Citation: Zheng-Min Wang, Qing-Ling Hong, Xiao-Hui Wang, Hao Huang, Yu Chen, Shu-Ni Li. RuP Nanoparticles Anchored on N-doped Graphene Aerogels for Hydrazine Oxidation-Boosted Hydrogen Production[J]. Acta Physico-Chimica Sinica, ;2023, 39(12): 230302. doi: 10.3866/PKU.WHXB202303028 shu

RuP Nanoparticles Anchored on N-doped Graphene Aerogels for Hydrazine Oxidation-Boosted Hydrogen Production

Zheng-Min Wang ¹ ,
Qing-Ling Hong ² ,
Xiao-Hui Wang ¹ ,
Hao Huang ^3,, ,
Yu Chen ^2,, ,
Shu-Ni Li ^1,,

1.
Key Laboratory of Macromolecular Science of Shaanxi Province, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an 710062, China
2.
School of Materials Science and Engineering, Shaanxi Normal University, Xi'an 710062, China
3.
Department of Microsystems, University of South-Eastern Norway, Borre 3184, Norway

Corresponding author: Hao Huang, huanghao881015@163.com Yu Chen, ndchenyu@gmail.com Shu-Ni Li, lishuni@snnu.edu.cn
Received Date: 13 March 2023
Revised Date: 3 April 2023
Accepted Date: 4 April 2023
Available Online: 10 April 2023
Fund Project: the National Natural Science Foundation of China 21972089the National Natural Science Foundation of China 22002083the Science and Technology Innovation Team of Shaanxi Province 2023-CX-TD-27the Fundamental Research Funds for the Central Universities GK202202001

'Green hydrogen' is a promising clean energy carrier for use instead of traditional fuels. For obtaining 'green hydrogen', electrochemical water splitting has been receiving considerable attention due to its eco-friendly and low-cost properties. However, the sluggish kinetics of the anodic oxygen evolution reaction (OER) reduces the efficiency of hydrogen production. Accordingly, the hydrazine oxidation reaction (HzOR) with low theoretical potential (−0.33 V vs. RHE) has been proposed as a reasonable alternative for the OER. In this study, graphene aerogel (GA) was utilized as a conductive substrate with a 3D porous framework. Ru^Ⅲ-polyethyleneimine (Ru^Ⅲ-PEI) complexes were adsorbed on the GA surface. Phytic acid (PA) was further adsorbed to form Ru^Ⅲ-PEI-GA-PA hybrids through the hydrogen bond interaction between PA and PEI, which can serve as a precursor to synthesize RuP nanoparticles anchored on N-doped GA (RuP/N-GA) through the phosphorization reaction. In the pyrolysis process, the ultra-small RuP was formed at the GA surface. Additionally, the decomposition of PEI and PA can introduce abundant N and P heteroatoms into the structure of GA. As a result, RuP/N-GA hybrids achieve efficient HzOR with a low working potential of −54 mV at 10 mA∙cm⁻². Moreover, the novel RuP/N-GA hybrids with low Ru loading also exhibit a promising hydrogen evolution reaction (HER) activity with an overpotential of −19.6 mV at 10 mA∙cm⁻². Among various RuP/N-GA hybrids, the Tafel plot of HER at RuP/N-GA-900 reveals the smallest value to be 37.03 mV∙dec⁻¹, which affords the fastest HER kinetics. Meanwhile, the result suggests that the HER at RuP/N-GA-900 undergoes a Heyrovsky mechanism similar to that of Pt. The theoretical results revealed that the anchored structure and the presence of N heteroatoms can promote the HzOR on RuP nanoparticles. The free energy of hydrazine molecular adsorption on RuP/N-GA was −0.68 eV, indicating that N-doping in the RuP/N-GA structure can adjust the electronic structure of the Ru active site, which also contributes to the enhanced HzOR activity of the Ru site. Additionally, RuP/N-GA hybrids exhibited excellent cycling and long-term stability for both HER and HzOR, superior to those of commercial Pt/C. Based on the bifunctional activity of RuP/N-GA hybrids, the constructed two-electrode hydrazine split system exhibits an extremely low cell voltage of 41 mV at 10 mA∙cm⁻² for the hydrogen production, which achieves the goal of energy-saved hydrogen production at low voltage. The excellent electrocatalytic activity of RuP/N-GA hybrids is attributed to the ultrasmall RuP nanoparticles for abundant Ru active sites. Meanwhile, the synergistic effect between N-doping in GA frameworks with RuP nanoparticles contributes to the activity enhancement of RuP/N-GA hybrids, in which the 3D porous N-GA with few-layer morphology accelerates the electron and mass transfer and the electron interaction between N-GA and RuP nanoparticles promotes the electrocatalytic activity of RuP nanoparticles for both HER and HzOR. This study extends the bifunctional electrocatalyst for the HER and HzOR to achieve energy-saved hydrogen production and sheds new light on the design and synthesis of advanced electrocatalysts via the adsorption-phosphatization method.
- Ruthenium phosphide,
- Graphene aerogel,
- Anchored structure,
- Hydrazine oxidation reaction,
- Hydrogen evolution reaction
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