Highly efficient H2 production from H2S via a robust graphene-encapsulated metal catalyst,Energy & Environmental Science

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Highly efficient H2 production from H2S via a robust graphene-encapsulated metal catalyst
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2019-11-23 , DOI: 10.1039/c9ee03231b
Mo Zhang _{1,

2,

3,

4,

5} , Jing Guan _{6,

7,

8,

9} , Yunchuan Tu _{1,

2,

3,

4,

5} , Shiming Chen _{10,

11,

12,

13,

14} , Yong Wang _{1,

2,

3,

4,

5} , Suheng Wang _{1,

2,

3,

4,

5} , Liang Yu _{10,

11,

12,

13,

14} , Chao Ma _{9,

15,

16,

17,

18} , Dehui Deng _{1,

2,

3,

4,

5} , Xinhe Bao _{10,

11,

12,

13,

14}

Affiliation

State Key Laboratory of Physical Chemistry of Solid Surfaces
Collaborative Innovation Center of Chemistry for Energy Materials (iChEM)
College of Chemistry and Chemical Engineering
Xiamen University
Xiamen 361005
School of Environmental & Municipal Engineering
Qingdao University of Technology
Qingdao 266033
China
State Key Laboratory of Catalysis
iChEM
Dalian Institute of Chemical Physics
Chinese Academy of Science
Dalian 116023
Center for High Resolution Electron Microscopy
College of Materials Science and Engineering
Hunan University
Changsha 410082

The electrocatalytic decomposition of the abundant and toxic H₂S from industrial by-products is a promising energy conversion technology for H₂ 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 H₂ 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% H₂ 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.

中文翻译：

通过坚固的石墨烯包封的金属催化剂从H2S高效生产H2

工业副产物中丰富而有毒的H ₂ S的电催化分解是一种有前途的能源转化技术，可用于生产H ₂并同时去除这种环境污染物。然而，由于缺乏低成本，有效和坚固的电催化剂，阻碍了这种技术的发展。在本文中，我们报道了显着石墨烯-包封的金属催化剂，即，氮掺杂的石墨烯包封非贵重的CoNi纳米合金作为阳极用于高效电ħ ₂选自H生产₂S.这种优化的催化剂可以以0.25 V的起始电势驱动阳极反应，该起始电势比水氧化反应所需的起始电势低1.24 V，并且输送的电流密度几乎是Pt / C的两倍。同时，它表现出约98％的H ₂法拉第效率，并保持了500小时以上的长期耐久性，而没有任何衰减。密度泛函理论计算表明，CoNi和氮掺杂剂协同促进了石墨烯表面上多硫化物的形成。此外，该演示还显示了1200 h去除H _2的稳定性来自工业合成气的S杂质通过这种石墨烯包裹的金属催化剂产生氢，证明了其在可持续能源应用中产生氢的巨大潜力。

更新日期：2019-11-23

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