An effective and durable interface structure design for oxygen reduction and methanol oxidation electrocatalyst

An effective and durable interface structure design for oxygen reduction and methanol oxidation electrocatalyst
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一种有效且耐用的氧还原和甲醇氧化电催化剂界面结构设计

DOI:
10.1016/j.apsusc.2019.04.237
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发表时间:
2019-09
影响因子:
6.7
通讯作者:
Xindong Wang
Xindong Wang
中科院分区:
材料科学1区
文献类型:
--
作者:
Zhaoyi Yang;Ming Chen;Min Xia;Meng Wang;Xindong Wang

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为了抑制传统Pt/XC-72催化剂中碳载体的腐蚀和Pt纳米颗粒的团聚,在催化剂/载体界面上原位沉积非晶碳化钨(WC)对传统Pt/C催化剂进行改性。结果表明,适量的WC可以提高催化剂的性能和耐久性,过量的W元素加入会与氧联合收割机结合,转化为WO 3,从而包覆Pt纳米颗粒,降低催化剂的活性位。当W含量控制在20wt%时,Pt-WC(20wt%W,PWC 20)催化剂的氧还原反应(ORR)极化曲线的半波电位(E1/2)较常规Pt/XC-72催化剂正移了31 mV,在0.85V时催化剂的质量活性和比活性提高了约2.0倍。经10,000次加速耐久性试验(ADT)后,PWC 20催化剂的电化学活性面积(ECSA)下降了21.7%,E1/2负移了22 mV,而传统Pt/XC-72催化剂的ECSA下降了49.49%,E1/2负移了42 mV。甲醇氧化反应(莫尔)的峰值电流密度是传统Pt/XC-72的1.41倍,甲醇氧化的正向扫描电位负移36 mV。在1000次ADT循环后,正向峰值电流密度下降了15.23%,而常规Pt/XC-72下降了26.62%。CO溶出伏安法和X射线光电子能谱(XPS)分析结果表明,WC对催化剂/载体界面的改性显著提高了常规Pt/C的抗CO毒性能力。WC和Pt之间的协同效应增强了金属-载体相互作用。通过对催化剂/载体界面的改性,提高了催化剂对ORR和莫尔的耐久性,同时也提高了质子交换膜燃料电池(PEMFC)阴极催化层的性能和耐久性。
In order to inhibit the corrosion of carbon support and agglomeration of Pt nanoparticles in conventional Pt/XC-72 catalyst, the conventional Pt/C catalyst was modified by in-situ deposition of amorphous tungsten carbide (WC) at the catalyst/support interface. The results show that proper amount of WC can improve the performance and durability of catalyst, and excessive addition of W element will combine with oxygen and transform into WO3, thus covering Pt nanoparticles and reducing the active site of catalyst. When W content is controlled at 20 wt%, the half-wave potential (E1/2) of oxygen reduction reaction (ORR) polarization curve of Pt-WC (20 wt% W, PWC20) catalyst is positively shifted by 31 mV compared with that of conventional Pt/XC-72 catalyst, and the mass activity and specific activity of catalyst are increased by about 2.0 times at 0.85 V. After 10,000 cycles of accelerated durability test (ADT), the electrochemical active area (ECSA) of PWC20 catalyst decreased by 21.7% and the E1/2was negatively shifted by 22 mV, while the ECSA of conventional Pt/XC-72 catalyst decreased by 49.49% and E1/2shifted by 42 mV negatively. The peak current density of methanol oxidation reaction (MOR) is 1.41 times higher than that of conventional Pt/XC-72, and the forward scanning potential of methanol oxidation shifts 36 mV negatively. After 1000 cycles of ADT, the forward peak current density decreased by 15.23%, while the conventional Pt/XC-72 decreased by 26.62%. The results of CO stripping voltammetry and X-ray photoelectron spectroscopy (XPS) analysis show that the modification of catalyst/support interface by WC significantly improves the anti-CO toxicity ability of conventional Pt/C. The synergistic effect between WC and Pt enhances the metal-support interaction. The durability of catalyst toward ORR and MOR was improved by the modification of catalyst/support interface, and the performance and durability of proton exchange membrane fuel cell (PEMFC) cathode catalyst layer were also improved.
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