As a vital chemical,ammonia(NH3)plays an irreplaceable role in many fields such as chemical synthesis and energy storage.Green renewable biomass can be converted into biofuels,but its nitrogen resources are underused ...As a vital chemical,ammonia(NH3)plays an irreplaceable role in many fields such as chemical synthesis and energy storage.Green renewable biomass can be converted into biofuels,but its nitrogen resources are underused throughout.Laser-driven pyrolysis is envisaged to debuts as a bridge to connect them to realize the direct conversion from nitrogen-rich biomass into ammonia.The pulsed laser-induced local-transient thermal effect recognized the biological nitrogen resources conversion,such as cheap and plentiful yeasts,to small gaseous molecules and achieved spectacular ammonia production rate up to 260.4 mg/h,an order of magnitude higher performance than thermochemical ammonia synthesis.Simultaneously,the tiny hot point generated by a low-energy laser(20W)guarantees the whole ammonia synthesis reaction systemis in amild environment of low temperature and normal pressure.Additionally,the remaining solid residue after laser-driven pyrolysis also can be further exploited as a highly active catalyst for electrocatalytic nitrate reduction reaction(NIRR).展开更多
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 nano...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.展开更多
基金Taishan Scholar Project of Shandong Province,Grant/Award Number:tsqn201812083Natural Science Foundation of Shandong Province,Grant/Award Numbers:ZR2021JQ15,ZR2022YQ42,ZR2020QE057,2022GJJLJRC-01+1 种基金Innovative Team Project of Jinan,Grant/Award Number:2021GXRC019National Natural Science Foundation of China,Grant/Award Numbers:51972147,52022037,52202366。
文摘As a vital chemical,ammonia(NH3)plays an irreplaceable role in many fields such as chemical synthesis and energy storage.Green renewable biomass can be converted into biofuels,but its nitrogen resources are underused throughout.Laser-driven pyrolysis is envisaged to debuts as a bridge to connect them to realize the direct conversion from nitrogen-rich biomass into ammonia.The pulsed laser-induced local-transient thermal effect recognized the biological nitrogen resources conversion,such as cheap and plentiful yeasts,to small gaseous molecules and achieved spectacular ammonia production rate up to 260.4 mg/h,an order of magnitude higher performance than thermochemical ammonia synthesis.Simultaneously,the tiny hot point generated by a low-energy laser(20W)guarantees the whole ammonia synthesis reaction systemis in amild environment of low temperature and normal pressure.Additionally,the remaining solid residue after laser-driven pyrolysis also can be further exploited as a highly active catalyst for electrocatalytic nitrate reduction reaction(NIRR).
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)+5 种基金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 MaterialsThe 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-IS09-0003The 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.
文摘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.