Surface-enriched ultrafine Pt nanoparticles coupled with defective CoP as efficient trifunctional electrocatalyst for overall water splitting and flexible Zn-air battery

doi:10.1016/S1872-2067(22)64198-6

Chinese Journal of Catalysis ›› 2023, Vol. 46: 36-47.DOI: 10.1016/S1872-2067(22)64198-6

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Surface-enriched ultrafine Pt nanoparticles coupled with defective CoP as efficient trifunctional electrocatalyst for overall water splitting and flexible Zn-air battery

Zexing Wu^a, Yuxiao Gao^a, Zixuan Wang^a, Weiping Xiao^c, Xinping Wang^a, Bin Li^d^,^*(), Zhenjiang Li^d, Xiaobin Liu^b, Tianyi Ma^e, Lei Wang^a^,^b^,^*()

^aKey Laboratory of Eco-chemical Engineering, Ministry of Education, International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China
^bShandong Engineering Research Center for Marine Environment Corrosion and Safety Protection, College of Environment and Safety Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China
^cCollege of Science, Nanjing Forestry University, Nanjing 210037, Jiangsu, China
^dSchool of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China
^eSchool of Science, STEM College, RMIT University, Melbourne, Australia

Received:2022-09-06 Accepted:2022-11-23 Online:2023-03-18 Published:2023-02-21
Contact: *E-mail: binli@qust.edu.cn (B. Li), inorchemwl@126.com (L. Wang)
Supported by:
National Natural Science Foundation of China(22002068);National Natural Science Foundation of China(21971132);National Natural Science Foundation of China(52272222);National Natural Science Foundation of China(52072197);The China Postdoctoral Science Foundation(2021M691700);The Youth Innovation and Technology Foundation of Shandong Higher Education Institutions, China(2019KJC004);Outstanding Youth Foundation of Shandong Province, China(ZR2019JQ14);Taishan Scholar Young Talent Program(tsqn201909114);Major Scientific and Technological Innovation Project(2019JZZY020405);Major Basic Research Program of Natural Science Foundation of Shandong Province(ZR2020ZD09);The Natural Science Foundation of Shandong Province of China(ZR2019BB002);The Natural Science Foundation of Shandong Province of China(ZR2018BB031);Talent Foundation funded by Province and Ministry Co-construction Collaborative Innovation Center of Eco-chemical Engineering(STHGYX2202);The Postdoctoral Innovation Project of Shandong Province

Abstract

Abstract:

Developing multifunctional electrocatalysts toward energy-related reactions could reduce the cost and improve the utilization efficiency of raw materials. Herein, defective CoP decorated with ultrafine Pt nanoparticles (Pt/d-CoP/NPC) with multifunctional electrocatalytic performances is prepared via facile pyrolysis and following chemical reduction process. The as-synthesized Pt/d-CoP/NPC owns high half-wave potential of 0.82 V for oxygen reduction reaction with excellent stability in 0.1 mol/L KOH. Density functional theory calculations demonstrate that the adsorption energy of *OO at Pt/d-CoP/NPC is stronger compared to Pt, yielding higher catalytic activity for ORR. Moreover, the resultant electrocatalyst possesses excellent catalytic activities with low overpotentials toward hydrogen evolution reaction (33 mV in 1 mol/L KOH, 6 mV in 0.5 mol/L H₂SO₄ and 70 mV in 1 mol/L PBS) and oxygen evolution reaction (320 mV) at 10 mA/cm². Water-splitting and rechargeable Zn-air batteries assembled with the as-synthesized Pt/d-CoP/NPC as electrodes exhibit outstanding activity and long-range stability. Remarkably, sustainable energies and homemade Zn-air battery can efficiently drive the Pt/d-CoP/NPC electrolyzer with sumless hydrogen bubbles generated, verifying the potential applications for renewable energy storage.

Key words: Trifunctional electrocatalyst, Hydrogen/oxygen evolution reaction, Oxygen reduction reaction, Flexible Zn-air battery, CoP

Zexing Wu, Yuxiao Gao, Zixuan Wang, Weiping Xiao, Xinping Wang, Bin Li, Zhenjiang Li, Xiaobin Liu, Tianyi Ma, Lei Wang. Surface-enriched ultrafine Pt nanoparticles coupled with defective CoP as efficient trifunctional electrocatalyst for overall water splitting and flexible Zn-air battery[J]. Chinese Journal of Catalysis, 2023, 46: 36-47.

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Figures/Tables 8

Fig. 1. (a) The synthesis of Pt/d-CoP/NPC. (b) XRD pattern of Pt/d-CoP/NPC. Low (c) and high (d) TEM images of Pt/d-CoP/NPC. (e) The electron paramagnetic resonance spectra of CoP/NPC and d-CoP/NPC. (f?j) EDX mappings of N, C, P, Pt and Co for Pt/d-CoP/NPC.

Fig. 2. (a) The XPS survey scan of Pt/d-CoP/NPC. (b) The P 2p spectrum of Pt/d-CoP/NPC. (c) The Co 2p spectrum of Pt/d-CoP/NPC and d-CoP/NPC. (d) The Pt 4f spectrum of Pt/d-CoP/NPC and Pt/C. (e) The Raman spectrum of Pt/d-CoP/NPC and d-CoP/NPC. (f) The FTIR spectrum of Pt/d-CoP/NPC.

Fig. 3. (a) The LSVs of CoP/NPC, d-CoP/NPC, Pt/d-CoP/NPC and Pt/C in 0.1 mol/L KOH. (b) The LSVs of Pt/d-CoP/NPC at different rotating rates and the K-L plots (inset). (c) The comparison of mass activity for Pt/d-CoP/NPC and Pt/C. (d) The electron transfer number and yield of H2O2 for Pt/d-CoP/NPC. (e) The current-time test of Pt/d-CoP/NPC at 0.82 V. (f) The comparison of half-wave potential of Pt/d-CoP/NPC and the recently reported electrocatalysts.

Fig. 4. (a) Reaction intermediates adsorption configurations on Pt/d-CoP/NPC (Pt site) for ORR. (b) The differential charge density distributions between adsorbed Pt and CoP. (c) Free energy diagrams of ORR for Pt/d-CoP/NPC and Pt (111). (d) The density of states (DOS) of Pt/d-CoP/NPC.

Fig. 5. (a) The LSVs of CoP/NPC, d-CoP/NPC, Pt/d-CoP/NPC and RuO2 in 1 mol/L KOH for OER and the overpotential in 10 and 100 mA/cm2 of CoP/NPC, d-CoP/NPC, Pt/d-CoP/NPC and RuO2 (inset). (b) The illustration of the Zn-air battery device. (c) The open-circuit voltage of liquid rechargeable Zn-air battery for Pt/d-CoP/NPC. (d) The charge and discharge polarization curves of Pt/d-CoP/NPC in liquid Zn-air battery. (e) The power density of Pt/d-CoP/NPC in liquid Zn-air battery. (f) The stability of charge and discharge in liquid Zn-air battery. (g) The stability of charge and discharge of Pt/d-CoP/NPC in flexible battery. (h) The small fans spin driven by flexible battery.

Fig. 6. (a) LSV curves of CoP/NPC, d-CoP/NPC, Pt/d-CoP/NPC and Pt/C for HER in 1 mol/L KOH. (b) Double layer capacitance of the samples. (c) In situ Raman spectroscopy analysis of HER for Pt/d-CoP/NPC. (d) LSVs in 0.5 mol/L H2SO4 of CoP/NPC, d-CoP/NPC, Pt/d-CoP/NPC and Pt/C for HER. (e) Tafel plots of researched samples in 0.5 mol/L H2SO4. (f) Comparison of Pt/d-CoP/NPC with related reported work. (g) LSVs in 1 mol/L PBS of CoP/NPC, d-CoP/NPC, Pt/d-CoP/NPC and Pt/C for HER. (h) Tafel plots in 1 mol/L PBS of CoP/NPC, d-CoP/NPC, Pt/d-CoP/NPC and Pt/C. (i) Stability test of Pt/d-CoP/NPC performed in 1 mol/L PBS for 24 h under a constant potential of -196 mV (no iR compensation).

Fig. 7. (a) Single electrolytic cell in 1 mol/L KOH of the overall water-splitting. (b) The cell voltage of Pt/d-CoP/NPC and related reporting work. (c) Stability test of Pt/d-CoP/NPC || Pt/d-CoP/NPC at a cell voltage of 1.54 V. (d) The Stirling engine driven by overall water-splitting using Pt/d-CoP/NPC || Pt/d-CoP/NPC and the photo of bubbles. (e) The photo of bubbles for wind energy powering the overall water-splitting cell. (f) Self-assembled rechargeable flexible Zn-air battery connected to Pt/d-CoP/NPC || Pt/d-CoP/NPC.

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Surface-enriched ultrafine Pt nanoparticles coupled with defective CoP as efficient trifunctional electrocatalyst for overall water splitting and flexible Zn-air battery

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