首页|调制双金属掺杂氮碳基纳米颗粒的电子态以实现增强的氧还原动力学

调制双金属掺杂氮碳基纳米颗粒的电子态以实现增强的氧还原动力学

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控制活性成分的局域电子结构以改善含氧中间体在电化学固液界面上的吸脱附特性是电催化氧还原反应催化领域的关键挑战.本文通过双金属共掺杂到碳氮基底中来调节金属纳米晶的电子态,从而实现催化活性中心电子结构的调制.首先,设计合成了一种典型的双金属纳米颗粒催化剂(Fe-Co NP/NC),灵活地调控电催化氧还原反应的反应动力学.同步辐射X射线吸收谱和X射线光电子能谱结果表明,铁和钴物种的共掺杂可以优化Fe-Co NP/NC催化剂的本征电荷分布,促进氧还原动力学,并最终获得了显著的电催化氧还原反应电催化活性.Fe-Co NP/NC催化剂在0.80 V工作电压下表现出超高的动力学电流密度(71.94 mA/cm2),半波电位达0.915 V,明显优于相应的单组分金属纳米颗粒样品.该研究发现为优化活性中心的电子结构以实现更优异的电催化氧还原反应催化活性和更快的反应动力学提供了一种通用的策略.
Modulation of Electronic States in Bimetallic-doped Nitrogen-Carbon Based Nanoparticles for Enhanced Oxygen Reduction Kinetics
Controlling the local electronic structure of active ingredients to improve the adsorption-desorption characteristics of oxygen-contain-ing intermediates over the electro-chemical liquid-solid interfaces is a critical challenge in the field of oxy-gen reduction reaction(ORR)catalysis.Here,we offer a simple approach for modulating the electronic states of metal nanocrystals by bimetal co-doping in-to carbon-nitrogen substrate,allowing us to modulate the electronic structure of catalytic ac-tive centers.To test our strategy,we designed a typical bimetallic nanoparticle catalyst(Fe-Co NP/NC)to flexibly alter the reaction kinetics of ORR.Our results from synchrotron X-ray absorption spectroscopy and X-ray photoelectron spectroscopy showed that the co-dop-ing of iron and cobalt could optimize the intrinsic charge distribution of Fe-Co NP/NC cata-lyst,promoting the oxygen reduction kinetics and ultimately achieving remarkable ORR ac-tivity.Consequently,the carefully designed Fe-Co NP/NC exhibits an ultra-high kinetic cur-rent density at the operating voltage(71.94 mA/cm2 at 0.80 V),and the half-wave potential achieves 0.915 V,which is obviously better than that of the corresponding controls including Fe NP/NC,Co NP/NC.Our findings provide a unique perspective for optimizing the elec-tronic structure of active centers to achieve higher ORR catalytic activity and faster kinetics.

Oxygen reduction reactionReaction kineticsElectronic state modulationCo-dopingElectrocatalysis

龚宸、杨晨宇、周婉琳、苏徽、刘庆华

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中国科学技术大学国家同步辐射实验室,合肥 230029

湖南师范大学化学化工学院,长沙 410081

氧还原反应 反应动力学 电子态调制 共掺杂 电催化

Natural Science Foundation of Anhui ProvinceNatural Science Foundation of Anhui Province

2208085J012208085QA28

2024

10.1063/1674-0068/cjcp2304033

化学物理学报(英文版)
中国物理学会

化学物理学报(英文版)

CSTPCDEI
影响因子：0.162
ISSN：1674-0068
年,卷(期)：2024.37(4)