Rapid laser synthesis of surfactantless tantalum-based nanomaterials as bifunctional catalysts for direct peroxide–peroxide fuel cells  

作　　者：Xiaoyong Mo Brigitte Bouchet Fabre Nathalie Herlin-Boime Edmund C.M.Tse 

机构地区：[1]HKU-CAS Joint Laboratory on New Materials,Department of Chemistry,University of Hong Kong,Hong Kong SAR,China [2]NIMBE,CEA,CNRS,CEA Saclay,UniversitéParis-Saclay,Gif-sur-Yvette,France [3]HKU Zhejiang Institute of Research and Innovation,Hangzhou,China

出　　处：《SmartMat》2023年第6期84-97,共14页智能材料（英文）

基　　金：Edmund C.M.Tse would like to express gratitude to the National Natural Science Foundation of China(NSFC)for providing a Young Scientists Fund(No.22002132);the European Union(EU)for sponsoring the SABYDOMA project via the Horizon 2020 program(H2020:862296);on energy catalysis and sustainable nanomaterials.Xiaoyong Mo thanks Frankie Y.F.Chan at the Electron Microscope Unit(EMU)at the University of Hong Kong(HKU)for his help with the characterization of nanomaterials.Xiaoyong Mo was supported by an Algaia-HKU Chemistry RPg Award and an SZSTI Basic Science General Program(No.JCYJ20210324122011031);The authors thank the Research Grants Council(RGC)in Hong Kong(China)for an EU-HK Research and Innovation Cooperation Co-funding Mechanism(RGC:E-HKU704/19);a CAS-RGC Joint Laboratory Funding Scheme(RGC:JLFS/P-704/18);an Early Career Scheme(RGC:27301120)for expanding the electrochemical investigation capability as well as upgrading the nanomaterials characterization instruments at the HKU-CAS Joint Laboratory on New Materials;The authors also thank the support provided by the National Research Agency(ANR)through the SNON(Sun light oxi-nitrides for energetic applications project)project reference ANR-13-IS09-0003;The help of two Master students,Laura Line Risal and Shunxing Deng,is gratefully acknowledged.The authors are also grateful to Jocelyne Leroy and Eddy Foy for performing XPS and XRD analyses.

摘　　要：Efficient and durable electrocatalysts are instrumental in enabling next-generation fuel cell technologies.At present,expensive precious metals are used as state-of-the-art catalysts.In this report,cost-effective nanosized tantalum-based alternatives are synthesized for the first time via a green and scalable laser pyrolysis method as bifunctional catalysts for direct peroxide–peroxide fuel cells.This rapid laser pyrolysis strategy allows for the production of nanoparticles at a laboratory scale of grams per hour,compatible with a detailed exploration of the functional properties of as-synthesized nanoparticles.By varying the precursor ratio between ammonia and tantalum ethanolate,five tantalum-based nanomaterials(TaNOC)are prepared with crystalline phases of Ta_(2)O_(5),Ta_(4)N_(5),Ta_(3)N_(5),and TaN in tunable ratios.Electrochemical studies in neutral and alkaline conditions demonstrate that Ta_(4)N_(5) is the active component for both H_(2)O_(2) oxidation and reduction.Kinetic isotope effect studies show that protons are involved at or before the rate-determining step.Long-term stability studies indicate that Ta_(3)N_(5) grants surfactant-free TaNOC-enhanced longevity during electrocatalytic operations.Taken together,bifunctional TaNOC can act as active and robust electrocatalysts for H_(2)O_(2) reduction and oxidation.Laser pyrolysis is envisioned to produce refractory metal nanomaterials with boosted corrosion resistance for energy catalysis.

关 键 词：bifunctional catalysis laser pyrolysis peroxide fuel cells tantalum nanomaterials 

分 类 号：O64[理学—物理化学]