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Hydrogen evolution reactions boosted by bridge bonds between electrocatalysts and electrodes

机译:析氢反应提高了桥债券electrocatalysts和电极之间

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The interfacial interactions between nanostructured electrode materials and electrodes play an important part in the performance enhancement of electrochemical energy devices. However, the mechanism of interfacial interactions, as well as its influence on device performance, still remains unclear and is rarely studied. In this work, a CoS2 nanobelt catalyst assembled on Ti foil (CoS2 nanobelts/Ti) is prepared through in situ chemical conversions and chosen as an example to probe the interfacial interactions between the CoS2 catalyst and the Ti electrode, and the correlation between the interfacial interaction and the hydrogen evolution reaction (HER) performance. By a series of characterization studies and analyses, we propose that interfacial bridge bonds (Ti-S-Co and Ti-O-Co) in a covalent form may exist in the CoS2 nanobelts/Ti as well as its precursor Co(OH)(3) nanobelts growing on Ti foil, which is further supported by density functional theory (DFT) calculations. Moreover, as a binder-free electrocatalytic electrode, the CoS2 nanobelts/Ti shows boosted HER performance, including higher catalytic activity, and lower overpotential and Tafel slope, compared to its counterpart transformed from a solution-produced precursor. The HER performance enhancement is ascribed to the existence of interfacial bridge bonds that not only strengthen the electrode-catalyst mechanical integrity, but also serve as efficient charge transfer channels between the electrode and the catalyst, thus ensuring a stable and fluent electron transfer for the HER. Furthermore, the DFT calculations reveal that the CoS2 nanobelts/Ti catalyst with interfacial covalent interactions can facilitate the adsorption of H+ ions/H-2 molecules and the desorption of H-2 molecules for an accelerated HER. This work provides a new insight into the interfacial interactions between electrodes and electrode materials in electrochemical devices, and paves the way for the rational design and construction of high-performance electrochemical devices for practical energy applications.
机译:之间的界面相互作用纳米电极材料和电极发挥重要作用的性能增强电化学能源设备。然而,界面的机制相互作用,以及对设备的影响性能,仍然不清楚,很少研究。装配在钛箔(CoS2纳米/ Ti)通过原位化学转换和准备选择为例,调查界面CoS2催化剂之间的相互作用和Ti电极之间的相关性界面交互和氢进化反应(她)性能。特性的研究和分析,我们建议界面(Ti-S-Co桥债券和Ti-O-Co)以共价键形式可能存在CoS2纳米/ Ti及其前体有限公司(OH)(3)纳米钛箔上生长,这是通过密度泛函理论进一步支持(DFT)计算。electrocatalytic电极,CoS2纳米/ Ti显示了她的表演,包括高催化活性和降低过电压和塔菲尔斜率,而其对手从一个solution-produced前体。归因于她的性能增强界面的存在桥债券不仅加强electrode-catalyst机械完整性,也作为有效电极之间的电荷转移渠道和催化剂,从而确保稳定她流利的电子转移。此外,DFT计算揭示的CoS2纳米/钛催化剂界面共价相互作用可以促进吸附和H +离子/ h2o分子为加速解吸,氢分子她的界面和电极之间的相互作用电极材料的电化学设备,,为合理设计和铺平了道路建设高性能电化学为实际能源应用设备。

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