Citation: Xingyan Liu, Chaogang Jia, Guangmei Jiang, Chenghua Zhang, Mingzuo Chen, Xiaofei Zhao, Xiaocheng Zhang, Min Fu, Siqi Li, Jie Wu, Yiming Jia, Youzhou He. Single-atom Pd anchored in the porphyrin-center of ultrathin 2D-MOFs as the active center to enhance photocatalytic hydrogen-evolution and NO-removal[J]. Chinese Chemical Letters, ;2024, 35(9): 109455. doi: 10.1016/j.cclet.2023.109455 shu

Single-atom Pd anchored in the porphyrin-center of ultrathin 2D-MOFs as the active center to enhance photocatalytic hydrogen-evolution and NO-removal

Xingyan Liu ^{a, 1} ,
Chaogang Jia ^{a, 1} ,
Guangmei Jiang ^a ,
Chenghua Zhang ^{b, *,} ,
Mingzuo Chen ^a ,
Xiaofei Zhao ^{c, *,} ,
Xiaocheng Zhang ^a ,
Min Fu ^a ,
Siqi Li ^d ,
Jie Wu ^e ,
Yiming Jia ^f ,
Youzhou He ^{a, *,}

a.
Chongqing Key Laboratory of Catalysis and New Environmental Materials, College of Environment and Resources, Chongqing Technology and Business University, Chongqing 400067, China
b.
School of Pharmacy, North Sichuan Medical College, Nanchong 637100, China
c.
Carbon Neutrality Technology Application Research Center, College of River and Ocean Engineering, Chongqing Jiaotong University, Chongqing 400074, China
d.
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
e.
National Local Joint Engineering Research Center for Road Engineering and Disaster Prevention and Reduction Technology in Mountainous Areas, China Merchants Chongqing Communications Technology Research and Design Institute Co., Ltd., Chongqing 400067, China
f.
Chongqing Culture Relics and Archaeology Research Institute, Chongqing 400013, China

zchua@nsmc.edu.cn

zxf@cqjtu.edu.cn

yzhectbu@163.com

Received Date: 26 August 2023
Revised Date: 6 December 2023
Accepted Date: 22 December 2023
Available Online: 26 December 2023

Figures(4)

Single-atom catalysts were widely used to treat atmospheric pollution and alleviate energy crises through photocatalysis. However, how to prevent the aggregation of single atoms during the preparation and catalytic processes remained a great challenge. Herein, a novel ultrathin two-dimensional porphyrin-based single-atom photocatalyst Ti-MOF (abbreviated as TMPd) obtained through a simple hydrothermal synthesis strategy was used for photocatalytic hydrogen evolution and NO removal, in which the single-atom Pd tightly anchored in the center of porphyrin to ensure single-atom Pd stable existence. Compared with most reported MOFs-based photocatalysts, the TMPd showed an excellent hydrogen evolution rate (1.32 mmol g⁻¹ h⁻¹) and the NO removal efficiency (62%) under visible light irradiation. Aberration-corrected high-angle annular dark-field scanning transmission electron microscope (HAADF-STEM) and synchrotron-radiation-based X-ray absorption fine-structure spectroscopy (XAFS) proved that pd in TMPd existed in an isolated state, and the atomic force microscope (AFM) proved the ultrathin morphology of TMPd. DFT calculations had demonstrated that single-atom Pd could serve as the active center and more effectively achieve electron transfer, indicating that single-atom Pd played a vital role in photocatalytic hydrogen evolution. In addition, a possible photocatalytic pathway of NO removal was proposed based on ESR and in-situ infrared spectra, in which the catalysts anchored with single-atom Pd could produce more active substances and more effectively oxidize NO to NO₂⁻ or NO₃⁻. The results suggested that coordinating single-atom metal species as the active site in the center of porphyrin could be a feasible strategy to obtain various ultrathin porphyrin-based single-atom photocatalysts to acquire excellent photocatalytic performance further.
- Porphyrin-based MOFs,
- Single-atom Pd,
- Ultrathin 2D nanosheets,
- Hydrogen evolution,
- NO removal
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