Spontaneous redox synthesis of Prussian blue/graphene nanocomposite as a non-precious metal catalyst for efficient four-electron oxygen reduction in acidic medium
Spontaneous redox synthesis of Prussian blue/graphene nanocomposite as a non-precious metal catalyst for efficient four-electron oxygen reduction in acidic medium
复制标题
DOI：
10.1016/j.jpowsour.2013.03.156
复制
发表时间：
2013-10
影响因子：
9.2
通讯作者：
Lei Xu;Guoquan Zhang;Jie Chen;Yufei Zhou;Guang'en Yuan;Fenglin Yang
中科院分区：
文献类型：
--
作者：
Lei Xu;Guoquan Zhang;Jie Chen;Yufei Zhou;Guang'en Yuan;Fenglin Yang
以Fe粉、K3[Fe（CN）6]和氧化石墨烯为前驱体，在酸性溶液中通过自发氧化还原反应合成了普鲁士蓝/石墨烯（PB/GE）纳米复合材料。通过扫描电子显微镜、透射电子显微镜、拉曼光谱和X射线光电子能谱对所得PB/GE纳米复合材料进行了表征。PB/GE纳米复合物修饰玻碳电极（PB/GE-GCE）对氧还原反应（ORR）具有良好的电催化活性和长期稳定性。PB的还原态为普鲁士白色，在酸性溶液中对O2和H2 O2的还原具有良好的电催化活性。旋转环-盘伏安法测量清楚地表明，在PB-GCE上ORR的主要产物是在所有电位下由O2的4 e −还原产生的水。PB/GE-GCE的ORR主要发生在PB晶格内部，在E> −0.5 V时通过4 e −还原途径进行，在GE纳米片上，在E < −0.5 V时通过“2 + 2”机制进行，其中H2 O2作为中间产物。PB/GE纳米复合材料是一种潜在的高效和低成本的燃料电池催化剂。
A Prussian blue/graphene (PB/GE) nanocomposite is synthesized as a non-precious metal catalyst by a spontaneous redox reaction in acidic solution with Fe powder, K3[Fe(CN)6], and graphene oxide as precursors. The resulting PB/GE nanocomposite is characterized by scanning electron microscopy, transmission electron microscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy. The PB/GE nanocomposite-modified glassy carbon electrode (PB/GE–GCE) exhibits good electrocatalytic activity and long-term stability toward the oxygen reduction reaction (ORR). The reduced form of PB, Prussian white, has favorable electrocatalytic activity for the reduction of O2and H2O2in acidic solutions. Rotating ring-disk voltammetric measurements clearly show that the dominant product of ORR at the PB–GCE is water produced by the 4e−reduction of O2at all potentials. ORR at the PB/GE–GCE occurs mainly inside the PB lattice through the 4e−reduction pathway atE> −0.5 V and on GE nanosheets through the “2 + 2” mechanism involving H2O2as the intermediate product atE< −0.5 V. The PB/GE nanocomposite is a potentially efficient and cost-effective catalyst for fuel cells.