期刊
SMALL METHODS
卷 4, 期 9, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smtd.202000208
关键词
bifunctional electrocatalysts; energy-efficient hydrogen evolution; hydrogen production; overall hydrazine splitting; pH-universal environments
资金
- National Key RAMP
- D Program of China [2017YFA0700104]
- National Natural Science Foundation of China [21601136, 51971157, 21677171, 51761165012]
- Tianjin Science Fund for Distinguished Young Scholars [19JCJQJC61800]
Using hydrazine oxidation reaction (HzOR) to replace the oxygen evolution reaction is an effective way to decrease the overpotential of the anodic reaction in overall water splitting (OWS), facilitating cost-effective and safe hydrogen production. Herein, Rh2S3/N-doped carbon hybrids (Rh2S3/NC) are first reported as novel and efficient bifunctional electrocatalysts for hydrazine-assisted hydrogen generation over a wide pH range. Specifically, Rh2S3/NC exhibits low overpotentials for the hydrogen evolution reaction (HER) in alkaline (38 mV), neutral (46 mV), and acidic (21 mV) electrolytes, to reach the current density of 10 mA cm(-2), and maintains the activities over 70 h. Meanwhile, Rh2S3/NC also displays competitive HzOR performance at all-pH electrolytes. Thus, serving as a bifunctional electrocatalyst for both HER and HzOR, Rh2S3/NC shows overwhelming-Pt/C performance in three electrolytes, and can save over 93.3%, 85.2%, and 78.3% energy consumption compared to the corresponding OWS system. Moreover, theoretical calculations confirm that Rh2S3/NC owns low free-energy changes of the H adsorption and the dehydrogenation of adsorbed NHNH both of which are beneficial to enhance catalytic activity. This work develops a novel bifunctional electrocatalyst with free pH-dependent condition for the hydrazine-assisted electrolysis system to furtherly reduce the cost of massive industrial H-2 production.
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