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Composition-optimized manganese phosphide nanoparticles anchored on porous carbon network for efficiently electrocatalytic hydrogen evolution
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2023-06-02 , DOI: 10.1016/j.cej.2023.143879
Wangzhi Wu, Yujin Huang, Xueqian Wang, Pei Kang Shen, Jinliang Zhu

Electrocatalytic water splitting is an efficient method for producing high purity hydrogen and has the advantage of emitting zero waste. Manganese phosphides are considered to be promising electrocatalysts for the hydrogen evolution reaction (HER) with their electrocatalytic properties being composition-dependent. In this work, we achieved the targeted synthesis of manganese-rich Mn2P, phosphorus-rich MnP, and their heterostructure Mn2P-MnP nanoparticles dispersed uniformly on a P, N-doped carbon network (Mn2P-MnP/PNC) through a facile strategy involving the use of phosphate resin derived with potassium hydroxide. Systematic studies were conducted on formation mechanism of Mn2P-MnP/PNC. Density functional theory (DFT) calculations indicate that Mn2P-MnP has an optimized electronic structure and Gibbs free energy of H adsorption, with that of Mn2P-MnP (0.057 eV) being closest to zero compared to Mn2P (-0.306 eV) and MnP (0.325 eV). The Mn2P-MnP/PNC only requires small overpotentials of 63 and 98 mV to achieve 10 mA cm−2 for HER in H2SO4 and KOH solution, respectively. Furthermore, Mn2P-MnP/PNC exhibits ultrahigh stability for HER in both acid and alkaline solutions, retaining a current rate of 98.18% and 97.57% after 96 and 120 h chronoamperometry tests, respectively.



中文翻译:

锚定在多孔碳网络上的组成优化的磷化锰纳米颗粒用于高效电催化析氢

电催化水分解是生产高纯度氢气的有效方法,具有零排放的优点。磷化锰被认为是用于析氢反应 (HER) 的有前途的电催化剂,其电催化性能与组成有关。在这项工作中,我们实现了富锰Mn 2 P、富磷MnP及其均匀分散在P、N掺杂碳网络上的异质结构Mn 2 P-MnP纳米粒子的靶向合成(Mn 2 P-MnP/PNC ) 通过一种简单的策略,涉及使用氢氧化钾衍生的磷酸盐树脂。对Mn 2的形成机理进行了系统研究P-MnP/PNC。密度泛函理论 (DFT) 计算表明 Mn 2 P-MnP 具有优化的电子结构和 H 吸附吉布斯自由能,与 Mn 2 P (-) 相比,Mn 2 P -MnP (0.057 eV) 最接近零0.306 eV) 和 MnP (0.325 eV)。Mn 2 P-MnP/PNC 仅需要 63 和 98 mV 的小过电势即可分别在 H 2 SO 4和 KOH 溶液中实现 10 mA cm -2的 HER 。此外,Mn 2 P-MnP/PNC 在酸性和碱性溶液中均表现出超高的 HER 稳定性,在 96 小时和 120 小时计时电流法测试后分别保持 98.18% 和 97.57% 的电流速率。

更新日期:2023-06-07
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