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Covalently functionalized layered MoS2 supported Pd nanoparticles as highly active oxygen reduction electrocatalysts.
Nanoscale ( IF 5.8 ) Pub Date : 2020-08-06 , DOI: 10.1039/d0nr04446f
Dimitrios K Perivoliotis 1 , Yuta Sato 2 , Kazu Suenaga 2 , Nikos Tagmatarchis 1
Affiliation  

Molybdenum disulfide nanosheets covalently modified with a 1,2-dithiolane derivative were used as a novel substrate for the immobilization of Pd nanoparticles (PdNPs) towards the development of a highly efficient hybrid electrocatalyst, namely PdNPs/f-MoS2, for the oxygen reduction in an alkaline medium. The newly prepared hybrid material was thoroughly characterized through complementary techniques such as Raman and IR spectroscopy, TGA, HRTEM, STEM/EELS, and EDS. The PdNPs/f-MoS2 nanohybrid exhibited excellent performance towards oxygen electroreduction with a positive onset potential of +0.066 V and a half-wave potential of −0.116 V vs. Hg/HgO, along with a high current response, which are superior to those of its graphene counterpart and comparable to those of the benchmark Pd/C product. Moreover, PdNPs/f-MoS2 was proved to be remarkably stable as chronoamperometric assays showed minimum activity loss among the tested materials, clearly outperforming the commercial catalyst. The excellent performance of PdNPs/f-MoS2 is attributable to (i) the high affinity of the catalytic PdNPs with the f-MoS2 substrate, (ii) the absence of any capping agent for the stabilization of PdNPs onto f-MoS2, and more importantly (iii) the preservation of the integrity of the MoS2 basal plane during the functionalization process. Lastly, the oxygen reduction on PdNPs/f-MoS2 proceeded through the energy efficient four-electron pathway, showing great potential for the use of layered transition metal dichalcogenides in energy conversion applications, comprising fuel cells.

中文翻译:

共价官能化的层状MoS2负载的Pd纳米颗粒作为高活性氧还原电催化剂。

用1,2-二硫杂环戊烷衍生物共价修饰的二硫化钼纳米片用作固定Pd纳米粒子(Pd NPs)的新型底物,以开发高效的杂化电催化剂,即Pd NPs / f-MoS 2。在碱性介质中减少氧气。通过互补技术(例如拉曼光谱和红外光谱,TGA,HRTEM,STEM / EELS和EDS)对新制备的杂化材料进行了全面表征。Pd NPs / f-MoS 2纳米杂化物表现出优异的抗氧电还原性能,正起始电位为+0.066 V,半波电位为-0.116 V vs。Hg / HgO以及高电流响应,不仅优于其石墨烯,而且可与基准Pd / C产品相媲美。此外,Pd NPs / f-MoS 2被证明是非常稳定的,因为计时电流分析法显示了被测材料中的最小活性损失,明显优于市售催化剂。Pd NPs / f-MoS 2的优异性能归因于(i)催化性Pd NP与f-MoS 2底物的高亲和力,(ii)不存在任何用于将Pd NP稳定在f -MoS 2,更重要的是(iii)保持MoS完整性功能化过程中的2个基面。最后,Pd NPs / f-MoS 2上的氧还原通过高效的四电子途径进行,显示了在包括燃料电池在内的能量转换应用中使用层状过渡金属二卤化碳的巨大潜力。
更新日期:2020-09-18
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