机构地区:[1]扬州大学化学化工学院,江苏扬州225002 [2]NanoScience Technology Center,University of Central Florida,Orlando,FL 32826,USA [3]Department of Chemical Sciences,Ariel University,Ariel 40700,Israel
出 处:《物理化学学报》2023年第9期99-108,共10页Acta Physico-Chimica Sinica
基 金:国家自然科学基金(21972124,22102105,22272148)资助项目。
摘 要:实现绿色甲醇电解制氢需要高效的双功能催化剂。本文采用热处理结合乙二醇还原法成功制备了MoP-NC纳米球负载的超细Pt纳米粒子(平均粒径为2.53 nm)复合催化剂(Pt/MoP-NC)用于高效甲醇电解制氢。MoP-NC纳米球不仅能提高Pt纳米粒子的分散性并且增强Pt的抗中毒能力。电化学测试表明Pt/MoP-NC催化剂在酸性甲醇氧化反应(MOR)和析氢反应(HER)中具有较高的催化性能;其中,MOR的正向扫描峰值电流密度为90.7 m A·cm^(-2),是商业Pt/C催化剂的3.2倍,在10 mA·cm^(-2)的电流密度下,HER的过电位低至30 m V,与商业Pt/C接近。由Pt/MoP-NC||Pt/MoP-NC组装的两电极电解槽驱动10 mA·cm^(-2)的电流密度仅需要0.67 V的电压,比相同条件下电解水的电压低1.02 V,大大降低了能量输入。Pt/MoP-NC的高催化性能主要来源于Pt活性中心与相邻层状多孔球形结构的MoP-NC载体之间电子效应及配体效应引起的抗一氧化碳中毒能力的提升和含氧物种的容易生成。Hydrogen energy is a potential energy storage carrier due to its advantages of cleanliness,high efficiency and renewability.Electrocatalytic water splitting is an ideal method to generate hydrogen,and the slow kinetics of water oxidation,namely,oxygen evolution reaction(OER),greatly restricts its practical application.To reduce the energy consumption required for OER,methanol oxidation reaction(MOR)with a much lower theoretical potential is very promising to replace OER to assist hydrogen generation.The theoretical potential of MOR is only 0.016 V vs.SHE(standard hydrogen electrode),which is much lower than that of OER(1.23 V),and the energy-saving can be about 60%compared to that of traditional water electrolysis.Therefore,using MOR instead of OER to realize methanol electrolysis for hydrogen production is an effective way to reduce energy consumption.An efficient bifunctional catalyst is very important for green hydrogen generation from overall methanol electrolysis.Currently,Pt-based materials are still the best catalyst for hydrogen evolution reaction(HER)and MOR,while they are more challenging in the MOR as they are prone to intermediates poisoning during the catalytic reactions.The introduction of transition metal-based promoters such as phosphides is an effective strategy to promote the catalytic ability for methanol oxidation.Herein,ultrafine Pt nanoparticles with an average particle size of 2.53 nm evenly grown on MoPNC nanosphere(Pt/MoP-NC)were demonstrated as an efficient electrocatalyst for methanol electrolysis towards hydrogen generation.The introduction of MoP-NC nanospheres support not only restricts the aggregation of Pt,but also improves the catalytic performance and anti-poisoning ability.Specifically,Pt/MoP-NC catalyst exhibited high methanol oxidation performance with a peak current density of 90.7 mA·cm^(-2),which was 3.2 times higher than that of commercial Pt/C catalysts,and good hydrogen evolution reaction performance with a low overpotential of 30 mV to offer 10 mA·cm^(-2)in an acid me
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