氮掺杂石墨烯气凝胶锚定RuP纳米粒子用于水合肼氧化辅助产氢

doi:10.3866/PKU.WHXB202303028

物理化学学报 >> 2023, Vol. 39 >> Issue (12): 2303028.doi: 10.3866/PKU.WHXB202303028

所属专题：能源电催化

论文上一篇

氮掺杂石墨烯气凝胶锚定RuP纳米粒子用于水合肼氧化辅助产氢

王正慜¹, 洪庆玲², 王晓慧¹, 黄昊³^,*(), 陈煜²^,*(), 李淑妮¹^,*()

¹ 陕西师范大学化学化工学院, 陕西省大分子科学重点实验室, 西安 710062
² 陕西师范大学材料科学与工程学院, 西安 710062
³ 挪威东南大学微系统系, 博尔 3184, 挪威

收稿日期:2023-03-13 录用日期:2023-04-04 发布日期:2023-04-10
通讯作者: 黄昊,陈煜,李淑妮 E-mail:huanghao881015@163.com;ndchenyu@gmail.com;lishuni@snnu.edu.cn
基金资助:
国家自然科学基金(21972089);国家自然科学基金(22002083);陕西省创新能力支撑计划(2023-CX-TD-27);中央高校基本科研业务费(GK202202001)

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

Zheng-Min Wang¹, Qing-Ling Hong², Xiao-Hui Wang¹, Hao Huang³^,*(), Yu Chen²^,*(), Shu-Ni Li¹^,*()

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

Received:2023-03-13 Accepted:2023-04-04 Published:2023-04-10
Contact: Hao Huang, Yu Chen, Shu-Ni Li E-mail:huanghao881015@163.com;ndchenyu@gmail.com;lishuni@snnu.edu.cn
Supported by:
the National Natural Science Foundation of China(21972089);the National Natural Science Foundation of China(22002083);the Science and Technology Innovation Team of Shaanxi Province(2023-CX-TD-27);the Fundamental Research Funds for the Central Universities(GK202202001)

1. WHXB202303028-SI-6p.pdf(1508KB)

摘要/Abstract

摘要：

氢能是替代传统燃料的理想清洁能源。电解水析氢由于其环保和低成本的特性而受到广泛关注，然而，阳极析氧反应(OER)的缓慢动力学降低了制氢效率。因此，肼氧化反应(HzOR)以其低的理论电压电位(−0.33 V vs. RHE)成为了OER的合理替代方案。本工作中，以三维多孔的石墨烯气凝胶(GA)为导电基底，将Ru^Ⅲ-聚乙烯亚胺(Ru^Ⅲ-PEI)配合物吸附在GA表面。通过植酸(PA)和PEI之间的氢键相互作用GA进一步吸附PA，形成Ru^Ⅲ-PEI-GA-PA复合物。对Ru^Ⅲ-PEI-GA-PA复合物前驱体进行磷化后，合成了锚定在N掺杂GA上的RuP纳米粒子(RuP/N-GA)。在热解过程中，在GA表面形成了超小的RuP纳米粒子。此外，PEI和PA的分解可以将丰富的N和P杂原子引入GA的结构中。因此，RuP/N-GA复合物具有高效的HzOR性能，在10 mA∙cm⁻²时的工作电位低至−54 mV。此外，这种低Ru负载的新型RuP/N-GA复合物具有良好的析氢反应(HER)活性，电流密度为10 mA∙cm⁻²时的HER过电势为−19.6 mV。在各种RuP/N-GA复合物中，RuP/N-GA-900具有最小的HER塔菲尔斜率(37.03 mV∙dec⁻¹)，表现出了最快的HER动力学。同时也表明RuP/N-GA-900的HER过程具有与Pt类似的Heyrovsky机制。理论计算结果表明，锚定结构和N杂原子的存在可以促进肼在RuP纳米粒子上的氧化。肼分子吸附在RuP/N-GA上的自由能为−0.68 eV，表明掺杂的N可以调节Ru活性位点的电子结构，有助于增强Ru的HzOR活性。此外，RuP/N-GA复合物对HER和HzOR均表现出优于商业Pt/C的循环稳定性和长期稳定性。基于RuP/N-GA复合物的双功能活性，所构建的双电极肼分解系统在10 mA∙cm⁻²下表现出41 mV的极低分解电压就可以产氢，实现了低电压下节能制氢的目标。RuP/N-GA复合物优异的电催化活性归因于超小的RuP纳米粒子提供了丰富的Ru活性位点。此外，GA骨架中N的掺杂与RuP纳米颗粒之间的协同效应有助于提高RuP/N-GA复合物的活性。三维多孔的N-GA加速了电荷转移和传质过程，并且N-GA和RuP纳米粒子之间的相互作用增强了RuP纳米粒子对HER和HzOR的电催化活性。这项工作提出了一种HzOR辅助制氢的双功能电催化剂，并为通过吸附-磷化法设计和合成先进电催化剂提供了新思路。

关键词: 磷化钌, 石墨烯气凝胶, 锚定结构, 肼氧化反应, 析氢反应

Abstract:

'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.

Key words: Ruthenium phosphide, Graphene aerogel, Anchored structure, Hydrazine oxidation reaction, Hydrogen evolution reaction

王正慜, 洪庆玲, 王晓慧, 黄昊, 陈煜, 李淑妮. 氮掺杂石墨烯气凝胶锚定RuP纳米粒子用于水合肼氧化辅助产氢[J]. 物理化学学报, 2023, 39(12), 2303028. doi: 10.3866/PKU.WHXB202303028

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 Phys. -Chim. Sin. 2023, 39(12), 2303028. doi: 10.3866/PKU.WHXB202303028

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202303028

https://www.whxb.pku.edu.cn/CN/Y2023/V39/I12/2303028

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Electrocatalyst	Electrolyte	Overpotential/mV	Ref.
RuP/N-GA-900	1 mol∙L⁻¹ KOH	19.6	This work
RuP nanoparticles	1 mol∙L⁻¹ KOH	22	14
RuP_x nanoparticles in N, P-codoped carbon nanospheres	1 mol∙L⁻¹ KOH	74	15
RuP nanoparticles	1 mol∙L⁻¹ KOH	31	16
RuP₂ in N, P-codoped carbon	1 mol∙L⁻¹ KOH	52	17
Ru nanocrystal	1 mol∙L⁻¹ KOH	81	29
Ru nanoparticles on multi-walled carbon nanotubes	1 mol∙L⁻¹ KOH	17	30
NiTe nanoarrays with RuO₂	1 mol∙L⁻¹ KOH	19	31
P-doped Ru supported on XC-72 carbon	1 mol∙L⁻¹ KOH	31	32
S-doped RuP nanoparticles in N, P, and S-codoped carbon	1 mol∙L⁻¹ KOH	92	33
Ru/CoO hybrid	1 mol∙L⁻¹ KOH	55	34
RuBe nanosheets	1 mol∙L⁻¹ KOH	34.8	35
Ru MOF-assisted CoFe nanoarrays	1 mol∙L⁻¹ KOH	50	36
Ru nanoparticles on N-doped porous carbon nanosheets	1 mol∙L⁻¹ KOH	50	37

Catalyst	Electrolyte	Work potential/mV	Ref.
RuP/N-GA-900	1.0 mol∙L⁻¹ KOH + 0.4 mol∙L⁻¹ N₂H₄	−54	This work
Ru single atoms into WO₃	1.0 mol∙L⁻¹ KOH + 0.5 mol∙L⁻¹ N₂H₄	−58	38
Ru nanoparticles on N-doped carbon	1.0 mol∙L⁻¹ KOH + 0.5 mol∙L⁻¹ N₂H₄	−39	39
RuP₂ nanoparticles on carbon microsheets	1.0 mol∙L⁻¹ KOH + 0.3 mol∙L⁻¹ N₂H₄	−70	40
CoRuO_x in N-doped carbon shell	1.0 mol∙L⁻1 KOH + 0.5 mol∙L⁻¹ N₂H₄	−19	41
carbon-coated RuP₂ porous microsheets	1.0 mol∙L−1 KOH + 0.3 mol∙L⁻¹ N₂H₄	−36	42
NiFeP on nickel foam	1.0 mol∙L⁻¹ KOH + 0.1 mol∙L⁻¹ N₂H₄	77	43
Co-doped Ni₂P	1.0 mol∙L⁻¹ KOH + 0.1 mol∙L⁻¹ N₂H₄	10	44
PdCo nanoparticles into carbon nanofibers	3.0 mol∙L⁻¹ KOH + 0.2 mol∙L⁻¹ N₂H₄	25	45
CoP/Co nanoparticles on carbon layers	1.0 mol∙L⁻¹ KOH + 0.5 mol∙L⁻¹ N₂H₄	−69	46
V-doped Ni₃N nanosheet self-supported on Ni foam	1.0 mol∙L⁻¹ KOH + 0.1 mol∙L⁻¹ N₂H₄	2	47
Low-crystalline Rh metallene	1.0 mol∙L⁻¹ KOH + 0.1 mol∙L⁻¹ N₂H₄	−2	48
RhIr mesoporous nanospheres	1.0 mol∙L⁻¹ KOH + 0.5 mol∙L⁻1 N₂H₄	−12 mV	49

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氮掺杂石墨烯气凝胶锚定RuP纳米粒子用于水合肼氧化辅助产氢

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

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