Defective Ru-doped & alpha;-MnO2 nanorods enabling efficient hydrazine oxidation for energy-saving hydrogen production via proton exchange membranes at near-neutral pH | |
Yu, Zhipeng1,2; Si, Chaowei3,4; Sabate, Ferran5; LaGrow, Alec P.6; Tai, Zhixin2; Diaconescu, Vlad Martin7; Simonelli, Laura7; Meng, Lijian8; Sabater, Maria J.5; Li, Bo9; Liu, Lifeng1,2 | |
通讯作者 | Sabater, Maria J.(mjsabate@itq.upv.es) ; Li, Bo(boli@imr.ac.cn) ; Liu, Lifeng(liu.lifeng@sslab.org.cn) |
2023-08-15 | |
发表期刊 | CHEMICAL ENGINEERING JOURNAL
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ISSN | 1385-8947 |
卷号 | 470页码:10 |
摘要 | Proton exchange membrane water electrolysis (PEMWE) showes substantial advantages over the conventional alkaline water electrolysis (AWE) for power-to-hydrogen (PtH) conversion, given the faster response and wider dynamic current range of the PEMWE technology. However, PEMWE is currently still expensive due partly to the high voltage needed to operate at high current densities and inevitable usage of precious iridium/rutheniumbased catalysts to expedite the slow kinetics of the oxygen evolution reaction (OER) and to ensure sufficient durability under strongly acidic conditions. Herein, we report that ruthenium doped & alpha;-manganese oxide (Ru/ & alpha;-MnO2) nanorods show outstanding electrocatalytic performance toward the hydrazine (N2H4) oxidation reaction (HzOR) in near-neutral media (weak alkaline and weak acid), which can be used to replace the energydemanding OER for PEMWE. The as-prepared Ru/& alpha;-MnO2 is found to comprise abundant defects. When used to catalyze HzOR in the acid-hydrazine electrolyte (0.05 M H2SO4 + 0.5 M N2H4), it can deliver an anodic current density of 10 mA cm-2 at a potential as low as 0.166 V vs. reversible hydrogen electrode (RHE). Moreover, Ru/ & alpha;-MnO2 exhibits remarkable corrosion/oxidation resistance and remains electrochemically stable during HzOR for at least 1000 h. Theoretical calculations and experimental studies prove that Ru doping elongates the Mn-O bond and produces abundant cationic defects, which induces charge delocalization and significantly lowers material's electrical resistance and overpotential, resulting in excellent HzOR catalytic activity and stability. The introduction of N2H4 significantly reduces the energy demand for hydrogen production, so that PEMWE can be accomplished under remarkably low voltages of 0.254 V at 10 mA cm-2 and 0.935 V at 100 mA cm-2 for a long term without notable degradation. This work opens a new avenue toward energy-saving PEMWE with earthabundant OER catalysts. |
关键词 | Cationic defect Ru doping PEM water electrolysis Hydrazine oxidation reaction Electrocatalysis |
资助者 | Songshan Lake Mate- rials Laboratory ; Ministry of Science amp; Technology of China ; Natural Science Foundation of Liao Ning Province ; ShenYang Normal University ; China Scholarship Council ; National Innovation Agency of Portugal |
DOI | 10.1016/j.cej.2023.144050 |
收录类别 | SCI |
语种 | 英语 |
资助项目 | Songshan Lake Mate- rials Laboratory[Y2D1051Z311] ; Ministry of Science amp; Technology of China[22J4021Z311] ; Natural Science Foundation of Liao Ning Province[2021 -MS -004] ; ShenYang Normal University[BS202208] ; China Scholarship Council[201806150015] ; National Innovation Agency of Portugal[POCI-01- 0247-FEDER-046109] |
WOS研究方向 | Engineering |
WOS类目 | Engineering, Environmental ; Engineering, Chemical |
WOS记录号 | WOS:001023134200001 |
出版者 | ELSEVIER SCIENCE SA |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.imr.ac.cn/handle/321006/178478 |
专题 | 中国科学院金属研究所 |
通讯作者 | Sabater, Maria J.; Li, Bo; Liu, Lifeng |
作者单位 | 1.Songshan Lake Mat Lab, Dongguan 523808, Peoples R China 2.Int Iberian Nanotechnol Lab INL, Clean Energy Cluster, Ave Mestre Jose Veiga, P-4715330 Braga, Portugal 3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 4.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China 5.Univ Politecn Valencia, Inst Tecnol Quim, Consejo Super Invest Cient, Ave Naranjos S-N, Valencia 46022, Spain 6.Okinawa Inst Sci & Technol Grad Univ, Sci Imaging Sect, Okinawa, Japan 7.ALBA Synchrotron, Carrer Llum 2-26, Cerdanyola Del Valles 08290, Barcelona, Spain 8.Inst Politecn Porto, Inst Super Engn Porto, Ctr Innovat Engn & Ind Technol, P-4249015 Porto, Portugal 9.ShenYang Normal Univ, Coll Chem & Chem Engn, Shenyang 110034, Peoples R China |
推荐引用方式 GB/T 7714 | Yu, Zhipeng,Si, Chaowei,Sabate, Ferran,et al. Defective Ru-doped & alpha;-MnO2 nanorods enabling efficient hydrazine oxidation for energy-saving hydrogen production via proton exchange membranes at near-neutral pH[J]. CHEMICAL ENGINEERING JOURNAL,2023,470:10. |
APA | Yu, Zhipeng.,Si, Chaowei.,Sabate, Ferran.,LaGrow, Alec P..,Tai, Zhixin.,...&Liu, Lifeng.(2023).Defective Ru-doped & alpha;-MnO2 nanorods enabling efficient hydrazine oxidation for energy-saving hydrogen production via proton exchange membranes at near-neutral pH.CHEMICAL ENGINEERING JOURNAL,470,10. |
MLA | Yu, Zhipeng,et al."Defective Ru-doped & alpha;-MnO2 nanorods enabling efficient hydrazine oxidation for energy-saving hydrogen production via proton exchange membranes at near-neutral pH".CHEMICAL ENGINEERING JOURNAL 470(2023):10. |
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