Single palladium site in ordered porous heteroatom-doped carbon for high-performance alkaline hydrogen oxidation

Haoxuan Liu; Jiantao Fu; Hongyi Li; Jiaqiang Sun; Xijun Liu; Yuan Qiu; Xianyun Peng; Yifan Liu; Haihong Bao; Longchao Zhuo; Rui Cao; Shusheng Zhang; Jun Luo

doi:10.1016/j.apcatb.2021.121029

Single palladium site in ordered porous heteroatom-doped carbon for high-performance alkaline hydrogen oxidation

Haoxuan Liu, Jiantao Fu, Hongyi Li, Jiaqiang Sun, Xijun Liu, Yuan Qiu, Xianyun Peng, Yifan Liu, Haihong Bao, Longchao Zhuo, Rui Cao, Shusheng Zhang, Jun Luo

Research output: Contribution to journal › Article › peer-review

77 Scopus citations

Abstract

Alkaline exchange membrane fuel cells are impeded by the lack of cost-effective, highly efficient catalysts for the sluggish hydrogen oxidation reaction (HOR). Herein, single-atomic Pd sites supported by ordered porous N,S-doped carbon are synthesized, exhibiting remarkable alkaline HOR performance. This catalyst exhibits an ultrahigh anodic current density and mass-specific kinetic current of 2.01 mA cm^–2 and 27,719 A g_Pd^–1 (at an overpotential of 50 mV), respectively, not only outperforming the Pt/C counterpart but also making it among the best reported HOR catalysts. Furthermore, this catalyst exhibits a negligible activity decay during long-term electrolysis and a good CO tolerance capability. Experiments and theoretical calculations indicate that the synergistic effect from single Pd sites and heteroatom doping (N and S) weakens the binding energy of H_ad intermediates, thereby accounting for its superior HOR activity. This study provides a guideline for developing single-atomic site catalysts for highly efficient, stable alkaline HOR.

Original language	English
Article number	121029
Journal	Applied Catalysis B: Environmental
Volume	306
DOIs	https://doi.org/10.1016/j.apcatb.2021.121029
State	Published - Jun 5 2022
Externally published	Yes

Funding

This work was financially supported by National Natural Science Foundation of China ( 51971157 , 22075211 , 21601136 , and 51621003 ), the Tianjin Science Fund for Distinguished Young Scholars ( 19JCJQJC61800 ), and the Guangzhou Panyu Polytechnic Science & Technology Project No. 2021KJ01 . The authors also acknowledged Beijing Super Cloud Computing Center for providing the computational resources.

Funders	Funder number
Guangzhou Panyu Polytechnic Science & Technology Project	2021KJ01
Tianjin Science Fund for Distinguished Young Scholars	19JCJQJC61800
National Natural Science Foundation of China	21601136, 51621003, 51971157, 22075211

Keywords

Alkaline hydrogen oxidation
Hydrogen fuel cells
Ordered porous carbon
Single-atomic Pd sites
Synergistic effect

UN SDGs

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

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10.1016/j.apcatb.2021.121029

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title = "Single palladium site in ordered porous heteroatom-doped carbon for high-performance alkaline hydrogen oxidation",

abstract = "Alkaline exchange membrane fuel cells are impeded by the lack of cost-effective, highly efficient catalysts for the sluggish hydrogen oxidation reaction (HOR). Herein, single-atomic Pd sites supported by ordered porous N,S-doped carbon are synthesized, exhibiting remarkable alkaline HOR performance. This catalyst exhibits an ultrahigh anodic current density and mass-specific kinetic current of 2.01 mA cm–2 and 27,719 A gPd–1 (at an overpotential of 50 mV), respectively, not only outperforming the Pt/C counterpart but also making it among the best reported HOR catalysts. Furthermore, this catalyst exhibits a negligible activity decay during long-term electrolysis and a good CO tolerance capability. Experiments and theoretical calculations indicate that the synergistic effect from single Pd sites and heteroatom doping (N and S) weakens the binding energy of Had intermediates, thereby accounting for its superior HOR activity. This study provides a guideline for developing single-atomic site catalysts for highly efficient, stable alkaline HOR.",

keywords = "Alkaline hydrogen oxidation, Hydrogen fuel cells, Ordered porous carbon, Single-atomic Pd sites, Synergistic effect",

author = "Haoxuan Liu and Jiantao Fu and Hongyi Li and Jiaqiang Sun and Xijun Liu and Yuan Qiu and Xianyun Peng and Yifan Liu and Haihong Bao and Longchao Zhuo and Rui Cao and Shusheng Zhang and Jun Luo",

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doi = "10.1016/j.apcatb.2021.121029",

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T1 - Single palladium site in ordered porous heteroatom-doped carbon for high-performance alkaline hydrogen oxidation

AU - Liu, Haoxuan

AU - Fu, Jiantao

AU - Li, Hongyi

AU - Sun, Jiaqiang

AU - Liu, Xijun

AU - Qiu, Yuan

AU - Peng, Xianyun

AU - Liu, Yifan

AU - Bao, Haihong

AU - Zhuo, Longchao

AU - Cao, Rui

AU - Zhang, Shusheng

AU - Luo, Jun

PY - 2022/6/5

Y1 - 2022/6/5

N2 - Alkaline exchange membrane fuel cells are impeded by the lack of cost-effective, highly efficient catalysts for the sluggish hydrogen oxidation reaction (HOR). Herein, single-atomic Pd sites supported by ordered porous N,S-doped carbon are synthesized, exhibiting remarkable alkaline HOR performance. This catalyst exhibits an ultrahigh anodic current density and mass-specific kinetic current of 2.01 mA cm–2 and 27,719 A gPd–1 (at an overpotential of 50 mV), respectively, not only outperforming the Pt/C counterpart but also making it among the best reported HOR catalysts. Furthermore, this catalyst exhibits a negligible activity decay during long-term electrolysis and a good CO tolerance capability. Experiments and theoretical calculations indicate that the synergistic effect from single Pd sites and heteroatom doping (N and S) weakens the binding energy of Had intermediates, thereby accounting for its superior HOR activity. This study provides a guideline for developing single-atomic site catalysts for highly efficient, stable alkaline HOR.

AB - Alkaline exchange membrane fuel cells are impeded by the lack of cost-effective, highly efficient catalysts for the sluggish hydrogen oxidation reaction (HOR). Herein, single-atomic Pd sites supported by ordered porous N,S-doped carbon are synthesized, exhibiting remarkable alkaline HOR performance. This catalyst exhibits an ultrahigh anodic current density and mass-specific kinetic current of 2.01 mA cm–2 and 27,719 A gPd–1 (at an overpotential of 50 mV), respectively, not only outperforming the Pt/C counterpart but also making it among the best reported HOR catalysts. Furthermore, this catalyst exhibits a negligible activity decay during long-term electrolysis and a good CO tolerance capability. Experiments and theoretical calculations indicate that the synergistic effect from single Pd sites and heteroatom doping (N and S) weakens the binding energy of Had intermediates, thereby accounting for its superior HOR activity. This study provides a guideline for developing single-atomic site catalysts for highly efficient, stable alkaline HOR.

KW - Alkaline hydrogen oxidation

KW - Hydrogen fuel cells

KW - Ordered porous carbon

KW - Single-atomic Pd sites

KW - Synergistic effect

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Single palladium site in ordered porous heteroatom-doped carbon for high-performance alkaline hydrogen oxidation

Abstract

Funding

Keywords

UN SDGs

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