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Engineering a Self-Grown TiO2/Ti-MOF Heterojunction with Selectively Anchored High-Density Pt Single-Atomic Cocatalysts for Efficient Visible-Light-Driven Hydrogen Evolution |
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| Authors: | Xiaoyu He Dr. Yujia Ding Zhennan Huang Dr. Min Liu Prof. Miaofang Chi Prof. Zili Wu Prof. Carlo U. Segre Prof. Chunshan Song Prof. Xiang Wang Prof. Xinwen Guo |
| Affiliation: | 1. State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024 China Contribution: Conceptualization (lead), Data curation (lead), Formal analysis (lead), Investigation (lead), Writing - original draft (lead);2. Department of Physics and CSRRI, Illinois Institute of Technology, Chicago, IL, 60616 USA Contribution: Conceptualization (supporting), Investigation (lead), Writing - original draft (supporting);3. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831 USA Contribution: Conceptualization (supporting), Investigation (lead), Writing - original draft (supporting);4. State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024 China Contribution: Conceptualization (supporting), Supervision (supporting), Writing - review & editing (supporting);5. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831 USA Contribution: Investigation (equal), Writing - original draft (equal);6. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831 USA Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831 USA Contribution: Conceptualization (supporting), Supervision (supporting), Writing - review & editing (supporting);7. Department of Physics and CSRRI, Illinois Institute of Technology, Chicago, IL, 60616 USA Contribution: Investigation (equal), Supervision (supporting), Writing - review & editing (supporting);8. State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024 China |
| 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 |