Bimetallic and postsynthetically alloyed PtCu nanostructures with tunable reactivity for the methanol oxidation reaction.
Bimetallic and postsynthetically alloyed PtCu nanostructures with tunable reactivity for the methanol oxidation reaction.
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双金属和合成后合金化的 PtCu 纳米结构，具有可调的甲醇氧化反应反应性
DOI：
10.1039/d0na00076k
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发表时间：
2020-04-15
影响因子：
4.7
通讯作者：
中科院分区：
文献类型：
--
作者：
通过控制催化剂的形貌和结构来设计有效的催化剂是提高燃料电池能量效率的关键。需要很好地理解特定结构对电催化活性、选择性和稳定性的影响。在这里，我们提出了一个简单的方法来合成PtCu纳米结构与可控的组成，以铜纳米线为模板，抗坏血酸为还原剂。进一步的退火工艺提供了具有可调晶体结构的合金PtCu。PtCu纳米线形式的独特结构与可调组合物的组合为更好地理解催化过程中的反应机理提供了大量信息。HClO 4循环伏安（CV）测试证实，各种相变发生在镁合金和合金样品，影响形态和晶胞结构。在双功能协同效应和第二金属插入的影响下，这两个系列的结构对甲醇的电氧化表现出上级性能。典型地，具有立方结构（a = 3.702 μ m）的后产物合金A-Pt 14 Cu 86具有较好的甲醇氧化反应（莫尔）催化性能。进行密度泛函理论（DFT）计算以使用吉布斯自由能确定最佳途径，并通过过电位变化验证电催化性能对晶格结构的依赖性。双金属PtCu具有高CO耐受性，保持高稳定性。本工作为系统设计新型催化剂和探索燃料电池及其他相关应用的电催化机理提供了一种方法。
Designing effective catalysts by controlling morphology and structure is key to improving the energy efficiency of fuel cells. A good understanding of the effects of specific structures on electrocatalytic activity, selectivity, and stability is needed. Here, we propose a facile method to synthesize PtCu bimetallic nanostructures with controllable compositions by using Cu nanowires as a template and ascorbic acid as a reductant. A further annealing process provided the alloy PtCu with tunable crystal structures. The combination of distinct structures with tunable compositions in the form of PtCu nanowires provides plenty of information for better understanding the reaction mechanism during catalysis. HClO4 cyclic voltammetry (CV) tests confirmed that various phase transformations occurred in bimetallic and alloy samples, affecting morphology and unit cell structures. Under a bifunctional synergistic effect and the influence of the insertion of a second metal, the two series of structures show superior performance toward methanol electrooxidation. Typically, the post-product alloy A-Pt14Cu86 with a cubic structure (a = 3.702 Å) has better methanol oxidation reaction (MOR) catalysis performance. Density functional theory (DFT) calculations were performed to determine an optimal pathway using the Gibbs free energy and to verify the dependence of the electrocatalytic performance on the lattice structure via overpotential changes. Bimetallic PtCu has high CO tolerance, maintaining high stability. This work provides an approach for the systematic design of novel catalysts and the exploration of electrocatalytic mechanisms for fuel cells and other related applications.
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