首页|磷化调控构筑分层结构的Ni2P催化剂用于高效电氧化尿素

磷化调控构筑分层结构的Ni2P催化剂用于高效电氧化尿素

扫码查看
尿素电解对于发展可持续、清洁的能源转化技术,以应对全球能源短缺和环境问题的挑战具有重要意义.因此,设计有效的尿素氧化电催化剂,深入了解中心金属离子的电子环境,对实现高性能的尿素基能量转换技术具有重要意义.在本文中,我们成功合成了分层结构的Ni2P纳米片@纳米棒,简称P-Ni2P HNNs,作为能够提高尿素氧化反应效率的高效电催化剂.这一催化剂的设计采用了水解共沉淀-氧化工艺和磷取代法.X射线吸收精细结构谱分析表明,P-Ni2P HNNs具有较高的尿素氧化电化学活性,其中Nin+金属的电子结构能够增强Ni―O―O键的耦合,从而提高了尿素氧化反应的动力学性能.由于Nin+金属活性中心以及结构的巧妙设计,P-Ni2P HNNs表现出卓越的尿素氧化反应活性和稳定性.在10 mA∙cm-2时,其过电位低至132 mV,Tafel斜率为33.7 mV∙dec-1,同时在10 mA∙cm-2时的稳定性可达6 h.此外,采用P-Ni2P HNNs-2/NF作为阳极组装成尿素电解电池.该装置在10 mA∙cm-2时获得1.411 V的低电位,在1.595 V时可达100 mA∙cm-2的高电流密度.本研究提供了一种有效可行的方法,用于设计高效的镍基磷化催化剂,有望推动磷化物在各种能源相关应用方面的进一步研究.
P-Regulated Hierarchical Structure Ni2P Assemblies toward Efficient Electrochemical Urea Oxidation
Urea electrolysis is critically important for the advancement of sustainable and clean energy conversion technologies,addressing global energy shortages and environmental concerns.The urea oxidation reaction(UOR)poses a significant challenge due to its unfavorable thermodynamics,making it a pivotal step in urea splitting.The 6-electron transfer process of UOR presents a bottleneck due to its sluggish kinetics.Consequently,the development of efficient urea oxidation electrocatalysts and gaining insights into the electronic configuration of the central metal ion are of paramount significance in achieving high-performance urea-based energy conversion technologies.In this study,we report the successful synthesis of hierarchical Ni2P nanosheets@nanorods(P-Ni2P HNNs)as promising catalysts to enhance UOR efficiency.This catalyst is designed and constructed using a hexamethylenetetramine-hydrolytic coprecipitation-oxidation process and a straightforward phosphorus-substituted method.X-ray absorption fine structure spectroscopy indicates that the presence of P-modified metal centers is responsible for the elevated UOR activity of P-Ni2P HNNs,with the electronic structure of Nin+significantly enhancing Ni―O―O bond coupling for rapid UOR kinetics.Thanks to the highly exposed Nin+centers and the well-designed architecture,P-Ni2P HNNs exhibit superior UOR activity and stability,with a low overpotential of 132 mV at 10 mA∙cm-2,a small Tafel slope of 33.7 mV∙dec-1,and sustained durability for 6 h at 10 mA∙cm-2.Furthermore,a two-electrode cell for overall urea electrolysis is assembled with a P-Ni2P HNNs-2/NF anode,yielding a low potential of 1.411 V at 10 mA∙cm-2 and a high current density of 100 mA∙cm-2 at 1.595 V.This study presents an effective and viable approach for designing and synthesizing high-efficiency nickel-based phosphide electrocatalysts,which could pave the way for cost-effective and energy-efficient electrochemical hydrogen production,and advance phosphide research for various energy-related applications.

Porous hierarchical structurePhosphorus strategyElectrocatalysisNi2PUrea oxidation

李清、张光勋、徐玉霞、孙洋洋、庞欢

展开 >

扬州大学广陵学院,江苏 扬州 225009

扬州大学化学化工学院,江苏 扬州 225009

多孔分层结构 磷化策略 电催化 Ni2P 尿素氧化

Project of Jiangsu Qinglan.国家自然科学基金江苏省自然科学基金教育部长江学者计划江苏省青蓝工程资助项目

U1904215BK20200044Q2018270

2024

物理化学学报
中国化学会

物理化学学报

CSTPCD北大核心
影响因子:0.951
ISSN:1000-6818
年,卷(期):2024.40(9)