Nanostructured catalyst-integrated electrodes with remarkably reduced catalyst loadings,high catalyst utilization and facile fabrication are urgently needed to enable cost-effective,green hydrogen production via proto...Nanostructured catalyst-integrated electrodes with remarkably reduced catalyst loadings,high catalyst utilization and facile fabrication are urgently needed to enable cost-effective,green hydrogen production via proton exchange membrane electrolyzer cells(PEMECs).Herein,benefitting from a thin seeding layer,bottom-up grown ultrathin Pt nanosheets(Pt-NSs)were first deposited on thin Ti substrates for PEMECs via a fast,template-and surfactant-free electrochemical growth process at room temperature,showing highly uniform Pt surface coverage with ultralow loadings and vertically well-aligned nanosheet morphologies.Combined with an anode-only Nafion 117 catalyst-coated membrane(CCM),the Pt-NS electrode with an ultralow loading of 0.015 mgPt cm−2 demonstrates superior cell performance to the commercial CCM(3.0 mgPt cm^(−2)),achieving 99.5%catalyst savings and more than 237-fold higher catalyst utilization.The remarkable performance with high catalyst utilization is mainly due to the vertically well-aligned ultrathin nanosheets with good surface coverage exposing abundant active sites for the electrochemical reaction.Overall,this study not only paves a new way for optimizing the catalyst uniformity and surface coverage with ultralow loadings but also provides new insights into nanostructured electrode design and facile fabrication for highly efficient and low-cost PEMECs and other energy storage/conversion devices.展开更多
Developing microwave absorption(MA)materials with satisfied comprehensive performance is a great challenge for tackling severe electromagnetic pollution.In particular,the magnetic component/carbon hybrids absorbers al...Developing microwave absorption(MA)materials with satisfied comprehensive performance is a great challenge for tackling severe electromagnetic pollution.In particular,the magnetic component/carbon hybrids absorbers always suffer from high filler loading.Herein,we propose a feasible strategy to construct hierarchical porous carbon with tightly embedded Ni nanoparticles(Ni@NPC).These highly dispersed Ni nanoparticles produce strong magnetic coupling networks to enhance magnetic loss abilities.Moreover,the interconnected hierarchical dielectric carbon network affords favorable dipolar/interfacial polarization,conduction loss,multiple reflection and scattering.Impressively,with an ultralow filler loading of 5 wt.%,the resultant Ni@NPC/paraffin composite achieves an excellent MA performance with a minimum reflection loss of as high as-72.4 dB and a broad absorption bandwidth of 5.0 GHz.This capability outperforms most current magnetic-dielectric hybrids counterparts.Furthermore,the MA capacity can be easily tuned with adjustments in thickness,content and type of magnetic material.Thus,this work opens up new avenues for the development of high-performance and lightweight MA materials.展开更多
Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir d...Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir doped in tetragonal PdO matrix(IrSAs-PdO)via a lattice-confined strategy.The optimized IrSAs-PdO-0.10 exhibited remarkable OER activity with an overpotential of 277 mV at 10 mA·cm^(-2) and long-term stability of 1000 h in 0.5 M H_(2)SO_(4).Furthermore,the turnover frequency attains 1.6 s^(-1) at an overpotential of 300 mV with a 24-fold increase in the intrinsic activity.The high activity originates from isolated iridium sites with low valence states and decreased Ir–O bonding covalency,and the excellent stability is a result of the effective confinement of iridium sites by Ir–O–Pd motifs.Moreover,we demonstrated for the first time that SACs have great potential in realizing ultralow loading of iridium(as low as microgram per square center meter level)in a practical water electrolyzer.展开更多
Despite recent progress in the synthesis and application of graphene-based aerogels, some challenges such as scalable and cost-effective production, and miniaturization still remain, which hinder the practical applica...Despite recent progress in the synthesis and application of graphene-based aerogels, some challenges such as scalable and cost-effective production, and miniaturization still remain, which hinder the practical application of these materials. Here we report a large-scale electrospinning method to generate graphene-based aerogel microspheres （AMs）, which show broadband, tunable and high-performance microwave absorption. Graphene/Fe3O4 AMs with a large number of openings with hierarchical connecting radial microcharmels can be obtained via electrospinning-freeze drying followed by calcination. Importantly, for a given Fe3O4：graphene mass ratio, altering the shape of aerogel monoliths or powders into aerogel microspheres leads to unique electromagnetic wave properties. As expected, the reflection loss of graphene/Fe3O4 AMs-1：1 with only 5 wt.% absorber loading reaches -51.5 dB at 9.2 GHz with a thickness of 4.0 mm and a broad absorption bandwidth （RL 〈-10 dB） of 6.5 GHz. Furthermore, switching to coaxial electrospinning enables the fabrication of SiO2 coatings to construct graphene/Fe3O4@SiO2 core-shell AMs. The coatings influence the electromagnetic wave absorption of graphene/Fe3O4 AMs significantly. In view of these advantages, we believe that this processing technique may be extended to fabricate a wide range of unique graphene-based architectures for functional design and applications.展开更多
基金The authors greatly appreciate the support from the U.S.Department of Energy’s Office of Energy Efficiency and Renewable Energy(EERE)under the Hydrogen and Fuel Cell Technologies Office Awards DE-EE0008426 and DE-EE0008423National Energy Technology Laboratory under Award DEFE0011585.
文摘Nanostructured catalyst-integrated electrodes with remarkably reduced catalyst loadings,high catalyst utilization and facile fabrication are urgently needed to enable cost-effective,green hydrogen production via proton exchange membrane electrolyzer cells(PEMECs).Herein,benefitting from a thin seeding layer,bottom-up grown ultrathin Pt nanosheets(Pt-NSs)were first deposited on thin Ti substrates for PEMECs via a fast,template-and surfactant-free electrochemical growth process at room temperature,showing highly uniform Pt surface coverage with ultralow loadings and vertically well-aligned nanosheet morphologies.Combined with an anode-only Nafion 117 catalyst-coated membrane(CCM),the Pt-NS electrode with an ultralow loading of 0.015 mgPt cm−2 demonstrates superior cell performance to the commercial CCM(3.0 mgPt cm^(−2)),achieving 99.5%catalyst savings and more than 237-fold higher catalyst utilization.The remarkable performance with high catalyst utilization is mainly due to the vertically well-aligned ultrathin nanosheets with good surface coverage exposing abundant active sites for the electrochemical reaction.Overall,this study not only paves a new way for optimizing the catalyst uniformity and surface coverage with ultralow loadings but also provides new insights into nanostructured electrode design and facile fabrication for highly efficient and low-cost PEMECs and other energy storage/conversion devices.
基金financially supported by the National Natural Science Foundation of China(Nos.21776308 and 21908245)the Science Foundation of China University of Petroleum,Beijing(No.2462018YJRC009)the China Postdoctoral Science Foundation(No.2018T110187)。
文摘Developing microwave absorption(MA)materials with satisfied comprehensive performance is a great challenge for tackling severe electromagnetic pollution.In particular,the magnetic component/carbon hybrids absorbers always suffer from high filler loading.Herein,we propose a feasible strategy to construct hierarchical porous carbon with tightly embedded Ni nanoparticles(Ni@NPC).These highly dispersed Ni nanoparticles produce strong magnetic coupling networks to enhance magnetic loss abilities.Moreover,the interconnected hierarchical dielectric carbon network affords favorable dipolar/interfacial polarization,conduction loss,multiple reflection and scattering.Impressively,with an ultralow filler loading of 5 wt.%,the resultant Ni@NPC/paraffin composite achieves an excellent MA performance with a minimum reflection loss of as high as-72.4 dB and a broad absorption bandwidth of 5.0 GHz.This capability outperforms most current magnetic-dielectric hybrids counterparts.Furthermore,the MA capacity can be easily tuned with adjustments in thickness,content and type of magnetic material.Thus,this work opens up new avenues for the development of high-performance and lightweight MA materials.
基金supported by the National Key R&D Program of China(No.2022YFB4002000)the National Natural Science Foundation of China(No.22232004)+2 种基金the Strategic priority research program of CAS(No.XDA21090400)the Jilin Province Science and Technology Development Program(NOs.20210301008GX and 20210502002ZP)the Jilin Province Development and Reform Commission Program(No.2023C032-6).
文摘Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir doped in tetragonal PdO matrix(IrSAs-PdO)via a lattice-confined strategy.The optimized IrSAs-PdO-0.10 exhibited remarkable OER activity with an overpotential of 277 mV at 10 mA·cm^(-2) and long-term stability of 1000 h in 0.5 M H_(2)SO_(4).Furthermore,the turnover frequency attains 1.6 s^(-1) at an overpotential of 300 mV with a 24-fold increase in the intrinsic activity.The high activity originates from isolated iridium sites with low valence states and decreased Ir–O bonding covalency,and the excellent stability is a result of the effective confinement of iridium sites by Ir–O–Pd motifs.Moreover,we demonstrated for the first time that SACs have great potential in realizing ultralow loading of iridium(as low as microgram per square center meter level)in a practical water electrolyzer.
基金This work was financially supported by the National Natural Science Foundation of China （No. 51573149）, the Science and Technology Planning Project of Sichuan Province （No. 2016GZ0224）, the Fundamental Research Funds for the Central Universities （No. 2682016CX069） and the Student Research Training Program （No. 2017005）.
文摘Despite recent progress in the synthesis and application of graphene-based aerogels, some challenges such as scalable and cost-effective production, and miniaturization still remain, which hinder the practical application of these materials. Here we report a large-scale electrospinning method to generate graphene-based aerogel microspheres （AMs）, which show broadband, tunable and high-performance microwave absorption. Graphene/Fe3O4 AMs with a large number of openings with hierarchical connecting radial microcharmels can be obtained via electrospinning-freeze drying followed by calcination. Importantly, for a given Fe3O4：graphene mass ratio, altering the shape of aerogel monoliths or powders into aerogel microspheres leads to unique electromagnetic wave properties. As expected, the reflection loss of graphene/Fe3O4 AMs-1：1 with only 5 wt.% absorber loading reaches -51.5 dB at 9.2 GHz with a thickness of 4.0 mm and a broad absorption bandwidth （RL 〈-10 dB） of 6.5 GHz. Furthermore, switching to coaxial electrospinning enables the fabrication of SiO2 coatings to construct graphene/Fe3O4@SiO2 core-shell AMs. The coatings influence the electromagnetic wave absorption of graphene/Fe3O4 AMs significantly. In view of these advantages, we believe that this processing technique may be extended to fabricate a wide range of unique graphene-based architectures for functional design and applications.
基金support from the Office of Naval Research(N000141812155)support from the National Science Foundation(DMREF 1437263)supported in part by the National Science Foundation through the UC Irvine Materials Research Science and Engineering Center(DMR-2011967)。
