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1.
ACS Nano ; 18(14): 10008-10018, 2024 Apr 09.
Artigo em Inglês | MEDLINE | ID: mdl-38551183

RESUMO

Two-dimensional (2D) heterojunction nanomaterials offer exceptional physicochemical and catalytic properties, thanks to their special spatial electronic structure. However, synthesizing morphologically uniform 2D platinum (Pt)-based metallic nanomaterials with diverse crystalline phases remains a formidable challenge. In this study, we have achieved the successful synthesis of advanced 2D platinum-tellurium heterojunction nanosheet assemblies (Ptx-PtTe2 HJNSAs, x = 0, 1, 2), seamlessly integrating both trigonal PtTe2 (t-PtTe2) and cubic Pt (c-Pt) phases. By enabling efficient electron transport and leveraging the specific electron density present at the heterojunction, the Pt2-PtTe2 HJNSAs/C demonstrated exceptional formic acid oxidation reaction (FAOR) activity and stability. Specifically, the specific and mass activities reached 8.4 mA cm-2 and 6.1 A mgPt-1, which are 46.7 and 50.8 times higher than those of commercial Pt/C, respectively. Impressively, aberration-corrected high-angle annular dark field scanning transmission electron microscopy (AC-HAADF-STEM) revealed a closely packed arrangement of atomic layers and a coherent intergrowth heterogeneous structure. Density functional theory (DFT) calculations further indicated that rearrangement of electronic structure occurred on the surface of Pt2-PtTe2 HJNSAs resulting in a more favorable dehydrogenation pathway and excellent CO tolerance, beneficial for performance improvement. This work inspires the targeted exploration of Pt-based nanomaterials through 2D heterostructure design, leading to an important impact on fuel cell catalysis and beyond.

2.
Nat Commun ; 15(1): 1097, 2024 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-38321034

RESUMO

Bimetallic PtRu are promising electrocatalysts for hydrogen oxidation reaction in anion exchange membrane fuel cell, where the activity and stability are still unsatisfying. Here, PtRu nanowires were implanted with a series of oxophilic metal atoms (named as i-M-PR), significantly enhancing alkaline hydrogen oxidation reaction (HOR) activity and stability. With the dual doping of In and Zn atoms, the i-ZnIn-PR/C shows mass activity of 10.2 A mgPt+Ru-1 at 50 mV, largely surpassing that of commercial Pt/C (0.27 A mgPt-1) and PtRu/C (1.24 A mgPt+Ru-1). More importantly, the peak power density and specific power density are as high as 1.84 W cm-2 and 18.4 W mgPt+Ru-1 with a low loading (0.1 mg cm-2) anion exchange membrane fuel cell. Advanced experimental characterizations and theoretical calculations collectively suggest that dual doping with In and Zn atoms optimizes the binding strengths of intermediates and promotes CO oxidation, enhancing the HOR performances. This work deepens the understanding of developing novel alloy catalysts, which will attract immediate interest in materials, chemistry, energy and beyond.

3.
Small ; 20(22): e2310036, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38126916

RESUMO

Strain effect in the structurally defective materials can contribute to the catalysis optimization. However, it is challenging to achieve the performance improvement by strain modulation with the help of geometrical structure because strain is spatially dependent. Here, a new class of compressively strained platinum-iridium-metal zigzag-like nanowires (PtIrM ZNWs, M = nickel (Ni), cobalt (Co), iron (Fe), zinc (Zn) and gallium (Ga)) is reported as the efficient alkaline hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR) catalysts. Particularly, the optimized PtIrNi ZNWs with 3% compressive strain (cs-PtIrNi ZNWs) can achieve the highest HER/HOR performances among all the catalysts investigate. Their HOR mass and specific activities are 3.2/14.4 and 2.6/32.7 times larger than those of PtIrNi NWs and commercial Pt/C, respectively. Simultaneously, they can exhibit the superior stability and high CO resistance for HOR. Further, experimental and theoretical studies collectively reveal that the compressive strain in cs-PtIrNi ZNWs effectively weakens the adsorption of hydroxyl intermediate and modulates the electronic structure, resulting in the weakened hydrogen binding energy (HBE) and moderate hydroxide binding energy (OHBE), beneficial for the improvement of HOR performance. This work highlights the importance of strain tuning in enhancing Pt-based nanomaterials for hydrogen catalysis and beyond.

4.
ACS Nano ; 17(18): 17779-17789, 2023 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-37708057

RESUMO

The development of high-performance platinum (Pt)-based electrocatalysts for the hydrogen oxidation reaction (HOR) is highly desirable for hydrogen fuel cells, but it is limited by the sluggish kinetics and severe carbon monoxide (CO) poisoning in alkaline medium. Herein, we explore a class of facet-selected Pt-nickel-indium fishbone-like nanowires (PtNiIn FNWs) featuring high-index facets (HIFs) of Pt3In skin as efficient alkaline HOR catalysts. Impressively, the optimized Pt66Ni6In28 FNWs show the highest mass and specific activities of 4.02 A mgPt-1 and 6.56 mA cm-2, 2.0/2.1 and 13.9/15.6 times larger than those of commercial PtRu/C and commercial Pt/C, respectively, along with a competitive CO-tolerance ability. Specifically, they exhibit only 6.0% current density decay after 10000 s of operation and 25.7% activity loss after 2000 s in the presence of 1000 ppm of CO. Moreover, an isotope experiment and density functional theory (DFT) calculations further prove that the unique structure and synergy among Pt, Ni, and In endow these Pt66Ni6In28 FNWs with an optimized hydrogen binding energy (HBE) and an advantageous hydroxide binding energy (OHBE), giving them excellent alkaline HOR properties. The combined construction of surface-skin and HIFs in PtNiIn FNWs will offer an available method to realize the potential applications of advanced non-PtRu-based catalysts in fuel cells and beyond.

5.
J Am Chem Soc ; 145(35): 19274-19282, 2023 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-37585588

RESUMO

To promote the commercialization of direct formic acid fuel cell (DFAFC), it is vital to explore new types of direct formic acid oxidation (FAOR) catalysts with high activity and direct pathway. Here, we report the synthesis of intermetallic platinum-lead/platinum nanoplates inlaid with sub-monolayer antimony oxide surface (PtPb/Pt@sub-SbOx NPs) for efficient catalytic applications in FAOR. Impressively, they can achieve the remarkable FAOR specific and mass activities of 28.7 mA cm-2 and 7.2 A mgPt-1, which are 151 and 60 times higher than those of the state-of-the-art commercial Pt/C, respectively. Furthermore, the X-ray photoelectron spectroscopy and X-ray absorption spectroscopy results collectively reveal the optimization of the local coordination environment by the surface sub-monolayer SbOx, along with the electron transfer from Pb and Sb to Pt, driving the predominant dehydrogenation process. The sub-monolayer SbOx on the surface can effectively attenuate the CO generation, largely improving the FAOR performance of PtPb/Pt@sub-SbOx NPs. This work develops a class of high-performance Pt-based anodic catalyst for DFAFC via constructing the unique intermetallic core/sub-monolayer shell structure.

6.
J Am Chem Soc ; 145(28): 15393-15404, 2023 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-37429024

RESUMO

Designing efficient formic acid oxidation reaction (FAOR) catalysts with remarkable membrane electrode assembly (MEA) performance in a direct formic acid fuel cell (DFAFC) medium is significant yet challenging. Herein, we report that the monoclinic-phased platinum-tellurium nanotrepang (m-PtTe NT) can be adopted as a highly active, selective, and stable FAOR catalyst with a desirable direct reaction pathway. The m-PtTe NT exhibits the high specific and mass activities of 6.78 mA cm-2 and 3.2 A mgPt-1, respectively, which are 35.7/22.9, 2.8/2.6, and 3.9/2.9 times higher than those of commercial Pt/C, rhombohedral-phased Pt2Te3 NT (r-Pt2Te3 NT), and trigonal-phased PtTe2 NT (t-PtTe2 NT), respectively. Simultaneously, the highest reaction tendency for the direct FAOR pathway and the best tolerance to poisonous CO intermediate can also be realized by m-PtTe NT. More importantly, even in a single-cell medium, the m-PtTe NT can display a much higher MEA power density (171.4 mW cm-2) and stability (53.2% voltage loss after 5660 s) than those of commercial Pt/C, demonstrating the great potential in operating DFAFC device. The in-situ Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy jointly demonstrate that the unique nanostructure of m-PtTe NT can effectively optimize dehydrogenation steps and inhibit the CO intermediate adsorption, as well as promote the oxidation of noxious CO intermediate, thus achieving the great improvement of FAOR activity, poisoning tolerance, and stability. Density functional theory calculations further reveal that the direct pathway is the most favorable on m-PtTe NT than r-Pt2Te3 NT and t-PtTe2 NT. The higher activation energy to produce CO and the relatively weaker binding with CO of m-PtTe NT result in the better CO tolerance. This work achieves remarkable FAOR and MEA performances of advanced Pt-based anodic catalysts for DFAFCs via a phase engineering strategy.

7.
J Am Chem Soc ; 145(28): 15109-15117, 2023 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-37289521

RESUMO

Designing platinum (Pt)-based formic acid oxidation reaction (FAOR) catalysts with high performance and high selectivity of direct dehydrogenation pathway for direct formic acid fuel cell (DFAFC) is desirable yet challenging. Herein, we report a new class of surface-uneven PtPbBi/PtBi core/shell nanoplates (PtPbBi/PtBi NPs) as the highly active and selective FAOR catalysts, even in the complicated membrane electrode assembly (MEA) medium. They can achieve unprecedented specific and mass activities of 25.1 mA cm-2 and 7.4 A mgPt-1 for FAOR, 156 and 62 times higher than those of commercial Pt/C, respectively, which is the highest for a FAOR catalyst by far. Simultaneously, they show highly weak adsorption of CO and high dehydrogenation pathway selectivity in the FAOR test. More importantly, the PtPbBi/PtBi NPs can reach the power density of 161.5 mW cm-2, along with a stable discharge performance (45.8% decay of power density at 0.4 V for 10 h), demonstrating great potential in a single DFAFC device. The in situ Fourier transform infrared spectroscopy (FTIR) and X-ray absorption spectroscopy (XAS) results collectively reveal a local electron interaction between PtPbBi and PtBi. In addition, the high-tolerance PtBi shell can effectively inhibit the production/adsorption of CO, resulting in the complete presence of the dehydrogenation pathway for FAOR. This work demonstrates an efficient Pt-based FAOR catalyst with 100% direct reaction selectivity, which is of great significance for driving the commercialization of DFAFC.

8.
Small ; 19(38): e2208202, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37222629

RESUMO

Pursuing highly active and long-term stable ruthenium (Ru) based oxygen evolution reaction (OER) catalyst for water electrolysis under acidic conditions is of great significance yet a tremendous challenge to date. To solve the problem of serious Ru corrosion in an acid medium, the trace lattice sulfur (S) inserted RuO2 catalyst is prepared. The optimized catalyst (Ru/S NSs-400) has shown a record stability of 600 h for the solely containing Ru (iridium-free) nanomaterials. In the practical proton exchange membrane device, the Ru/S NSs-400 can even sustain more than 300 h without obvious decay at the high current density of 250 mA cm-2 . The detailed investigations reveal that S doping not only changes the electronic structure of Ru via forming RuS coordination for high adsorption of reaction intermediates but also stabilizes Ru from over-oxidation. This strategy is also effective for improving the stability of commercial Ru/C and homemade Ru-based nanoparticles. This work offers a highly effective strategy to design high-performance OER catalysts for water splitting and beyond.

9.
ACS Nano ; 17(6): 5861-5870, 2023 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-36920478

RESUMO

Thickness regulation of transition metal hydroxides/oxides nanosheets with superior catalytic properties represents a promising strategy to enhance catalytic performance, but it remains an enormous challenge to achieve precise control, especially when it comes to the ultrathin limit (several atomic layers). In this work, a facile strategy of alkylamine-confined growth is proposed for the synthesis of thickness-tunable metal hydroxide/oxide nanosheets. Specifically, ultrathin cobalt hydroxide and cobaltous oxide hybrid (Co(OH)2-CoO) nanosheets (Co-O NSs) with a thickness in the range of 2-6 nm (5-13 atomic layers) are synthesized by using alkylamines with different carbon chain lengths as the ligand to modulate vertical coordination ability. Co-O NSs with a thickness of 2 nm (Co-O NSs-2 nm) exhibit excellent oxygen evolution reaction (OER) performance with an overpotential of 278 mV at 10 mA/cm2. The maximized number of active sites including oxygen vacancies, optimal adsorption strength, and the highest electrical conductivity are considered as the potential factors contributing to the excellent OER performance of Co-O NSs-2 nm. This work holds great significance for the precise thickness-tunable synthesis of transition metal layered hydroxide nanosheets with modulated and improved catalytic performance.

10.
Adv Mater ; 35(11): e2208672, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36574979

RESUMO

Developing high-performance catalysts for fuel cell catalysis is the most critical and challenging step for the commercialization of fuel cell technology. Here 1D trimetallic platinum-iron-cobalt nanosaws (Pt3 FeCo NSs) with low-coordination features are designed as efficient bifunctional electrocatalysts for practical fuel cell catalysis. The oxygen reduction reaction (ORR) activity of Pt3 FeCo NSs (10.62 mA cm-2 and 4.66 A mg-1 Pt at 0.90 V) is more than 25-folds higher than that of the commercial Pt/C, even after 30 000 voltage cycles. Density functional theory calculations reveal that the strong inter-d-orbital electron transfer minimizes the ORR barrier with higher selectivity at robust valence states. The volcano correlation between the intrinsic structure featured with low-coordination Pt-sites and corresponding electronic activities is discovered, which guarantees high ORR activities. The Pt3 FeCo NSs located in the membrane electrode assembly (MEA) also achieve very high peak power density (1800.6 mW cm-2 ) and competitive specific/mass activities (1.79 mA cm-2 and 0.79 A mg-1 Pt at 0.90 ViR-free cell voltage) as well as a long-term lifetime in specific H2 O2 medium for proton-exchange-membrane fuel cells, ranking top electrocatalysts reported to date for MEA. This work represents a class of multimetallic Pt-based nanocatalysts for practical fuel cells and beyond.

11.
Angew Chem Int Ed Engl ; 62(3): e202213783, 2023 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-36400747

RESUMO

High-entropy alloys (HEAs) have been attracting extensive research interests in designing advanced nanomaterials, while their precise control is still in the infancy stage. Herein, we have reported a well-defined PtBiPbNiCo hexagonal nanoplates (HEA HPs) as high-performance electrocatalysts. Structure analysis decodes that the HEA HP is constructed with PtBiPb medium-entropy core and PtBiNiCo high-entropy shell. Significantly, the HEA HPs can reach the specific and mass activities of 27.2 mA cm-2 and 7.1 A mgPt -1 for formic acid oxidation reaction (FAOR), being the record catalyst ever achieved in Pt-based catalysts, and can realize the membrane electrode assembly (MEA) power density (321.2 mW cm-2 ) in fuel cell. Further experimental and theoretical analyses collectively evidence that the hexagonal intermetallic core/atomic layer shell structure and multi-element synergy greatly promote the direct dehydrogenation pathway of formic acid molecule and suppress the formation of CO*.

13.
Nat Commun ; 12(1): 6261, 2021 Oct 29.
Artigo em Inglês | MEDLINE | ID: mdl-34716289

RESUMO

High-entropy alloys (HEAs) with unique physicochemical properties have attracted tremendous attention in many fields, yet the precise control on dimension and morphology at atomic level remains formidable challenges. Herein, we synthesize unique PtRuNiCoFeMo HEA subnanometer nanowires (SNWs) for alkaline hydrogen oxidation reaction (HOR). The mass and specific activities of HEA SNWs/C reach 6.75 A mgPt+Ru-1 and 8.96 mA cm-2, respectively, which are 2.8/2.6, 4.1/2.4, and 19.8/18.7 times higher than those of HEA NPs/C, commercial PtRu/C and Pt/C, respectively. It can even display enhanced resistance to CO poisoning during HOR in the presence of 1000 ppm CO. Density functional theory calculations reveal that the strong interactions between different metal sites in HEA SNWs can greatly regulate the binding strength of proton and hydroxyl, and therefore enhances the HOR activity. This work not only provides a viable synthetic route for the fabrication of Pt-based HEA subnano/nano materials, but also promotes the fundamental researches on catalysis and beyond.

14.
Adv Mater ; 33(51): e2105308, 2021 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-34610648

RESUMO

To improve the electroactivity and stability of electrocatalysts, various modulation strategies have been applied in nanocatalysts. Among different methods, heteroatom doping has been considered as an effective method, which modifies the local bonding environments and the electronic structures. Meanwhile, the design of novel two-dimensional (2D) nanostructures also offers new opportunities for achieving efficient electrocatalysts. In this work, Mn-doped ultrathin Ru nanosheet branches (RuMn NSBs), a newly reported 2D nanostructure, is synthesized. With the ultrathin and naturally abundant edges, the RuMn NSBs have exhibited bifunctionalities of hydrogen evolution reaction and oxygen evolution reaction with high electroactivity and durability in different electrolytes. Experimental characterizations have revealed that RuO bonds are shortened due to Mn doping, which is the key factor that leads to improved electrochemical performances. Density functional theory (DFT) calculations have confirmed that the introduction of Mn enables flexible modulations on the valence states of Ru sites. The inversed redox state evolutions of Ru and Mn sites not only improve the electroactivity for the water splitting but also the long-term stability due to the pinning effect of Ru sites. This work has provided important inspirations for the design of future advanced Ru-based electrocatalysts with high performances and durability.

15.
Nano Lett ; 21(15): 6625-6632, 2021 Aug 11.
Artigo em Inglês | MEDLINE | ID: mdl-34319751

RESUMO

Developing a large-scale method to produce platinum (Pt)-based electrocatalysts for the oxygen reduction reaction (ORR) is highly desirable to propel the commercialization of the membrane electrode assembly (MEA). Here, we successfully report the large-scale production of surfactant-free ruthenium-doped Pt-cobalt octahedra grown on carbon (Ru-Pt3Co/C), which display a much higher ORR activity and stability and MEA stability than Pt3Co/C and Pt/C. Significantly, the in-situ X-ray absorption fine structure result reveals that Ru can drive the reduced Pt atoms to reverse to their initial state after the ORR by transferring a redundant electron from Pt to Ru, preventing the over-reduction of Pt active sites and boosting the chemical stability. Theory investigations further confirm that the doped Ru can accelerate the breach and desorption of oxygen intermediates, making it active and durable for the ORR. The present work sheds light on the exploration of a large-scale strategy for producing advanced Pt-based nanocatalysts, which may offer significant advantages for practical fuel cell applications in the future.

16.
Nano Lett ; 21(12): 5075-5082, 2021 Jun 23.
Artigo em Inglês | MEDLINE | ID: mdl-34061555

RESUMO

Platinum (Pt) catalysts play a key role in energy conversion and storage processes, but the realization of further performance enhancement remains challenging. Herein, we report a new class of Pt superstructures (SSs) with surface distortion engineering by electrochemical leaching of PtTex SSs that can largely boost the oxygen reduction reaction (ORR), the methanol oxidation reaction (MOR), and the hydrogen evolution reaction (HER). In particular, the high-distortion (H)-Pt SSs achieve a mass activity of 2.24 A mg-1 at 0.90 VRHE for the ORR and 2.89 A mg-1 for the MOR as well as a low overpotential of 25.3 mV at 10 mA cm-2 for the HER. Moreover, the distorted surface features of Pt SSs can be preserved by mitigating the detrimental effects of agglomeration/degradation during long-time electrocatalysis. A multiscale modeling demonstrates that surface compressions, defects, and nanopores act in synergy for the enhanced ORR performance. This work highlights the advances of stable superstructure and distortion engineering for realizing high-performance Pt nanostructures.

17.
Small ; 17(14): e2007302, 2021 04.
Artigo em Inglês | MEDLINE | ID: mdl-33719172

RESUMO

To explore nanocatalysts with high electro-catalytic performance and less loading of precious metals, efforts have been made to develop electrochemical methods with high spatial resolution at the single nanoparticle level. Herein, a highly sensitive single-nanoparticle coulometry method is successfully developed to study the electrochemical activity and oscillation of single PtTe nanocatalysts. Based on microbattery reactions involving the formic acid electro-oxidation and the deposition of Ag on the single PtTe nanocatalyst surface, this method enables the transition from the undetectable sub-fA electric signal of the formic acid electro-oxidation into strong localized surface plasmon resonance scattering signal of Ag detected by dark-field microscopy. The lowest limiting current for a single nanocatalyst is found to be as low as 25.8 aA. Different trends of activity versus the formic acid concentration and types of activity of the single nanocatalyst have been discovered. Unveiled frequency-amplitude graph shows that the two electrochemical oscillation modes of low frequency with high amplitude and vice versa coexist in a single PtTe nanocatalyst, indicating the abundantly smooth surfaces and defects of nanocatalysts. This conducted study will open up the new avenue for further behavioral and mechanistic investigation of more types of nanocatalysts in the electrochemistry community.


Assuntos
Nanopartículas Metálicas , Catálise , Técnicas Eletroquímicas , Eletroquímica , Oxirredução
18.
Sci Bull (Beijing) ; 64(1): 36-43, 2019 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-36659520

RESUMO

The water-gas shift (WGS) reaction is an essential industrial reaction for upgrading hydrogen (H2) by removing carbon monoxide (CO), while highly efficient platinum (Pt)-based catalysts for WGS with simultaneously high activity and stability are still yet to be developed due to the poisoning issue during the reaction. Herein, we report on the porous PtPb peanut nanocrystals (porous PtPb PNCs) and porous PtPb octahedron nanocrystals (porous PtPb ONCs) with controllable ratios of Pt/Pb as extremely active and stable catalysts towards WGS reaction. It exhibits the composition-dependent activity with porous PtPb PNCs-40/ZnO being the most active for WGS to H2, 16.9 times higher than that of the commercial Pt/C. The porous PtPb PNCs-40/ZnO also display outstanding durability with barely activity decay and negligible structure and composition changes after ten successive reaction cycles. X-ray photoelectron spectroscopy (XPS) results reveal that the suitable binding energy of Pt 4f7/2 and the high ratio of Pt(0) to Pt(II) in porous PtPb PNCs/ZnO and porous PtPb ONCs/ZnO are crucial for the enhanced WGS activity. The CO stripping results indicate the optimized CO adsorption strength on the Pt surface ensure the excellent WGS activity and the outstanding durability. The present work demonstrates an important advance in tuning the porous metal nanomaterials as highly efficient and durable catalysts for catalysis, energy conversion and beyond.

19.
J Am Chem Soc ; 140(27): 8384-8387, 2018 07 11.
Artigo em Inglês | MEDLINE | ID: mdl-29924607

RESUMO

The selective hydrogenation of α, ß-unsaturated aldehyde is an extremely important transformation, while developing efficient catalysts with desirable selectivity to highly value-added products is challenging, mainly due to the coexistence of two conjugated unsaturated functional groups. Herein, we report that a series of Pt-based zigzag nanowires (ZNWs) can be adopted as selectivity controllers for α, ß-unsaturated aldehyde hydrogenation, where the excellent unsaturated alcohol (UOL) selectivity (>95%) and high saturated aldehyde (SA) selectivity (>94%) are achieved on PtFe ZNWs and PtFeNi ZNWs+AlCl3, respectively. The excellent UOL selectivity of PtFe ZNWs is attributed to the lower electron density of the surface Pt atoms, while the high SA selectivity of PtFeNi ZNWs+AlCl3 is due to synergy between PtFeNi ZNWs and AlCl3, highlighting the importance of Pt-based NWs with precisely controlled surface and composition for catalysis and beyond.

20.
J Am Chem Soc ; 139(28): 9576-9582, 2017 07 19.
Artigo em Inglês | MEDLINE | ID: mdl-28657302

RESUMO

Although explosive studies on pursuing high-performance Pt-based nanomaterials for fuel cell reactions have been carried out, the combined controls of surface composition, exposed facet, and interior structure of the catalyst remains a formidable challenge. We demonstrate herein a facile chemical approach to realize a new class of intermetallic Pt-Pb-Ni octahedra for the first time. Those nanostructures with unique intermetallic core, active surface composition, and the exposed facet enhance oxygen reduction electrocatalysis with the optimized PtPb1.12Ni0.14 octahedra exhibiting superior specific and mass activities (5.16 mA/cm2 and 1.92 A/mgPt) for oxygen reduction reaction (ORR) that are ∼20 and ∼11 times higher than the commercial Pt/C, respectively. Moreover, the PtPb1.12Ni0.14 octahedra can endure at least 15 000 cycles with negligible activity decay, showing a new class of Pt-based electrocatalysts with enhanced performance for fuel cells and beyond.

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