularly important. Herein, we report a strategy for synthesizing SrTiO3/TiO2 epitaxial heterojunctions (ST/T), in which highly ordered SrTiO3 mesocrystals are selectively topologically grown on the TiO2 {001} facet. It exhibits good photocatalytic activity for tetracycline (TC) degradation. Notably, single-particle spectroscopy was employed to accurately monitor the transfer and recombination of carriers at the specific nanoregions of individual particle. The weaker photoluminescence (PL) intensity and longer lifetime at the epitaxial central site of ST/T particle indicate that the epitaxial heterointerface promotes the separation of charge carriers. Moreover, in situ monitoring of TC degradation on single ST/T particle confirms that the epitaxial heterojunction suppressed the PL lifetime decay, further demonstrating the pivotal role of site-selective topotactic epitaxy. This study presents a strategy for rational designing heterojunction photocatalysts and is beneficial for in-depth monitoring and understanding the structure-activity relationship at the single-particle level.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.8
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

Article Engineering, Environmental

Insight into a strategy to improve charge carrier migration in lead-free bismuth-based halide perovskite for efficient selective oxidation of thioanisole under visible light

Zihao Cui, Yaqiang Wu, Shuhui Zhang, Hui Fu, Guoqiang Chen, Zaizhu Lou, Xiaolei Liu, Qianqian Zhang, Zeyan Wang, Zhaoke Zheng, Hefeng Cheng, Yuanyuan Liu, Ying Dai, Baibiao Huang, Peng Wang

Summary: In this study, a new lead-free perovskite solid solution Cs-3(BixSb1-x)(2)Br-9 with tunable band gap was prepared through a facile and efficient co-precipitation method. The introduction of Sb atoms in Cs3Bi2Br9 significantly broadened the absorption of visible light, making it a promising visible-light photocatalyst. The CBSB solid solution also exhibited excellent stability, showing no apparent decrease in catalytic activity in a five-cycle experiment. This research provides new insights into improving the carrier lifetime of lead-free perovskite materials, presents a new approach for selective photo-oxidation, and may have implications for other solar energy conversion areas related to halide perovskites.

CHEMICAL ENGINEERING JOURNAL (2023)

Article Engineering, Environmental

Stabilizing Cu2O for enhancing selectivity of CO2 electroreduction to C2H4 with the modification of Pd nanoparticles

Difei Xiao, Xiaolei Bao, Minghui Zhang, Zaiqi Li, Zeyan Wang, Yugang Gao, Zhaoke Zheng, Peng Wang, Hefeng Cheng, Yuanyuan Liu, Ying Dai, Baibiao Huang

Summary: This study successfully stabilized Cu+ and *CO intermediates and improved the production efficiency of C2H4 during CO2RR by designing and synthesizing the Pd-Cu2O catalyst.

CHEMICAL ENGINEERING JOURNAL (2023)

Article Chemistry, Physical

Dual-plasmon-enhanced nitrophenol hydrogenation over W18O49-Au heterostructures studied at the single-particle level

Yayang Xu, Shiqiang Yu, Fengxia Tong, Zeyan Wang, Peng Wang, Yuanyuan Liu, Hefeng Cheng, Yuchen Fan, Wei Wei, Ying Dai, Zhaoke Zheng, Baibiao Huang

Summary: The coupling of W18O49 and Au in W18O49-Au heterostructures enhanced the light absorption and carrier separation ability of this dual-plasmonic system, leading to highly enhanced performance for nitrophenol hydrogenation. The rate constant of W18O49-Au reached 0.2044 min(-1), which was 12 and 102 times higher than that of Au and W18O49, respectively. The hot electron injection process from W18O49 to Au, demonstrated by single-particle photoluminescence (PL) spectroscopy, was found to be beneficial for boosting the catalytic performance.

CATALYSIS SCIENCE & TECHNOLOGY (2023)

Article Chemistry, Multidisciplinary

Extended Light Absorption and Improved Charge Separation by Protonation of the Organic Ligand in a Bismuth-Based Metal-Organic Framework

Longfei Lei, Yuanyuan Liu, Yujia Zhang, Caiyun Zhang, Yujie Li, Zeyan Wang, Peng Wang, Zhaoke Zheng, Hefeng Cheng, Ying Dai, Baibiao Huang

Summary: A new method to extend the light absorption and improve the photocatalytic activity of metal-organic frameworks (MOFs) with nitrogen-containing ligand is reported in this study, involving the protonation of nitrogen. The protonation of nitrogen in the thiazolyl ring in the MOFs was found to lead to a wider visible light absorption as well as improved charge separation and transfer, resulting in enhanced photocatalytic activity. This work provides a new idea for the design of nitrogen-containing Bi-based MOFs with enhanced photocatalytic performance.

CHEMISTRY-A EUROPEAN JOURNAL (2023)

Article Chemistry, Multidisciplinary

In Situ Monitoring of the Spatial Distribution of Oxygen Vacancies and Enhanced Photocatalytic Performance at the Single-Particle Level

Yujia Zhang, Yan Liu, Ting Zhang, Xueqin Gong, Zeyan Wang, Yuanyuan Liu, Peng Wang, Hefeng Cheng, Ying Dai, Baibiao Huang, Zhaoke Zheng

Summary: A single-particle spectroscopy technique is used to quantitatively monitor the spatial distribution of oxygen vacancies (OVs) on different facets. Taking monoclinic BiVO4 as an example, by tracking the photoluminescence (PL) lifetimes and spectra of different facets before and after hydrogen treatment, we confirm that the PL emission originates from the OV state and determine that OVs are more likely to be generated on the {010} facets. This anisotropic defect engineering significantly prolongs the carrier lifetime and accelerates the activation of molecular oxygen.

NANO LETTERS (2023)

Article Chemistry, Physical

Electronic Structure Manipulation via Site-Selective Atomically Dispersed Ni for Efficient Photocatalytic CO2 Reduction

Yuyin Mao, Minghui Zhang, Shenghe Si, Guangyao Zhai, Xiaolei Bao, Kepeng Song, Lirong Zheng, Yuanyuan Liu, Zeyan Wang, Zhaoke Zheng, Peng Wang, Ying Dai, Hefeng Cheng, Baibiao Huang

Summary: In this study, two different nickel single-atom catalysts (Ni-SACs) were constructed on WO2.72 nanowires, including bulk doping of single Ni atoms in WO2.72 (B-Ni-1/WO2.72) and surface anchoring of single Ni atoms on WO2.72 (S-Ni-1/WO2.72), to explore the electronic structure manipulation for enhancing CO2 photoreduction. The results showed that B-Ni-1/WO2.72 exhibited superior photocatalytic performance compared to S-Ni-1/WO2.72, achieving a CO yield of 80.5 mmol g(-1) h(-1) with a selectivity of 98.7%. This study provides valuable insights into the optimization of site-related electronic structures for efficient single-atom catalysts in artificial photosynthesis.

ACS CATALYSIS (2023)

Article Chemistry, Physical

Electrocatalytic Waste-Treating-Waste Strategy for Concurrently Upgrading of Polyethylene Terephthalate Plastic and CO2 into Value-Added Formic Acid

Fahao Ma, Zaiqi Li, Riming Hu, Zengqi Wang, Junpeng Wang, Jinkai Li, Yong Nie, Zhaoke Zheng, Xuchuan Jiang

Summary: This study presents a waste-treating-waste strategy that converts PET plastic and CO2 wastes into formic acid. Engineered electrocatalysts enable high selectivity of formic acid at ultralow potentials. Experimental and theoretical results reveal the significant effects of oxygen vacancies and interface electron transfer on catalytic performance.

ACS CATALYSIS (2023)

Article Chemistry, Inorganic & Nuclear

Insight into the complexation mechanism between a BiVO4 photoanode and tartaric acid for efficient photoelectrochemical H2 production

Zhaoqi Wang, Shuhua Wang, Xiaolei Liu, Yayang Xu, Dujuan Dai, Shuang Zhao, Peng Wang, Zhaoke Zheng, Yuanyuan Liu, Hefeng Cheng, Ying Dai, Zeyan Wang, Baibiao Huang

Summary: Recently, a highly active BiVO4-tartaric acid (C4H6O6) PEC fuel cell with efficient charge and energy transfer paths has been investigated. The complexation mechanism between BiVO4 and C4H6O6 is explored through theoretical calculations and experiments. The optimal metal complexation site of C4H6O6 is found to be crucial for enhancing the PEC performance, leading to improved photoelectric conversion and energy release. The research also suggests that other materials with similar complexation sites and energy band configurations can achieve enhanced PEC activity. This work provides an in-depth understanding of the complexation mechanism in C4H6O6-based PEC fuel cell and has potential for inspiring the design of efficient PEC fuel cells.

INORGANIC CHEMISTRY FRONTIERS (2023)

Article Chemistry, Physical

Enhanced thermal assisted photocatalysis reduction of carbon dioxide over a Fe2-xGaxO3 solid solution

Lingtong Lin, Danning Xing, Caiyun Zhang, Yuanyuan Liu, Zeyan Wang, Peng Wang, Zhaoke Zheng, Hefeng Cheng, Ying Dai, Baibiao Huang

Summary: Alpha-Fe2O3 is a promising photocatalytic material with low cost and excellent visible light absorption, but its efficiency is limited by charge recombination. This study introduces Ga in the form of Fe2-xGaxO3 solid solution to improve the electronic structure and photoelectrical activity. The introduction of Ga reverses the electron spin state, suppressing carrier recombination. Experimental results support the theoretical calculations, and Fe1.96Ga0.04O3 shows the best photothermal activity for CO2 reduction, with a CO evolution rate 2.4 times higher than pure Fe2O3. This work provides an alternative approach to enhance the activity of alpha-Fe2O3.

CATALYSIS SCIENCE & TECHNOLOGY (2023)

Article Chemistry, Multidisciplinary

Growth mechanism of [100]-oriented TaON film through an endotaxial transformation from a (012)-LiTaO3 single crystal substrate

Xuesen Qin, Huiliang Li, Zeyan Wang, Zhaoke Zheng, Peng Wang, Hefeng Cheng, Yuanyuan Liu, Yuchen Fan, Ying Dai, Baibiao Huang

Summary: Metal nitrides are usually prepared by high temperature nitridation with metal oxide precursors under an NH3 atmosphere. However, the preparation of oriented nitride nanostructures is challenging due to the differences in crystal structures between oxide precursors and nitride products. This work systematically investigates the endotaxial growth process of TaON from a LiTaO3 single crystal substrate and proposes a plausible growth mechanism. It contributes to a better understanding of the unique endotaxial growth process and facilitates the fabrication of other oriented nitride nanostructures.

CRYSTENGCOMM (2023)

No Data Available