4.8 Article

Highly efficient H2 production from H2S via a robust graphene-encapsulated metal catalyst

期刊

ENERGY & ENVIRONMENTAL SCIENCE
卷 13, 期 1, 页码 119-126

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/c9ee03231b

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资金

  1. Ministry of Science and Technology of China [2016YFA0204100, 2016YFA0200200]
  2. National Natural Science Foundation of China [21890753, 21573220, 21988101]
  3. Key Research Program of Frontier Sciences of the Chinese Academy of Sciences [QYZDB-SSW-JSC020]
  4. DNL Cooperation Fund, CAS [DNL180201]

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The electrocatalytic decomposition of the abundant and toxic H2S from industrial by-products is a promising energy conversion technology for H-2 production and simultaneously removing this environmental pollutant. However, the development of such a technology has been hindered by the lack of low-cost, efficient and robust electrocatalysts. Herein, we reported a remarkable graphene-encapsulated metal catalyst, i.e., nitrogen-doped graphene encapsulating a non-precious CoNi nanoalloy as the anode for highly efficient electrocatalytic H-2 production from H2S. This optimized catalyst could drive the anode reaction at an onset potential of 0.25 V, which was 1.24 V lower than that required for the water oxidation reaction, and delivered almost twice current density than that of Pt/C. Meanwhile, it exhibited approximately 98% H-2 faradaic efficiency and maintained long-term durability for more than 500 h without any decay. The density functional theory calculations revealed that the CoNi and nitrogen dopants synergistically facilitated the formation of polysulfides on graphene's surfaces. Furthermore, a demo showed 1200 h stability for removing H2S impurities from industrial syngas to produce hydrogen by this graphene-encapsulated metal catalyst, demonstrating its great potential for hydrogen production toward sustainable energy applications.

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