Promoting oxygen reduction kinetics of single Fe sites for robust neutral Zn-air batteries via engineering synergistic Fe nanocluster as proton-feeding center

Xu, Ren1,2; Wang, Xingkun1,2; Sun, Mingzi3; Zhang, Canhui1; Li, Cheng5,6; Cao, Zhengwen2; Gu, Meng4,5; Huang, Bolong3; Huang, Minghua1

2023-11-01

10.1016/j.cej.2023.146065

CHEMICAL ENGINEERING JOURNAL   Impact Factor & Quartile

1385-8947

1873-3212

Constructing highly efficient and cost-effective catalysts for neutral oxygen reduction reaction (ORR) remains extremely challenging due to the sluggish reaction kinetics resulting from the low ionic conductivity and limited OH- concentration in the neutral electrolytes. Herein, we intentionally integrate the atomic Fe-N4 sites and Fe nanoclusters on N-doped multimodally porous carbon (FeSA+NC@NMPC) to achieve coherent optimization of rapid oxygen-containing intermediate conversions and fast water dissociation to provide abundant protons for boosting neutral ORR performance. As expected, the FeSA+NC@NMPC exhibits an excellent half-wave potential of 0.76 V in 0.1 M phosphate buffer solutions, outperforming that of commercial Pt/C (0.73 V). Theoretical cal-culations reveal the synergistic effect between atomic Fe-N4 sites and Fe nanoclusters, in which the former possess stable O2 adsorption and rapid intermediate conversion, while the latter facilitates fast water dissociation to supply protons for accelerating the proton-coupled electron transfer process. Moreover, the FeSA+NC@NMPC- based neutral zinc-air batteries afford a high open-circuit potential of 1.42 V and outstanding cycling stability at 5 mA cm-2 for 100 h. This work utilizes the advantages of both single sites and clusters of Fe to provide an in-depth understanding of the neutral ORR mechanism and advances the development of related energy storage and conversion technologies.

Oxygen reduction reaction Fe single atomic sites Water dissociation Synergistic effect Neutral Zinc -air batteries

SCI

English

Corresponding

National Natural Science Foundation of China["22279124","52261145700"] ; Natural Science Foundation of Shandong Province[ZR2022ZD30] ; National Key Research and Development Project["2022YFA1503900","2022YFA1203400"] ; Guangdong scientific program[2019QN01L057] ; National Natural Science Foundation of China/Research Grant Council of Hong Kong Joint Research Scheme[N_PolyU502/21] ; Shenzhen Fundamental Research Scheme-General Program[JCYJ20220531090807017]

Engineering

Engineering, Environmental ; Engineering, Chemical

WOS:001083157900001

ELSEVIER SCIENCE SA

ENGINEERING

Web of Science

1.Ocean Univ China, Sch Mat Sci & Engn, Qingdao 266100, Peoples R China
2.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Qingdao 266101, Peoples R China
3.Hong Kong Polytech Univ, Dept Appl Biol & Chem Technol, Hung Hom, Kowloon, Hong Kong, Peoples R China
4.Eastern Inst Technol, Eastern Inst Adv Study, Ningbo 315200, Zhejiang, Peoples R China
5.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
6.Univ Birmingham, Sch Phys & Astron, Birmingham B15 2TT, England

Xu, Ren,Wang, Xingkun,Sun, Mingzi,et al. Promoting oxygen reduction kinetics of single Fe sites for robust neutral Zn-air batteries via engineering synergistic Fe nanocluster as proton-feeding center[J]. CHEMICAL ENGINEERING JOURNAL,2023,475.

Xu, Ren.,Wang, Xingkun.,Sun, Mingzi.,Zhang, Canhui.,Li, Cheng.,...&Huang, Minghua.(2023).Promoting oxygen reduction kinetics of single Fe sites for robust neutral Zn-air batteries via engineering synergistic Fe nanocluster as proton-feeding center.CHEMICAL ENGINEERING JOURNAL,475.

Xu, Ren,et al."Promoting oxygen reduction kinetics of single Fe sites for robust neutral Zn-air batteries via engineering synergistic Fe nanocluster as proton-feeding center".CHEMICAL ENGINEERING JOURNAL 475(2023).