1] School of Chemical Engineering, University of Adelaide, Adelaide, South Australia 5005, Australia [2] Australian Institute for Bioengineering and Nanotechnology, University of Queensland, Brisbane, Queensland 4072, Australia [3].
1] School of Chemical Engineering, University of Adelaide, Adelaide, South Australia 5005, Australia [2].
Nat Commun. 2014 Apr 28;5:3783. doi: 10.1038/ncomms4783.
Electrocatalytic reduction of water to molecular hydrogen via the hydrogen evolution reaction may provide a sustainable energy supply for the future, but its commercial application is hampered by the use of precious platinum catalysts. All alternatives to platinum thus far are based on nonprecious metals, and, to our knowledge, there is no report about a catalyst for electrocatalytic hydrogen evolution beyond metals. Here we couple graphitic-carbon nitride with nitrogen-doped graphene to produce a metal-free hybrid catalyst, which shows an unexpected hydrogen evolution reaction activity with comparable overpotential and Tafel slope to some of well-developed metallic catalysts. Experimental observations in combination with density functional theory calculations reveal that its unusual electrocatalytic properties originate from an intrinsic chemical and electronic coupling that synergistically promotes the proton adsorption and reduction kinetics.
通过析氢反应将水电化学还原为氢气可能为未来提供可持续的能源供应，但由于使用了贵金属铂催化剂，其商业应用受到了阻碍。到目前为止，所有替代铂的方法都基于非贵金属，据我们所知，没有关于超越金属的电催化析氢催化剂的报道。在这里，我们将石墨相氮化碳与氮掺杂石墨烯结合，制得了一种无金属的杂化催化剂，该催化剂具有出人意料的析氢反应活性，其过电势和塔菲尔斜率与一些发达的金属催化剂相当。实验观察与密度泛函理论计算相结合表明，其异常的电催化性能源于内在的化学和电子耦合，协同促进了质子吸附和还原动力学。
