Coupling atom ensemble and electron transfer in PdCu for superior catalytic kinetics in hydrogen generation
The design of high-performance catalysts is the key to the efficient utilization of hydrogen energy. In this work, a PdCu nanoalloy was successfully anchored on TiO 2 encapsulated with carbon to construct a catalyst. Outstanding kinetics of the hydrolysis of ammonia borane (turnover frequency of 279...
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| Published in | Nano research Vol. 16; no. 7; pp. 9012 - 9021 |
|---|---|
| Main Authors | , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Beijing
Tsinghua University Press
01.07.2023
Springer Nature B.V |
| Subjects | |
| Online Access | Get full text |
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| Abstract | The design of high-performance catalysts is the key to the efficient utilization of hydrogen energy. In this work, a PdCu nanoalloy was successfully anchored on TiO
2
encapsulated with carbon to construct a catalyst. Outstanding kinetics of the hydrolysis of ammonia borane (turnover frequency of 279
mol
H
2
⋅
min
−
1
⋅
mol
Pd
−
1
) ranking the third place among Pd-based catalysts was achieved in the absence of alkali. Both experimental research and theoretical calculations reveal a lower activation energy of the B-H bond on the PdCu nanoalloy catalyst than that on pristine Pd and a lower activation energy of the O-H bond than that on pristine Cu. The redistribution of d electron and the shift of the d-band center play a critical role in increasing the electron density of Pd and improving the catalytic performances of Pd
0.1
Cu
0.9
/TiO
2
-porous carbon (Pd
0.1
Cu
0.9
/T-PC). This work provides novel insights into highly dual-active alloys and sheds light on the mechanism of dual-active sites in promoting borohydride hydrolysis. |
|---|---|
| AbstractList | The design of high-performance catalysts is the key to the efficient utilization of hydrogen energy. In this work, a PdCu nanoalloy was successfully anchored on TiO
2
encapsulated with carbon to construct a catalyst. Outstanding kinetics of the hydrolysis of ammonia borane (turnover frequency of 279
mol
H
2
⋅
min
−
1
⋅
mol
Pd
−
1
) ranking the third place among Pd-based catalysts was achieved in the absence of alkali. Both experimental research and theoretical calculations reveal a lower activation energy of the B-H bond on the PdCu nanoalloy catalyst than that on pristine Pd and a lower activation energy of the O-H bond than that on pristine Cu. The redistribution of d electron and the shift of the d-band center play a critical role in increasing the electron density of Pd and improving the catalytic performances of Pd
0.1
Cu
0.9
/TiO
2
-porous carbon (Pd
0.1
Cu
0.9
/T-PC). This work provides novel insights into highly dual-active alloys and sheds light on the mechanism of dual-active sites in promoting borohydride hydrolysis. The design of high-performance catalysts is the key to the efficient utilization of hydrogen energy. In this work, a PdCu nanoalloy was successfully anchored on TiO2 encapsulated with carbon to construct a catalyst. Outstanding kinetics of the hydrolysis of ammonia borane (turnover frequency of 279 molH2⋅min−1⋅molPd−1) ranking the third place among Pd-based catalysts was achieved in the absence of alkali. Both experimental research and theoretical calculations reveal a lower activation energy of the B-H bond on the PdCu nanoalloy catalyst than that on pristine Pd and a lower activation energy of the O-H bond than that on pristine Cu. The redistribution of d electron and the shift of the d-band center play a critical role in increasing the electron density of Pd and improving the catalytic performances of Pd0.1Cu0.9/TiO2-porous carbon (Pd0.1Cu0.9/T-PC). This work provides novel insights into highly dual-active alloys and sheds light on the mechanism of dual-active sites in promoting borohydride hydrolysis. |
| Author | Guan, Shuyan Li, Baojun Mehdi, Sehrish Yuan, Huiyu Liu, Baozhong Wen, Hao Zhang, Huanhuan Zhao, Xinru Fan, Yanping Shen, Ruofan Guo, Xianji Ashraf, Saima Liu, Yanyan Liu, Tao |
| Author_xml | – sequence: 1 givenname: Xinru surname: Zhao fullname: Zhao, Xinru organization: College of Chemistry and Chemical Engineering, Henan Polytechnic University – sequence: 2 givenname: Yanyan surname: Liu fullname: Liu, Yanyan organization: College of Chemistry and Chemical Engineering, Henan Polytechnic University, College of Science, Henan Agriculture University – sequence: 3 givenname: Huiyu surname: Yuan fullname: Yuan, Huiyu organization: College of Materials Science and Engineering, Zhengzhou University – sequence: 4 givenname: Hao surname: Wen fullname: Wen, Hao organization: Research Center of Green Catalysis, College of Chemistry, College of Mechanical and Power Engineering, Zhengzhou University – sequence: 5 givenname: Huanhuan surname: Zhang fullname: Zhang, Huanhuan organization: College of Chemistry and Chemical Engineering, Henan Polytechnic University, Research Center of Green Catalysis, College of Chemistry, College of Mechanical and Power Engineering, Zhengzhou University – sequence: 6 givenname: Saima surname: Ashraf fullname: Ashraf, Saima organization: Research Center of Green Catalysis, College of Chemistry, College of Mechanical and Power Engineering, Zhengzhou University – sequence: 7 givenname: Shuyan surname: Guan fullname: Guan, Shuyan organization: College of Chemistry and Chemical Engineering, Henan Polytechnic University, Research Center of Green Catalysis, College of Chemistry, College of Mechanical and Power Engineering, Zhengzhou University – sequence: 8 givenname: Tao surname: Liu fullname: Liu, Tao organization: CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety, National Centre for Nanoscience and Technology – sequence: 9 givenname: Sehrish surname: Mehdi fullname: Mehdi, Sehrish organization: Research Center of Green Catalysis, College of Chemistry, College of Mechanical and Power Engineering, Zhengzhou University – sequence: 10 givenname: Ruofan surname: Shen fullname: Shen, Ruofan organization: Research Center of Green Catalysis, College of Chemistry, College of Mechanical and Power Engineering, Zhengzhou University – sequence: 11 givenname: Xianji surname: Guo fullname: Guo, Xianji organization: Research Center of Green Catalysis, College of Chemistry, College of Mechanical and Power Engineering, Zhengzhou University – sequence: 12 givenname: Yanping surname: Fan fullname: Fan, Yanping organization: College of Chemistry and Chemical Engineering, Henan Polytechnic University – sequence: 13 givenname: Baozhong surname: Liu fullname: Liu, Baozhong email: HPUliuking@163.com organization: College of Chemistry and Chemical Engineering, Henan Polytechnic University, State Collaborative Innovation Center of Coal Work Safety and Clean-efficiency Utilization – sequence: 14 givenname: Baojun surname: Li fullname: Li, Baojun email: lbjfcl@zzu.edu.cn organization: College of Chemistry and Chemical Engineering, Henan Polytechnic University, Research Center of Green Catalysis, College of Chemistry, College of Mechanical and Power Engineering, Zhengzhou University, Department of Chemistry, Tsinghua University |
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| Keywords | ensemble effect borohydride hydrolysis d-band holes PdCu nanoalloy dual-active sites |
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| Snippet | The design of high-performance catalysts is the key to the efficient utilization of hydrogen energy. In this work, a PdCu nanoalloy was successfully anchored... |
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| SubjectTerms | Activation energy Alloys Ammonia Atomic/Molecular Structure and Spectra Biomedicine Biotechnology Carbon Catalysts Chemistry and Materials Science Condensed Matter Physics Electron density Electron transfer Energy Experimental research Hydrogen Hydrogen bonds Hydrogen production Hydrolysis Kinetics Materials Science Nanoalloys Nanocomposites Nanoparticles Nanotechnology Palladium Reaction kinetics Research Article Titanium dioxide |
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| Title | Coupling atom ensemble and electron transfer in PdCu for superior catalytic kinetics in hydrogen generation |
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