Liu Wen, Hu Enyuan, Jiang Hong, Xiang Yingjie, Weng Zhe, Li Min, Fan Qi, Yu Xiqian, Altman Eric I, Wang Hailiang
Department of Chemistry and Energy Sciences Institute, Yale University, 520 West Campus Drive, West Haven, Connecticut 06511, USA.
Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973, USA.
Nat Commun. 2016 Feb 19;7:10771. doi: 10.1038/ncomms10771.
Rational design and controlled synthesis of hybrid structures comprising multiple components with distinctive functionalities are an intriguing and challenging approach to materials development for important energy applications like electrocatalytic hydrogen production, where there is a great need for cost effective, active and durable catalyst materials to replace the precious platinum. Here we report a structure design and sequential synthesis of a highly active and stable hydrogen evolution electrocatalyst material based on pyrite-structured cobalt phosphosulfide nanoparticles grown on carbon nanotubes. The three synthetic steps in turn render electrical conductivity, catalytic activity and stability to the material. The hybrid material exhibits superior activity for hydrogen evolution, achieving current densities of 10 mA cm(-2) and 100 mA cm(-2) at overpotentials of 48 mV and 109 mV, respectively. Phosphorus substitution is crucial for the chemical stability and catalytic durability of the material, the molecular origins of which are uncovered by X-ray absorption spectroscopy and computational simulation.
合理设计并可控合成包含具有独特功能的多种组分的杂化结构，是一种用于诸如电催化产氢等重要能源应用的材料开发的有趣且具有挑战性的方法，在电催化产氢领域，迫切需要具有成本效益、活性高且耐用的催化剂材料来替代昂贵的铂。在此，我们报告了一种基于生长在碳纳米管上的黄铁矿结构的钴磷硫化物纳米颗粒的高活性和稳定析氢电催化剂材料的结构设计与分步合成。这三个合成步骤依次赋予材料导电性、催化活性和稳定性。这种杂化材料表现出优异的析氢活性，在过电位分别为48 mV和109 mV时，实现了10 mA cm(-2)和100 mA cm(-2)的电流密度。磷取代对于材料的化学稳定性和催化耐久性至关重要，X射线吸收光谱和计算模拟揭示了其分子根源。
