Investigation of Activity of Sputtered Transition-Metal (TM)–C–N (TM = V, Cr, Mn, Co, Ni) Catalysts for Oxygen Reduction Reaction
Investigation of Activity of Sputtered Transition-Metal (TM)–C–N (TM = V, Cr, Mn, Co, Ni) Catalysts for Oxygen Reduction Reaction
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DOI：
10.1149/1.2803519
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发表时间：
2008
影响因子：
3.9
通讯作者：
Ruizhi Yang;K. Stevens;J. Dahn
中科院分区：
文献类型：
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作者：
Ruizhi Yang;K. Stevens;J. Dahn
研究了溅射过渡金属（TM）-C-N（TM = V、Cr、Mn、Co和Ni）薄膜在酸性和碱性电解液中的结构和对氧还原反应（ORR）的电催化活性随热处理温度的变化。所制备的膜最初都是无定形的。在一个临界热处理温度（Tc，不同的每种组合物）大量的氮释放发生和薄膜转化为一个异质的含氮的碳结构与铬3 C 2，钴，镍，V 8 C 7，或Mn 7 C 3，这取决于TM使用。在酸性电解液中，热处理后的CrxC 1-x-yNy、CoxC 1-x-yNy和NixC 1-x-yNy薄膜在Tc处开始显示氧还原活性，而VxC 1-x-yNy和MnxC 1-x-yNy薄膜在酸性电解液中几乎没有或没有氧还原活性。然而，所有热处理的TM x C1-x-y Ny（TM = V，Cr，Mn，Co和Ni）薄膜显示在碱性电解液中的氧还原活性，即使当加热到温度低于Tc。由于所有的TM xC 1-x-yNy薄膜都含有含氮的碳，因此研究了热处理溅射的C1-xNx和C薄膜以及石墨粉末的活性以进行比较。它们在酸性电解液中的活性远低于相同温度下热处理的CrxC 1-x-yNy、COxC 1-x-yNy和NixC 1-x-yNy薄膜。C1-xNx膜、C膜和石墨粉在碱性电解液中均表现出活性，但活性低于某些加热的CoxC 1-x-yNy和NixC 1-x-yNy膜。TM和热处理温度的选择起着重要的作用，在确定的活性溅射TM x C 1-x-y N y膜的ORR在酸性和碱性电解质。研究了热处理后TMxC 1-x-yNy库的耐腐蚀性能。经热处理的Cr x C 1-x-y N y库显示出良好的抗腐蚀钝化。
Variations with heat-treatment temperature of the structure and the electrocatalytic activity of sputtered transition-metal (TM)-C-N (TM = V, Cr, Mn, Co, and Ni) films for the oxygen reduction reaction (ORR) in acid and alkaline electrolytes were studied. The films prepared were all originally amorphous. At a critical heat-treatment temperature (T c , different for each composition) substantial nitrogen release occurred and the films transformed to a heterogeneous N-containing carbon structure with either Cr 3 C 2 , Co, Ni, V 8 C 7 , or Mn 7 C 3 , depending on the TM used. In acid electrolyte, heat-treated Cr x C 1-x-y N y , Co x C 1-x-y N y , and Ni x C 1-x-y N y films began to show oxygen reduction activity at T c , while V x C 1-x-y N y and Mn x C 1-x-y N y films showed little or no activity for ORR in acid electrolyte for all temperatures studied. However, all of the heat-treated TM x C 1-x-y N y (TM = V, Cr, Mn, Co, and Ni) films showed oxygen reduction activity in alkaline electrolyte even when heated to temperatures below T c . Because all the TM x C 1-x-y N y films heated above T c contained N-containing carbon, the activity of heat-treated sputtered C 1-x N x and C films, as well as graphite powder, were studied for comparison. Their activities were much lower in acid electrolyte than those of the Cr x C 1-x-y N y , CO x C 1-x-y N y , and Ni x C 1-x-y N y films heat-treated at the same temperatures. C 1-x N x films, C films, and graphite powder all showed activity in alkaline electrolyte but were less active than some heated Co x C 1-x-y N y and Ni x C 1-x-y N y films. The choice of TM and the heat-treatment temperature played important roles in determining the activity of the sputtered TM x C 1-x-y N y films for ORR in acid and alkaline electrolytes. The corrosion stability of the heat-treated TM x C 1-x-y N y libraries was studied as well. Heat-treated Cr x C 1-x-y N y libraries showed good passivation against corrosion.