Stepwise Coordination Engineering of Pt<sub>1</sub>/Au<sub>25</sub> Dual Catalytic Sites with Enhanced Electrochemical Activity and Stability
Abstract
AbstractDual‐site catalysts hold significant promise for accelerating complex electrochemical reactions, but a major challenge remains in balancing high loading with precise dual‐site architecture to achieve optimal activity, stability, and specificity simultaneously. Herein, a strategy of stepwise targeted coordination engineering is introduced to co‐anchor Pt single atoms (Pt1, 1.41 wt.%) and Au25(SG)18 nanoclusters (Au25, 18.92 wt.%) with high loadings on graphitic carbon nitride (g‐C3N4). This approach ensures that Pt1 and Au25 occupy distinct surface sites on the g‐C3N4 substrate, providing excellent stability and unprecedented electrochemical activity. In the catalysis of As(III), a sensitivity of 8.32 µA ppb−1 is achieved, more than double the previously reported values under neutral conditions. The enhanced detection limit (0.2 ppb) is crucial for monitoring water quality and protecting public health from arsenic contamination, a significant environmental and health risk. Furthermore, the formation of Pt─As and As─S bonds facilitates the easier breakage of As─O bonds, thereby lowering the reaction barrier energy of the rate‐determining step and significantly enhancing arsenious acid catalysis efficiency. These results not only offer an intriguing strategy for constructing highly efficient heterogeneous dual‐site catalysts but also reveal the atomic‐scale catalytic mechanisms that drive enhanced catalytic efficiency.
Article Details
Authors (14)
Xiangyu Xiao
Key Laboratory of Organic Compound Pollution Control Engineering (MOE) School of Environmental and Chemical Engineering Shanghai University Shanghai 200444 P. R. China
Pei‐Hua Li
Key Laboratory of Environmental Optics and Technology And Environmental Materials and Pollution Control Laboratory Institute of Solid State Physics HFIPS Chinese Academy of Sciences Hefei 230031 P. R. China
Liang Tang
Deli Wu
State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science & Engineering Tongji University Shanghai 200092 P. R. China
Huarong Xia
Innovative Centre for Flexible Devices (iFLEX), Max Planck-NTU Joint Lab for Artificial Senses, School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Republic of Singapore
Zong‐Yin Song
Key Laboratory of Environmental Optics and Technology And Environmental Materials and Pollution Control Laboratory Institute of Solid State Physics HFIPS Chinese Academy of Sciences Hefei 230031 P. R. China
Yong‐Huan Zhao
Key Laboratory of Environmental Optics and Technology And Environmental Materials and Pollution Control Laboratory Institute of Solid State Physics HFIPS Chinese Academy of Sciences Hefei 230031 P. R. China
Bo Liang
Meng Yang
Rui Tang
Institute of Chemical Biology and Nanomedicine, State Key Laboratory of Chemo and Biosensing, Hunan Provincial Key Laboratory of Biomacromolecular Chemical Biology, College of Chemistry and Chemical Engineering
Jingyi Yao
Key Laboratory of Organic Compound Pollution Control Engineering (MOE) School of Environmental and Chemical Engineering Shanghai University Shanghai 200444 P. R. China
Xing‐Jiu Huang
Key Laboratory of Environmental Optics and Technology And Environmental Materials and Pollution Control Laboratory Institute of Solid State Physics HFIPS Chinese Academy of Sciences Hefei 230031 China
Xiaodong Chen
Innovative Centre for Flexible Devices (iFLEX), Max Planck-NTU Joint Lab for Artificial Senses, School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Republic of Singapore
Zhendong Lei