Engineering a Self-Grown TiO2/Ti-MOF Heterojunction with Selectively Anchored High-Density Pt Single-Atomic Cocatalysts for Efficient Visible-Light-Driven Hydrogen Evolution

Xiaoyu He; Yujia Ding; Zhennan Huang; Min Liu; Miaofang Chi; Zili Wu; Carlo U. Segre; Chunshan Song; Xiang Wang; Xinwen Guo

doi:10.1002/anie.202217439

Engineering a Self-Grown TiO₂/Ti-MOF Heterojunction with Selectively Anchored High-Density Pt Single-Atomic Cocatalysts for Efficient Visible-Light-Driven Hydrogen Evolution

Xiaoyu He, Yujia Ding, Zhennan Huang, Min Liu, Miaofang Chi, Zili Wu, Carlo U. Segre, Chunshan Song, Xiang Wang, Xinwen Guo

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

32 Scopus citations

Abstract

A photocatalyst TiO₂/Ti-BPDC-Pt is developed with a self-grown TiO₂/Ti-metal–organic framework (MOF) heterojunction, i.e., TiO₂/Ti-BPDC, and selectively anchored high-density Pt single-atomic cocatalysts on Ti-BPDC for photocatalytic hydrogen evolution. This intimate heterojunction, growing from the surface pyrolytic reconstruction of Ti-BPDC, works in a direct Z-scheme, efficiently separating electrons and holes. Pt is selectively anchored on Ti-BPDC by ligands and is found in the form of single atoms with loading up to 1.8 wt %. The selective location of Pt is the electron-enriched domain of the heterojunction, which further enhances the utilization of the separated electrons. This tailored TiO₂/Ti-BPDC-Pt shows a significantly enhanced activity of 12.4 mmol g⁻¹ h⁻¹ compared to other TiO₂- or MOF-based catalysts. The structure-activity relationship further proves the balance of two simultaneously exposed domains of heterojunctions is critical to fulfilling this kind of catalyst.

Original language	English
Article number	e202217439
Journal	Angewandte Chemie - International Edition
Volume	62
Issue number	25
DOIs	https://doi.org/10.1002/anie.202217439
State	Published - Jun 19 2023

Funding

This work was financially supported by the National Natural Science Foundation of China (22278056), the Liaoning Revitalization Talent Program (XLYC2008032) and the Fundamental Research Funds for the Central Universities (DUT22LAB602). MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE‐AC02‐06CH11357. ZH, MC, and ZW were sponsored by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program. The scanning transmission electron microscopy work was conducted at the Center for Nanophase Materials Sciences (CNMS), Which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. This work was financially supported by the National Natural Science Foundation of China (22278056), the Liaoning Revitalization Talent Program (XLYC2008032) and the Fundamental Research Funds for the Central Universities (DUT22LAB602). MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. ZH, MC, and ZW were sponsored by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program. The scanning transmission electron microscopy work was conducted at the Center for Nanophase Materials Sciences (CNMS), Which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory.

Funders	Funder number
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Argonne National Laboratory	DE‐AC02‐06CH11357
Oak Ridge National Laboratory
National Natural Science Foundation of China	22278056
Fundamental Research Funds for the Central Universities	DUT22LAB602
Liaoning Revitalization Talents Program	XLYC2008032

Keywords

Charge Transfer
Heterojunction
MOFs
Photocatalysis
Structure-Activity Relationship

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1002/anie.202217439

Cite this

He, X., Ding, Y., Huang, Z., Liu, M., Chi, M., Wu, Z., Segre, C. U., Song, C., Wang, X., & Guo, X. (2023). Engineering a Self-Grown TiO₂/Ti-MOF Heterojunction with Selectively Anchored High-Density Pt Single-Atomic Cocatalysts for Efficient Visible-Light-Driven Hydrogen Evolution. Angewandte Chemie - International Edition, 62(25), Article e202217439. https://doi.org/10.1002/anie.202217439

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title = "Engineering a Self-Grown TiO2/Ti-MOF Heterojunction with Selectively Anchored High-Density Pt Single-Atomic Cocatalysts for Efficient Visible-Light-Driven Hydrogen Evolution",

abstract = "A photocatalyst TiO2/Ti-BPDC-Pt is developed with a self-grown TiO2/Ti-metal–organic framework (MOF) heterojunction, i.e., TiO2/Ti-BPDC, and selectively anchored high-density Pt single-atomic cocatalysts on Ti-BPDC for photocatalytic hydrogen evolution. This intimate heterojunction, growing from the surface pyrolytic reconstruction of Ti-BPDC, works in a direct Z-scheme, efficiently separating electrons and holes. Pt is selectively anchored on Ti-BPDC by ligands and is found in the form of single atoms with loading up to 1.8 wt %. The selective location of Pt is the electron-enriched domain of the heterojunction, which further enhances the utilization of the separated electrons. This tailored TiO2/Ti-BPDC-Pt shows a significantly enhanced activity of 12.4 mmol g−1 h−1 compared to other TiO2- or MOF-based catalysts. The structure-activity relationship further proves the balance of two simultaneously exposed domains of heterojunctions is critical to fulfilling this kind of catalyst.",

keywords = "Charge Transfer, Heterojunction, MOFs, Photocatalysis, Structure-Activity Relationship",

author = "Xiaoyu He and Yujia Ding and Zhennan Huang and Min Liu and Miaofang Chi and Zili Wu and Segre, {Carlo U.} and Chunshan Song and Xiang Wang and Xinwen Guo",

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He, X, Ding, Y, Huang, Z, Liu, M, Chi, M , Wu, Z, Segre, CU, Song, C, Wang, X & Guo, X 2023, 'Engineering a Self-Grown TiO₂/Ti-MOF Heterojunction with Selectively Anchored High-Density Pt Single-Atomic Cocatalysts for Efficient Visible-Light-Driven Hydrogen Evolution', Angewandte Chemie - International Edition, vol. 62, no. 25, e202217439. https://doi.org/10.1002/anie.202217439

Engineering a Self-Grown TiO₂/Ti-MOF Heterojunction with Selectively Anchored High-Density Pt Single-Atomic Cocatalysts for Efficient Visible-Light-Driven Hydrogen Evolution. / He, Xiaoyu; Ding, Yujia; Huang, Zhennan et al.
In: Angewandte Chemie - International Edition, Vol. 62, No. 25, e202217439, 19.06.2023.

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

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T1 - Engineering a Self-Grown TiO2/Ti-MOF Heterojunction with Selectively Anchored High-Density Pt Single-Atomic Cocatalysts for Efficient Visible-Light-Driven Hydrogen Evolution

AU - He, Xiaoyu

AU - Ding, Yujia

AU - Huang, Zhennan

AU - Liu, Min

AU - Chi, Miaofang

AU - Wu, Zili

AU - Segre, Carlo U.

AU - Song, Chunshan

AU - Wang, Xiang

AU - Guo, Xinwen

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N2 - A photocatalyst TiO2/Ti-BPDC-Pt is developed with a self-grown TiO2/Ti-metal–organic framework (MOF) heterojunction, i.e., TiO2/Ti-BPDC, and selectively anchored high-density Pt single-atomic cocatalysts on Ti-BPDC for photocatalytic hydrogen evolution. This intimate heterojunction, growing from the surface pyrolytic reconstruction of Ti-BPDC, works in a direct Z-scheme, efficiently separating electrons and holes. Pt is selectively anchored on Ti-BPDC by ligands and is found in the form of single atoms with loading up to 1.8 wt %. The selective location of Pt is the electron-enriched domain of the heterojunction, which further enhances the utilization of the separated electrons. This tailored TiO2/Ti-BPDC-Pt shows a significantly enhanced activity of 12.4 mmol g−1 h−1 compared to other TiO2- or MOF-based catalysts. The structure-activity relationship further proves the balance of two simultaneously exposed domains of heterojunctions is critical to fulfilling this kind of catalyst.

AB - A photocatalyst TiO2/Ti-BPDC-Pt is developed with a self-grown TiO2/Ti-metal–organic framework (MOF) heterojunction, i.e., TiO2/Ti-BPDC, and selectively anchored high-density Pt single-atomic cocatalysts on Ti-BPDC for photocatalytic hydrogen evolution. This intimate heterojunction, growing from the surface pyrolytic reconstruction of Ti-BPDC, works in a direct Z-scheme, efficiently separating electrons and holes. Pt is selectively anchored on Ti-BPDC by ligands and is found in the form of single atoms with loading up to 1.8 wt %. The selective location of Pt is the electron-enriched domain of the heterojunction, which further enhances the utilization of the separated electrons. This tailored TiO2/Ti-BPDC-Pt shows a significantly enhanced activity of 12.4 mmol g−1 h−1 compared to other TiO2- or MOF-based catalysts. The structure-activity relationship further proves the balance of two simultaneously exposed domains of heterojunctions is critical to fulfilling this kind of catalyst.

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KW - MOFs

KW - Photocatalysis

KW - Structure-Activity Relationship

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