Reduction of Graphene Oxide by Hydrogen Sulfide: A Promising Strategy for Pollutant Control and as an Electrode for Li‐S Batteries
Reduction of Graphene Oxide by Hydrogen Sulfide: A Promising Strategy for Pollutant Control and as an Electrode for Li‐S Batteries
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DOI：
10.1002/aenm.201301565
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发表时间：
2014-05
影响因子：
27.8
通讯作者：
Chen Zhang;Wei Lv;Weiguo Zhang;Xiaoyu Zheng;Mingbo Wu;Wei Wei-Wei;Ying Tao;Zhengjie Li;
中科院分区：
文献类型：
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作者：
Chen Zhang;Wei Lv;Weiguo Zhang;Xiaoyu Zheng;Mingbo Wu;Wei Wei-Wei;Ying Tao;Zhengjie Li;
DOI：10.1002/aenm.201301565对环境友好型工业和有效污染控制的日益增长的需求引起了学术界和工业组织对新工艺和新材料开发的极大关注。硫化氢（H2S）是一种主要的大气污染物，其来源广泛（天然气加工、化石燃料的提炼和消耗等）由于其对环境（酸雨）和生物体的高毒性，必须紧急去除和再利用。[ 1 ]人们在探索有效去除H2S方面做了大量工作，在大多数情况下，过渡金属氧化物和混合氧化物被用作H2S氧化的吸附剂和/或催化剂，而其他人则使用沸石、活性炭（AC）和碳纳米管（CNT）作为吸附剂。[2，3]碳材料作为吸附剂或催化剂载体具有吸引人的特性，可用于脱除H2S。例如，活性炭或碳纳米管已被广泛用作催化剂（ZnO，NiS 2等）的载体.催化氧化硫化氢。[ 3 ]然而，H2S的再生和充分利用以及高性能吸附剂的开发仍难以实现。因此，有必要开发一种合适的方法来消除和回收H2S，以实现其再生和环境保护。作为一种迷人的碳材料，石墨烯由于其独特的2D结构而具有优异的电学，热学和机械性能，使其在基础科学和各种应用中用途广泛，如能量存储，传感器，吸附等。石墨烯在去除H2S中的应用已经在实验和理论上进行了检验。[ 1a，2，5 ]密度泛函理论（DFT）研究表明，H 2 S分子仅物理吸附在石墨烯表面，因此，在大多数情况下，石墨烯对H 2 S氧化的催化活性较低，吸附容量也较低。氧化石墨烯（GO）是石墨烯最重要的衍生物，在石墨烯层上修饰了大量的含氧基团，由于其亲水性，这些基团有助于改善反应性和加工性能。虽然GO由于连续sp 2的破坏而具有差的导电性，
DOI: 10.1002/aenm.201301565 The increasing demand for environmentally friendly industries and effective pollution control has attracted great attention from both academic and industrial organizations for the development of new processes and novel materials. As a major air pollutant, hydrogen sulfi de (H 2 S), originating from various sources (natural gas processing, the refi ning and consumption of fossil fuel, etc.) must urgently be removed and reused due to its high toxicity towards the environment (acid rain) and living organisms. [ 1 ] Great efforts have been made to explore the effective removal of H 2 S and in most cases transitionmetal oxides and mixed oxides are used as adsorbents and/or catalysts for the oxidation of H 2 S, whereas others use zeolite, activated carbon (AC), and carbon nanotubes (CNTs) as adsorbents. [ 2,3 ] Carbon materials have appealing properties as adsorbents or catalyst supports for the removal of H 2 S. For instance, AC or CNTs have been widely used as supports of catalysts (ZnO, NiS 2 , etc.) for the catalytic oxidation of H 2 S. [ 3 ] Nevertheless, the regeneration and full utilization of the H 2 S and the development of high-performance adsorbents are still hard to realize. Thus, it is necessary to develop an appropriate approach to eliminate and recycle H 2 S to realize its regeneration and environmental protection. As a fascinating carbon material, graphene possesses excellent electrical, thermal, and mechanical properties due to its unique 2D structure, making it versatile in fundamental science and various applications, such as energy storage, sensors, adsorption, etc. [ 4 ] Due to its large and fully accessible surface and excellent conductivity, the use of graphene in the removal of H 2 S has been examined both experimentally and theoretically. [ 1a, 2, 5 ] Density functional theory (DFT) studies show that H 2 S molecules are physisorbed only on the surface of graphene, thus, in most cases, graphene has a low catalytic activity for H 2 S oxidation and also a low adsorption capacity. Graphene oxide (GO), the most important derivative of graphene, is decorated by abundant oxygen-containing groups on the graphene layer, and these help improve the reactivity and processability due to their hydrophilic nature. Although GO suffers from poor conductivity due to the destruction of the continuous sp 2