采用富磷化思路提升过渡金属磷化物电催化析氢性能的研究

Transition metal phosphides (TMPs) have attracted much attentions as promising candidates for anode materials of electrochemical water-splitting due to their high electrocatalytic activities. On the basis of deep understanding the relationship between the structure, composition and the electrocatalytic properties, seeking the strategies of promoting their electrocatalytic performance is critical to develop TMPs as the electrode of electrochemical water-splitting. Aiming at the above scientific problem, we propose the strategies of high phosphorus (P) content in phosphide and low-dimensional nanostructured electrode to enhance the catalytic activities of TMPs in this project. We will develop new method to synthesize TMPs with high P content and investigate their growth mechanism. In this project in order to prepare low-dimensional nanostructured electrode, the laser ablation in liquids will be used to synthesize TMPs nanostructures with different sizes and morphologies, and the relationship between particle size/morphologies and the electrocatalytic properties will be concluded. Combined with the first-principle theory calculations, the influence of the chemical compositions and the crystalline structure on the catalytic properties will be investigated. Successful employing above strategies would significantly improve the electrocatalytic performance of TMPs towards hydrogen production, and consequently provide theoretical basis and experimental foundation for a cost-effective way of hydrogen production via electrochemical water-splitting.

开发廉价、高效的电催化活性材料用于电解水制氢是解决当前环境污染和能源危机的有效途径，近年来过渡金属磷化物由于具有优良的电催化产氢活性和稳定性备受关注。在深刻理解结构、组分与催化性能的影响规律基础上寻求提高催化产氢活性途径是开发过渡金属磷化物作为电解水制氢电极材料的关键。根据以上关键问题，本项目提出富磷化结合低维纳米化改性方式提升过渡金属磷化物催化产氢性能的研究思路。探索制备过渡金属多磷化合物的新方法；掌握影响材料结晶质量和形貌的关键因素，探讨多磷化物的生长机制；利用激光液相烧蚀技术，低维纳米化晶粒结构，探索微观结构参数与催化性能间的影响规律；结合理论计算和实验数据，揭示材料的组分、结构与催化性能的影响规律和物理机制。最终利用富磷化和结构低维纳米化协同控制技术，实现过渡金属多磷化合物电催化产氢性能的大幅度提升，为寻求电解水制氢的节能新途径提出有效的理论基础和实验依据。

开发廉价、高效的电催化活性材料用于发展电解水制氢技术是解决当前环境污染和能源危机的有效途径，近年来过渡金属磷化物具有优良的电催化产氢活性和稳定性备受关注。在深刻理解结构、组分与催化性能的影响规律基础上寻求提高催化产氢活性的途径是开发过渡金属磷化物作为电解水制氢电极材料的关键。根据以上关键问题，本项目提出富磷化结合低维纳米化改性方式提升过渡金属磷化物的催化产氢活性的研究思路。经过几年的研究，项目取得了以下三方面的研究成就：1，探索了过渡金属多磷化合物合成制备的新方法，采用真空封管技术，控制烧结工艺参数对产物化学组成、结晶度及微观结构的影响及作用机制，实现了具有高比表面积的过渡金属多磷化合物纳米结构的可控生长。2，发展出过渡金属磷化物纳米阵列的自支撑电极制备方法，克服了颗粒催化剂脱落和传导电子受阻的问题。在导电衬底碳纸、碳布直接生长多磷化物纳米阵列，形成自支撑的工作电极用于电催化分解水，探究出材料物相和微结构参数与电催化产氢性能间的相互影响规律，探索出用于指导提升电催化产氢活性的方法。3，利用富磷化和结构低维纳米化协同控制技术，实现过渡金属多磷化合物电催化产氢性能的大幅度提升。该研究项目利用富磷化和结构低维纳米化协同控制技术，实现了过渡金属多磷化合物电催化产氢性能的大幅度提升，为寻求电解水制氢的节能新途径提出有效的理论基础和实验依据。