氧的电催化还原反应是燃料电池装置与金属空气电池的阴极反应,具有重大的研究意义.在众多的非铂催化剂中,碳材料因其低廉的价格以及独特的物理化学性质受到了广泛的关注.自从发现氮掺杂的碳纳米阵列具有优异的氧还原活性后,不同类型的氮掺杂的碳也得到了深入研究.例如近年来兴起的由金属有机框架衍生的氮掺杂的碳材料,兼具丰富的氮位点及良好的三维结构.氮的掺杂对碳原子具有电子调控的作用,是其高氧还原活性的根本原因.本文对金属有机框架衍生的氮掺杂的碳材料进行进一步的电子结构的优化,以提升催化性能.功函是电子逸出表面所需的最少的能量,是材料的电子结构性质之一,其对氧还原反应的影响也有报道,早期以理论计算为基础,探究氧气分子在碳材料表面的解离能与氮掺杂的碳的表面功函的关系,后续则采用开尔文探针显微镜,直接测量了不同元素掺杂的碳表面功函,并建立起功函与氧还原动力学的线性关系.本文通过控制碳材料的功函来调节其电子结构.铯是一种经典的给电子物质,通过将电子注入到掺杂材料表面来降低其功函.因此,本文通过CsCO3与2-甲基咪唑、Zn(NO3)2煅烧形成铯修饰的氮掺杂碳.电镜及XRD均观察不到所得材料中铯的存在,证明碳层中无大颗粒团聚的铯物种.EDS元素分布图表明,铯在碳层中呈原子级均匀分布.Raman谱结果表明,碳的G带发生明显的位置偏移,证明其面内电子结构发生了明显的改变.XPS结果证明铯成功与氮原子配位,通过铯氮键将电子注入到碳骨架.UPS则最终显示,经过铯的修饰,碳表面功函从4.25 eV下降到3.6 eV.表面功函的降低有利于氧气分子的解离,也调节OOH*中间体的吸附,使其吸附的自由能更接近最优值.材料改性后氧还原性能明显提升,起始电位达到0.91 V vs RHE,半波电位达到0.83 V vs RHE,均接近商业Pt/C催化剂.氧还原反应的动力学电流密度随功函的降低而增大,验证了前人的结论.本文提供了一个较为新颖的电子结构调控策略,为设计新的氧还原催化剂提供了新的思路. 相似文献
Cellulose - Dye contamination of water supplies has a serious threat to human health, prompting the development of highly effective and eco-friendly adsorbents. In this work, polyelectrolyte... 相似文献
How to efficiently utilize most abundant biomass of cellulose, lignin and their derivatives has become an emerging challenge as the anticipative oil depletion. In this paper, the ternary anionic copolymer of carboxymethyl cellulose-acrylamide-lignosulfonate (CAL) was successfully prepared by hydrothermal polymerization. Based on the flocculation characteristics of cationic methylene blue, the optimal polymerization process was confirmed as the raw material ratio of 1:1:1, initiator dosage of 0.9 wt %, the reaction time was 5 h and the reaction temperature was 55 °C. The results showed that the decolorization ratio was 87.5% at the CAL dosage of 600 mg/L for the 500 mg/L methylene blue simulated wastewater. The CAL achieved fast flocculation kinetics and super color removal ratios in the wide ranges of environmental pH, temperature and salt concentration. The flocculation mechanism is single charge neutralization. Moreover, the estimated treatment cost of CAL is 68.3% lower than that of commercial anionic PAM. The prepared anionic CAL flocculant has the characteristics of environmental safety, excellent flocculation performance and cost-effectiveness, which shows great potential in the field of dye wastewater treatment, and also provides a feasible way for the effective utilization of biomass resources.
The abuse of antibiotics will cause an increase of drug-resistant strains and environmental pollution,which in turn will affect human health.Therefore,it is important to develop effective detection techniques to determine the level of antibiotics contamination in various fields.Compared with traditional detection methods,electrochemical sensors have received extensive attention due to their advantages such as high sensitivity,low detection limit,and good selectivity.In this mini review,we summarized the latest developments and new trends in electrochemical sensors for antibiotics.Here,modification methods and materials of electrode are discussed.We also pay more attention to the practical applications of antibiotics electrochemical sensors in different fields.In addition,the existing problems and the future challenges ahead have been proposed.We hope that this review can provide new ideas for the development of electrochemical sensors for antibiotics in the future. 相似文献
An efficient sustainable and scalable strategy for the synthesis of porous cobalt/nitrogen co-doped carbons(Co@NCs) via pyrolysis of aniline-modified ZIFs,has been demonstrated.Aniline can coordinate and absorb on the surface of ZIF(ZIF-CoZn3-PhA),accelerate the precipitation of ZIFs,thus resulting in smaller ZIF particle size.Meanwhile,the aniline on the surface of ZIF-CoZn3-PhA promotes the formation of the protective carbon shell and smaller Co nanoparticles,and increases nitrogen content of the catalyst.Because of these prope rties of Co@NC-PhA-3,the oxidative esterification of 5-hydroxymethylfurfural can be carried out under ambient conditions.According to our experimental and computational results,a synergistic catalytic effect between CoN_x sites and Co nanoparticles has been established,in which both Co nanoparticles and CoN_x can activate O_2 while Co nanoparticles bind and oxidize HMF.Moreover,the formation and release of active oxygen species in CoN_x sites are reinfo rced by the electronic interaction between Co nanoparticles and CoN_x. 相似文献