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Palladium Nanoparticles with Surface Enrichment of Palladium Oxide Species Immobilized on the Aniline-Functionalized Graphene As an Advanced Electrocatalyst of Ethanol Oxidation
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2019-07-31 00:00:00 , DOI: 10.1021/acssuschemeng.9b02397 Honglei Yang 1 , Shuwen Li 1 , Fan Feng 1 , Shiyong Ou 1 , Feng Li 1 , Ming Yang 1 , Kailong Qian 1 , Jun Jin 1 , Jiantai Ma 1
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2019-07-31 00:00:00 , DOI: 10.1021/acssuschemeng.9b02397 Honglei Yang 1 , Shuwen Li 1 , Fan Feng 1 , Shiyong Ou 1 , Feng Li 1 , Ming Yang 1 , Kailong Qian 1 , Jun Jin 1 , Jiantai Ma 1
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A new electrocatalyst (denoted as Pd-PdOx/GS-NH2) was fabricated by anchoring Pd nanoparticles with surface enrichment of palladium oxide species (PdOx, including palladium oxides and palladium hydrous oxides) on the aniline-functionalized graphene (GS-NH2) in this work. The GS-NH2 with tunable contents of aniline groups was prepared by a diazo reaction under facile reaction conditions. Then, the surface-clean Pd nanoparticles were decorated on the surface of GS-NH2 by a facile and nonsurfactant approach. Afterward, the palladium oxide species was introduced on the surface of Pd nanoparticles by oxidation treatment in a short period of time. As a catalyst toward the ethanol electrooxidation reaction (EOR), Pd-PdOx/GS-NH2 displays the introduction of appropriate aniline groups and an oxidation treatment with a codependent electrochemical behavior of EOR, mainly owing to the synergy of aniline groups and PdOx. The introduction of aniline groups on the surface of graphene benefits the formation of small size and uniform distribution for nanoparticles and suppresses the dissolution of Pd during electrochemical tests, due to the strong interaction between aniline groups and nanoparticles. However, the excess contents of aniline groups can reduce electrical conductivity of the catalysts, and the optimal mass ratio of 1,4-diaminobenzene to graphene is 1:3. The generated PdOx can strikingly facilitate the removal of COads-like intermediates and elimination of poisoning species during the EOR process, thereby reducing the degradation rate of the catalyst. Therefore, the Pd-PdOx/GS-NH2 possesses superb EOR performance with robust durability and is a kind of great potential anode catalyst for direct ethanol fuel cells. This work also affords a new thought for rationally designing high-performance catalysts.
中文翻译：
表面富集固定在苯胺功能化石墨烯上的氧化钯物种的钯纳米颗粒，作为乙醇氧化的高级电催化剂
一种新的电极催化剂（表示为钯的PdO X / GS-NH 2）通过锚定钯纳米粒子与氧化钯物种的表面富集制造（PDO X GS-，包括钯的氧化物和钯水合氧化物）的苯胺-官能化石墨烯（ NH 2）。具有苯胺基团含量可调的GS-NH 2是通过在容易的反应条件下通过重氮反应制备的。然后，将表面清洁的Pd纳米颗粒装饰在GS-NH 2的表面上通过一种简便而又非表面活性剂的方法。然后，在短时间内通过氧化处理将氧化钯物质引入Pd纳米颗粒的表面。作为乙醇电氧化反应（EOR）的催化剂，Pd-PdO x / GS-NH 2显示出适当的苯胺基团的引入和具有EOR的电化学依赖性的氧化处理，这主要归因于苯胺基团和PdO的协同作用X。由于苯胺基团和纳米颗粒之间的强相互作用，在石墨烯表面引入苯胺基团有利于形成小尺寸和均匀分布的纳米颗粒，并在电化学测试过程中抑制了Pd的溶解。然而，苯胺基团的过量含量会降低催化剂的电导率，并且1,4-二氨基苯与石墨烯的最佳质量比为1：3。所产生的PdO X可明显便于除去CO的广告式的中间体和消除在EOR工艺中毒物质，从而降低了催化剂的降解率的。因此，Pd-PdO x / GS-NH 2具有优异的EOR性能和耐用性，是一种直接乙醇燃料电池的巨大潜在阳极催化剂。这项工作也为合理设计高性能催化剂提供了新思路。
更新日期：2019-07-31
中文翻译：
表面富集固定在苯胺功能化石墨烯上的氧化钯物种的钯纳米颗粒，作为乙醇氧化的高级电催化剂
一种新的电极催化剂（表示为钯的PdO X / GS-NH 2）通过锚定钯纳米粒子与氧化钯物种的表面富集制造（PDO X GS-，包括钯的氧化物和钯水合氧化物）的苯胺-官能化石墨烯（ NH 2）。具有苯胺基团含量可调的GS-NH 2是通过在容易的反应条件下通过重氮反应制备的。然后，将表面清洁的Pd纳米颗粒装饰在GS-NH 2的表面上通过一种简便而又非表面活性剂的方法。然后，在短时间内通过氧化处理将氧化钯物质引入Pd纳米颗粒的表面。作为乙醇电氧化反应（EOR）的催化剂，Pd-PdO x / GS-NH 2显示出适当的苯胺基团的引入和具有EOR的电化学依赖性的氧化处理，这主要归因于苯胺基团和PdO的协同作用X。由于苯胺基团和纳米颗粒之间的强相互作用，在石墨烯表面引入苯胺基团有利于形成小尺寸和均匀分布的纳米颗粒，并在电化学测试过程中抑制了Pd的溶解。然而，苯胺基团的过量含量会降低催化剂的电导率，并且1,4-二氨基苯与石墨烯的最佳质量比为1：3。所产生的PdO X可明显便于除去CO的广告式的中间体和消除在EOR工艺中毒物质，从而降低了催化剂的降解率的。因此，Pd-PdO x / GS-NH 2具有优异的EOR性能和耐用性，是一种直接乙醇燃料电池的巨大潜在阳极催化剂。这项工作也为合理设计高性能催化剂提供了新思路。
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