Nitrogen, Phosphorus, and Fluorine Tri-doped Graphene as a Multifunctional Catalyst for Self-Powered Electrochemical Water Splitting.
Nitrogen, Phosphorus, and Fluorine Tri-doped Graphene as a Multifunctional Catalyst for Self-Powered Electrochemical Water Splitting.
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DOI：
10.1002/anie.201607405
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发表时间：
2016-10
影响因子：
--
通讯作者：
Jintao Zhang;L. Dai
中科院分区：
文献类型：
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作者：
Jintao Zhang;L. Dai
清洁能源技术（例如水分解和金属-空气电池）需要电催化剂。报道了一种由氮、磷、氟三掺杂石墨烯组成的多功能电催化剂的开发，该催化剂是由聚苯胺包覆的氧化石墨烯和六氟磷酸铵（AHF）的混合物热活化得到的。研究发现，AHF的热分解为N、P、F的三掺杂提供了氮、磷、氟的来源，同时由于热气体的演化，促进了无模板多孔结构的形成。得到的N、P和F三掺杂石墨烯在氧还原反应（ORR）、析氧反应（OER）和析氢反应（HER）中表现出优异的电催化活性。该三功能无金属催化剂被进一步用作OER-HER双功能催化剂，用于电化学水分解装置中产生氧气和氢气，该装置由基于相同电催化剂制成的空气电极的集成锌空气电池供电。该集成装置由新开发的N、P、F三掺杂石墨烯多功能无金属催化剂制成，可在环境空气中工作，氢气和氧气的产气率分别为0.496和0.254 μL s-1，具有很大的实际应用潜力。
Electrocatalysts are required for clean energy technologies (for example, water-splitting and metal-air batteries). The development of a multifunctional electrocatalyst composed of nitrogen, phosphorus, and fluorine tri-doped graphene is reported, which was obtained by thermal activation of a mixture of polyaniline-coated graphene oxide and ammonium hexafluorophosphate (AHF). It was found that thermal decomposition of AHF provides nitrogen, phosphorus, and fluorine sources for tri-doping with N, P, and F, and simultaneously facilitates template-free formation of porous structures as a result of thermal gas evolution. The resultant N, P, and F tri-doped graphene exhibited excellent electrocatalytic activities for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). The trifunctional metal-free catalyst was further used as an OER-HER bifunctional catalyst for oxygen and hydrogen gas production in an electrochemical water-splitting unit, which was powered by an integrated Zn-air battery based on an air electrode made from the same electrocatalyst for ORR. The integrated unit, fabricated from the newly developed N, P, and F tri-doped graphene multifunctional metal-free catalyst, can operate in ambient air with a high gas production rate of 0.496 and 0.254 μL s-1 for hydrogen and oxygen gas, respectively, showing great potential for practical applications.