Xu Siran, Yu Xin, Liu Xian, Teng Chunlin, Du Yeshuang, Wu Qi
College of Chemistry and Chemical Engineering, Hubei Normal University, Huangshi 435002 China.
College of Chemistry and Chemical Engineering, Hubei Normal University, Huangshi 435002 China.
J Colloid Interface Sci. 2020 Oct 1;577:379-387. doi: 10.1016/j.jcis.2020.05.097. Epub 2020 May 26.
Developing highly efficient and low-cost electrocatalysts with superior durability for hydrogen evolution reaction (HER) is a big challenge. Here, we design and fabricate a highly efficient electrocatalyst with unique three-dimensional (3D) porous peony-like micro-flower Mn-CoP nano-structure on flexible carbon cloth (Mn-CoP PMFs/CC), which exhibits high electrocatalytic activity toward the HER in both acid and alkaline circumstances. Remarkably, benefiting from the unique 3D porous structure with large surface areas, good electron conductivity for fast electron transport, and effective channels for the release of gas, the resultant catalyst exhibits an ultra-low overpotential of 28 and 90 mV to arrive the current density of 10 mA/cm in 0.5 M HSO and 1.0 M KOH solutions, respectively. Meanwhile, the Mn-CoP PMFs/CC material shows small Tafel slopes and good long-term stability in acid and alkaline media. Density Functional Theory (DFT) calculations illustrate that Mn doping indeed improve electron transfer, and makes the thermo-neutral hydrogen adsorption free energy (ΔG) of CoP on the surface of (0 1 1) sharply close to zero, which is very conducive to the adsorption and desorption of hydrogen, thereby making Mn-CoP PMFs/CC with significant enhanced electrocatalytic HER performance. Our 3D porous electrocatalyst has greatly promoted the efficient electrolysis of water to produce hydrogen.
开发具有卓越耐久性的高效低成本析氢反应(HER)电催化剂是一项巨大挑战。在此,我们在柔性碳布上设计并制备了一种具有独特三维(3D)多孔牡丹状微花Mn-CoP纳米结构的高效电催化剂(Mn-CoP PMFs/CC),其在酸性和碱性环境中均对HER表现出高电催化活性。值得注意的是,得益于具有大表面积的独特3D多孔结构、有利于快速电子传输的良好电子导电性以及气体释放的有效通道,所得催化剂在0.5 M HSO和1.0 M KOH溶液中分别表现出28和90 mV的超低过电位以达到10 mA/cm的电流密度。同时,Mn-CoP PMFs/CC材料在酸性和碱性介质中显示出小的塔菲尔斜率和良好的长期稳定性。密度泛函理论(DFT)计算表明,Mn掺杂确实改善了电子转移,并使CoP在(0 1 1)表面的热中性氢吸附自由能(ΔG)急剧接近零,这非常有利于氢的吸附和解吸,从而使Mn-CoP PMFs/CC具有显著增强的电催化HER性能。我们的3D多孔电催化剂极大地促进了水的高效电解制氢。