A nanoporous PtCuTi alloy with a low Pt content and greatly enhanced electrocatalytic performance towards methanol oxidation and oxygen reduction
A nanoporous PtCuTi alloy with a low Pt content and greatly enhanced electrocatalytic performance towards methanol oxidation and oxygen reduction
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一种低Pt含量的纳米多孔PtCuTi合金，大大增强了甲醇氧化和氧还原的电催化性能
DOI：
10.1039/c6ta05570b
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发表时间：
2016-09
影响因子：
11.9
通讯作者：
Zhang Zhonghua
中科院分区：
文献类型：
--
作者：
Wang Ying;Yin Kuibo;Zhang Jie;Si Conghui;Chen Xiaoting;Lv Lanfen;Ma Wensheng;Gao Hui;Zhang Zhonghua
铂基电催化剂在直接甲醇燃料电池（DMFC）的阳极和阴极反应中都起着至关重要的作用，但其活性/耐久性和成本仍然是需要解决的主要问题。通过机械合金化与去合金化相结合的方法，我们以Cu基前驱体为原料，制备了一种低Pt含量的纳米多孔PtCuTi（np-PtCuTi）合金。np-PtCuTi合金呈现三维双连续互穿韧带/通道结构，韧带尺寸为3.1 ± 0.6nm。电化学测试结果表明，与商用PtC催化剂相比，np-PtCuTi合金对甲醇阳极氧化具有上级电催化活性（CO耐受性、比活性和质量活性）.此外，与PtC相比，np-PtCuTi催化剂显示出对阴极处的氧还原反应（ORR）的质量和比活性分别提高了1.9倍和4.2倍。更重要的是，np-PtCuTi催化剂显示出优异的ORR催化耐久性，并且在20 000次循环后质量活性保持初始值的91.8%。 此外，通过实验和密度泛函理论计算，从结构效应、合金化效应和电子效应三个方面对np-PtCuTi催化剂的活性增强机理进行了合理化解释。
Pt-based electrocatalysts play a crucial role in both the anode and cathode reactions of direct methanol fuel cells (DMFCs), but their activity/durability and cost are still the main issues to be addressed. Through the combination of mechanical alloying with dealloying, here we have fabricated a nanoporous PtCuTi (np-PtCuTi) alloy with a low Pt content from a Cu-based precursor. The np-PtCuTi alloy exhibits a three-dimensional bi-continuous interpenetrating ligament/channel structure with a ligament size of 3.1 ± 0.6 nm. Electrochemical measurements show that the np-PtCuTi alloy exhibits superior electrocatalytic activities (CO tolerance, specific and mass activity) towards methanol oxidation at the anode, compared to commercial PtC catalysts. Moreover, the np-PtCuTi catalyst shows an enhancement of 1.9 and 4.2 times in the mass and specific activity towards the oxygen reduction reaction (ORR) at the cathode compared to PtC, respectively. More importantly, the np-PtCuTi catalyst shows excellent catalytic durability for the ORR, and the mass activity retains 91.8% of the initial value after 20 000 cycles. In addition, the mechanisms for the activity enhancement of np-PtCuTi have been rationalized on the basis of the structural effect, alloying effect and electronic effect through experiments and density functional theory calculations.
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影响因子：
3.6
作者：
Shao-Horn, Y.;Sheng, W. C.;Morgan, D.
通讯作者：
Morgan, D.
影响因子：
5.7
作者：
Oezaslan, Mehtap;Hasche, Frederic;Strasser, Peter
通讯作者：
Strasser, Peter
影响因子：
10.8
作者：
Liu, Lifeng;Pippel, Eckhard;Goesele, Ulrich
通讯作者：
Goesele, Ulrich
影响因子：
8.6
作者：
Ruizhi Yang;J. Leisch;P. Strasser;M. Toney
通讯作者：
Ruizhi Yang;J. Leisch;P. Strasser;M. Toney
影响因子：
2.8
作者：
A. Sarkar;A. Murugan;A. Manthiram
通讯作者：
A. Sarkar;A. Murugan;A. Manthiram