A general polymer-assisted strategy enables unexpected efficient metal-free oxygen-evolution catalysis on pure carbon nanotubes
A general polymer-assisted strategy enables unexpected efficient metal-free oxygen-evolution catalysis on pure carbon nanotubes
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DOI：
10.1039/c7ee01702b
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发表时间：
2017-11
影响因子：
32.5
通讯作者：
You Zhang;Xuliang Fan;Junhua Jian;Dingshan Yu;Zishou Zhang;L. Dai
中科院分区：
文献类型：
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作者：
You Zhang;Xuliang Fan;Junhua Jian;Dingshan Yu;Zishou Zhang;L. Dai
首次提出了一种概念新颖的通用策略，即通过简单的聚合物包裹而不引入任何杂原子掺杂剂、官能团或边缘缺陷到石墨结构中，来显著提高无金属纯碳纳米管（CNT）对析氧反应（OER）的电催化活性。我们的策略是简单、高效、绿色、易于推广。在用某种电化学惰性聚合物包裹纯碳纳米管后，（即聚（乙烯-alt-马来酸）、聚聚乙烯醇聚醋酸乙烯酯（乙二醇））与极性含氧基团（即-COOH、-OH、-COOCH 3、-O-）通过非共价相互作用，容易地获得了一系列先进的无金属复合膜催化剂，这产生了意想不到的，令人惊讶的高OER活性-与商业贵RuO 2催化剂相当，尽管纯CNT具有相当差的OER活性。结合实验和计算的研究表明，所观察到的极好的OER活性可以归因于作为活性中心的CNT中的固有拓扑缺陷和作为助催化剂的涂覆的聚合物层的协同效应，以优化用于改善OER能量学的中间体的吸附能。
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.