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A general polymer-assisted strategy enables unexpected efficient metal-free oxygen-evolution catalysis on pure carbon nanotubes
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2017-08-22 00:00:00 , DOI: 10.1039/c7ee01702b
You Zhang 1, 2, 3, 4, 5 , Xuliang Fan 1, 2, 3, 4, 5 , Junhua Jian 1, 2, 3, 4, 5 , Dingshan Yu 1, 2, 3, 4, 5 , Zishou Zhang 1, 2, 3, 4, 5 , Liming Dai 6, 7, 8, 9
Affiliation  

A conceptually new and general strategy was, for the first time, proposed to significantly boost the electrocatalytic activity of metal-free pure carbon nanotubes (CNTs) towards the oxygen evolution reaction (OER) by simple polymer wrapping without introducing any heteroatom dopants, functional groups, or edge defects into the graphitic structure. Our strategy is straightforward, efficient, green, and easy to be scaled up. After wrapping pure CNTs with a certain class of electrochemically inert polymers (i.e. poly(ethylene-alt-maleic acid), poly(vinyl alcohol), poly(vinyl acetate), poly(ethylene glycol)) with polar oxygen-containing groups (i.e. –COOH, –OH, –COOCH3, –O–) through noncovalent interactions, a series of advanced metal-free composite membrane catalysts were easily achieved, which yielded unexpected, surprisingly high OER activity – on par with the commercial noble RuO2 catalyst, though pure CNTs have rather poor OER activity. Combined experimental and computational studies revealed that the observed superb OER activity could be attributed to a synergistic effect of intrinsic topological defects in the CNTs as active centers and the coated polymer layer as a co-catalyst to optimize the adsorption energies of intermediates for improving the OER energetics.

中文翻译:

通用的聚合物辅助策略可在纯碳纳米管上实现出乎意料的高效无金属析氧催化

首次提出了一种概念上新颖的通用策略,该策略通过简单的聚合物包裹而不引入任何杂原子掺杂剂,官能团来显着提高无金属的纯碳纳米管(CNT)对氧释放反应(OER)的电催化活性。或边缘缺陷进入石墨结构。我们的策略简单,高效,绿色且易于扩展。包裹纯碳纳米管与某一类电化学惰性聚合物(以后聚(乙烯- ALT -马来酸),聚(乙烯醇),聚(乙酸乙烯酯),聚(乙二醇)),与极性含氧基团(–COOH,–OH,–COOCH 3,–O–)通过非共价相互作用很容易实现了一系列先进的无金属复合膜催化剂,尽管与纯净的CNT相比,其具有较差的OER活性,但其与普通的贵金属RuO 2催化剂相比却具有出乎意料的惊人的高OER活性。 。联合的实验和计算研究表明,观察到的极好的OER活性可归因于CNTs内在的拓扑缺陷(作为活性中心)和包覆的聚合物层作为助催化剂的协同效应,从而优化了中间体的吸附能,从而改善了OER。能量学。
更新日期:2017-11-08
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