Rh-doped PdAg nanoparticles as efficient methanol tolerance electrocatalytic materials for oxygen reduction

Yingjun Sun; Bolong Huang; Nuoyan Xu; Yingjie Li; Mingchuan Luo; Chunji Li; Yingnan Qin; Lei Wang; Shaojun Guo

doi:10.1016/j.scib.2018.12.008

Rh-doped PdAg nanoparticles as efficient methanol tolerance electrocatalytic materials for oxygen reduction

Yingjun Sun, Bolong Huang, Nuoyan Xu, Yingjie Li, Mingchuan Luo, Chunji Li, Yingnan Qin, Lei Wang, Shaojun Guo^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

36 Citations (Scopus)

Abstract

Direct methanol fuel cells (DMFCs) have received extensive attention on their high efficiency, high reliability, and no carbon emission. Unfortunately, the poor methanol tolerance and sluggish oxygen reduction reaction (ORR) at cathode have seriously hindered their further development. Herein we report the synthesis of a new class of Rh-doped PdAg alloy nanoparticles (NPs) for boosting ORR activity with high methanol tolerance capacity concurrently. The ORR mass activity of typical Rh₄Pd₄₀Ag₅₆ NPs is 4.2 times higher than that of commercial Pt catalyst. Moreover, it shows a great methanol tolerance capability by maintaining 92.4% in ORR mass activity in alkaline solution with 0.1 mol L⁻¹ methanol, against a big decrease of almost 100% for commercial Pt. Even after 30,000 potential cycles with 1.0 mol L⁻¹ methanol, Rh₄Pd₄₀Ag₅₆ NPs still retain ORR mass activity of up to 68.3%. DFT calculations reveal that excellent ORR performance with excellent methanol tolerance originates the active d-band-pinning engineering for an efficient site-independent electron-transfer. A generalized d-band mediated fine electron-transfer tuning path has blueprinted for effectively minimizing intrinsic ORR barriers with high current density. The present work highlights the key role of Rh doping in enhancing the ORR activity and methanol tolerance ability of PdAg NPs for future high-performance DMFCs. © 2018 Science China Press

Original language	English
Pages (from-to)	54-62
Journal	Science Bulletin
Volume	64
Issue number	1
DOIs	https://doi.org/10.1016/j.scib.2018.12.008
Publication status	Published - 15 Jan 2019
Externally published	Yes

Bibliographical note

Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

Funding

This work was financially supported by the National Natural Science Foundation of China (NSFC) (51671003), National Basic Research Program of China (2017YFA0206701), the China Postdoctoral Science Foundation (2017M620526 and 2017M620518), Open Project Foundation of State Key Laboratory of Chemical Resource Engineering, the Start-up Supports from Peking University and Young Thousand Talented Program, and Early Career Scheme (ECS) fund (PolyU 253026/16P) from the Research Grant Council (RGC) in Hong Kong.

Research Keywords

Fuel cells
Methanol tolerance
Multimetallic
Oxygen reduction
Rh-doped

RGC Funding Information

RGC-funded

UN SDGs

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

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title = "Rh-doped PdAg nanoparticles as efficient methanol tolerance electrocatalytic materials for oxygen reduction",

abstract = "Direct methanol fuel cells (DMFCs) have received extensive attention on their high efficiency, high reliability, and no carbon emission. Unfortunately, the poor methanol tolerance and sluggish oxygen reduction reaction (ORR) at cathode have seriously hindered their further development. Herein we report the synthesis of a new class of Rh-doped PdAg alloy nanoparticles (NPs) for boosting ORR activity with high methanol tolerance capacity concurrently. The ORR mass activity of typical Rh4Pd40Ag56 NPs is 4.2 times higher than that of commercial Pt catalyst. Moreover, it shows a great methanol tolerance capability by maintaining 92.4% in ORR mass activity in alkaline solution with 0.1 mol L−1 methanol, against a big decrease of almost 100% for commercial Pt. Even after 30,000 potential cycles with 1.0 mol L−1 methanol, Rh4Pd40Ag56 NPs still retain ORR mass activity of up to 68.3%. DFT calculations reveal that excellent ORR performance with excellent methanol tolerance originates the active d-band-pinning engineering for an efficient site-independent electron-transfer. A generalized d-band mediated fine electron-transfer tuning path has blueprinted for effectively minimizing intrinsic ORR barriers with high current density. The present work highlights the key role of Rh doping in enhancing the ORR activity and methanol tolerance ability of PdAg NPs for future high-performance DMFCs. {\textcopyright} 2018 Science China Press",

keywords = "Fuel cells, Methanol tolerance, Multimetallic, Oxygen reduction, Rh-doped",

author = "Yingjun Sun and Bolong Huang and Nuoyan Xu and Yingjie Li and Mingchuan Luo and Chunji Li and Yingnan Qin and Lei Wang and Shaojun Guo",

note = "Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].",

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T1 - Rh-doped PdAg nanoparticles as efficient methanol tolerance electrocatalytic materials for oxygen reduction

AU - Sun, Yingjun

AU - Huang, Bolong

AU - Xu, Nuoyan

AU - Li, Yingjie

AU - Luo, Mingchuan

AU - Li, Chunji

AU - Qin, Yingnan

AU - Wang, Lei

AU - Guo, Shaojun

N1 - Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

PY - 2019/1/15

Y1 - 2019/1/15

N2 - Direct methanol fuel cells (DMFCs) have received extensive attention on their high efficiency, high reliability, and no carbon emission. Unfortunately, the poor methanol tolerance and sluggish oxygen reduction reaction (ORR) at cathode have seriously hindered their further development. Herein we report the synthesis of a new class of Rh-doped PdAg alloy nanoparticles (NPs) for boosting ORR activity with high methanol tolerance capacity concurrently. The ORR mass activity of typical Rh4Pd40Ag56 NPs is 4.2 times higher than that of commercial Pt catalyst. Moreover, it shows a great methanol tolerance capability by maintaining 92.4% in ORR mass activity in alkaline solution with 0.1 mol L−1 methanol, against a big decrease of almost 100% for commercial Pt. Even after 30,000 potential cycles with 1.0 mol L−1 methanol, Rh4Pd40Ag56 NPs still retain ORR mass activity of up to 68.3%. DFT calculations reveal that excellent ORR performance with excellent methanol tolerance originates the active d-band-pinning engineering for an efficient site-independent electron-transfer. A generalized d-band mediated fine electron-transfer tuning path has blueprinted for effectively minimizing intrinsic ORR barriers with high current density. The present work highlights the key role of Rh doping in enhancing the ORR activity and methanol tolerance ability of PdAg NPs for future high-performance DMFCs. © 2018 Science China Press

AB - Direct methanol fuel cells (DMFCs) have received extensive attention on their high efficiency, high reliability, and no carbon emission. Unfortunately, the poor methanol tolerance and sluggish oxygen reduction reaction (ORR) at cathode have seriously hindered their further development. Herein we report the synthesis of a new class of Rh-doped PdAg alloy nanoparticles (NPs) for boosting ORR activity with high methanol tolerance capacity concurrently. The ORR mass activity of typical Rh4Pd40Ag56 NPs is 4.2 times higher than that of commercial Pt catalyst. Moreover, it shows a great methanol tolerance capability by maintaining 92.4% in ORR mass activity in alkaline solution with 0.1 mol L−1 methanol, against a big decrease of almost 100% for commercial Pt. Even after 30,000 potential cycles with 1.0 mol L−1 methanol, Rh4Pd40Ag56 NPs still retain ORR mass activity of up to 68.3%. DFT calculations reveal that excellent ORR performance with excellent methanol tolerance originates the active d-band-pinning engineering for an efficient site-independent electron-transfer. A generalized d-band mediated fine electron-transfer tuning path has blueprinted for effectively minimizing intrinsic ORR barriers with high current density. The present work highlights the key role of Rh doping in enhancing the ORR activity and methanol tolerance ability of PdAg NPs for future high-performance DMFCs. © 2018 Science China Press

KW - Fuel cells

KW - Methanol tolerance

KW - Multimetallic

KW - Oxygen reduction

KW - Rh-doped

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DO - 10.1016/j.scib.2018.12.008

M3 - RGC 21 - Publication in refereed journal

SN - 2095-9273

VL - 64

SP - 54

EP - 62

JO - Science Bulletin

JF - Science Bulletin

IS - 1

ER -

Rh-doped PdAg nanoparticles as efficient methanol tolerance electrocatalytic materials for oxygen reduction

Abstract

Bibliographical note

Funding

Research Keywords

RGC Funding Information

UN SDGs

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