With the increasing consumption of fossil fuels,proton exchange membrane fuel cells(PEMFCs)have attracted considerable attention as green and sustainable energy conversion devices.The slow kinetics of the cathodic oxy...With the increasing consumption of fossil fuels,proton exchange membrane fuel cells(PEMFCs)have attracted considerable attention as green and sustainable energy conversion devices.The slow kinetics of the cathodic oxygen reduction reaction(ORR)has a major impact on the performance of PEMFCs,and although platinum(Pt)can accelerate the reaction rate of the ORR,the scarcity and high cost of Pt resources still limit the development of PEMFCs.Therefore,the development of low-cost high-performance ORR catalysts is essential for the commercial application and development of PEMFCs.This paper reviews the research progress of researchers on Pt-based ORR catalysts in recent years,including Pt/C catalysts,Pt-based alloy catalysts,Pt-based intermetallic compounds,and Pt-based single-atom catalysts(SACs),with a focus on Pt-based alloy catalysts with different nanostructures.We described in detail the difficulties and solutions in the research process of various ORR catalysts and explained the principle of their activity enhancement with density functional theory(DFT).In addition,an outlook on the development of Pt-based catalysts is given,and reducing the amount of Pt used and improving the performance of catalysts are the directions to work on in the coming period.展开更多
Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)...Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for formic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm^(-2),considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C occurs via a CO_(2)-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)suppresses CO^(*)formation while optimizing dehydrogenation steps and synergistic effect and modified Pt effectively enhance H_(2)O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources.展开更多
The regulation of interface electron-transfer and catalytic kinetics is very important to design the efficient electrocatalyst for alkaline hydrogen oxidation reaction(HOR).Here,we show the Pt-Ni alloy nanoparticles(P...The regulation of interface electron-transfer and catalytic kinetics is very important to design the efficient electrocatalyst for alkaline hydrogen oxidation reaction(HOR).Here,we show the Pt-Ni alloy nanoparticles(PtNi_(2))have an enhanced HOR activity compared with single component Pt catalyst.While,the interface electron-transfer kinetics of PtNi_(2)catalyst exhibits a very wide electron-transfer speed distribution.When combined with carbon dots(CDs),the interface charge transfer of PtNi_(2)-CDs composite is optimized,and then the PtNi_(2)-5 mg CDs exhibits about 2.67 times and 4.04 times higher mass and specific activity in 0.1 M KOH than that of 20%commercial Pt/C.In this system,CDs also contribute to trapping H^(+)and H_(2)O generated during HOR,tuning hydrogen binding energy(HBE),and regulating interface electron transfer.This work provides a deep understanding of the interface catalytic kinetics of Pt-based alloys towards highly efficient HOR catalysts design.展开更多
The melting mechanisms of Pt-based multimetallic nanoparticles(NPs)are important to help determine their optimal melting processes.To understand the melting and coalescence behaviors of heterogeneous NPs(Pd-Pt NPs)wit...The melting mechanisms of Pt-based multimetallic nanoparticles(NPs)are important to help determine their optimal melting processes.To understand the melting and coalescence behaviors of heterogeneous NPs(Pd-Pt NPs)with various sizes and compositions,molecular dynamics(MD)simulation was employed.The MD results for larger Pd-Pt NPs with an effective diameter of4.6-7.8 nm show that PtPd alloy can form at Pd/Pt interface before Pd NP melted completely,while for Pt-core/Pdshell NP and Pd-core/Pt-shell NP,PtPd alloy formed only after Pd portion melted completely.For smaller Pd-Pt NPs with an effective diameter of 2.5-4.0 nm,PdPt alloy is not formed until both Pd and Pt NPs melted completely.Besides,the coalescence process of Pd-Pt NPs depends on the melting temperature of Pt NP when Pt composition is higher than 20 at%.Furthermore,the melting mechanisms of Pd/Pt/Ir trimetallic NPs are investigated.A two-step melting process occurs in Pd-Pt-Ir NPs and Ir-core/Ptshell/Pd-shell NP,and the melting sequence of Pd-core/Ptshell/Ir-shell NP and Pt-core/Pd-shell/Ir-shell NP is different from Pd/Pt bimetallic NPs.展开更多
Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR cataly...Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR catalysts by density functional theory calculations,ranging from single-atom,nanocluster to bulk Pt catalysts.The results showed that the ORR overpotential of these Pt-based catalysts increased when its size enlarged to the nanoparticle scale or reduced to the single-atom scale,and the Pt_(38)cluster had the lowest ORR overpotential(0.46 V)compared with that of Pt_(111)(0.57 V)and single atom Pt(0.7 V).Moreover,we established a volcano curve relationship between the ORR overpotential and binding energy of O*(ΔE_(O*),confirming the intermediate species anchored on Pt38cluster with suitable binding energy located at top of volcano curve.The interaction between intermediate species and Pt-based catalysts were also investigated by the charge distribution and projected density of state and which further confirmed the results of volcano curve.展开更多
To achieve the goals of the peak carbon dioxide emissions and carbon neutral,the development and utilization of sustainable clean energy are extremely important.Hydrogen fuel cells are an important system for converti...To achieve the goals of the peak carbon dioxide emissions and carbon neutral,the development and utilization of sustainable clean energy are extremely important.Hydrogen fuel cells are an important system for converting hydrogen energy into electrical energy.However,the slow hydrogen oxidation reaction(HOR)kinetics under alkaline conditions has limited its development.Therefore,elucidating the catalytic mechanism of HOR in acidic and alkaline media is of great significance for the construction of highly active and stable catalysts.In terms of practicality,Pt is still the primary choice for commercialization of fuel cells.On the above basis,we first introduced the hydrogen binding energy theory and bifunctional theory used to describe the HOR activity,as well as the pH dependence.After that,the rational design strategies of Pt-based HOR catalysts were systematically classified and summarized from the perspective of activity descriptors.In addition,we further emphasized the importance of theoretical simulations and in situ characterization in revealing the HOR mechanism,which is crucial for the rational design of catalysts.Moreover,the practical application of Pt-based HOR catalysts in fuel cells was also presented.In closing,the current challenges and future development directions of HOR catalysts were discussed.This review will provide a deep understanding for exploring the mechanism of highly efficient HOR catalysts and the development of fuel cells.展开更多
Proton exchange membrane fuel cells(PEMFCs)are playing irreplaceable roles in the construction of the future sustainable energy system.However,the insufficient performance of platinum(Pt)-based electrocatalysts for ox...Proton exchange membrane fuel cells(PEMFCs)are playing irreplaceable roles in the construction of the future sustainable energy system.However,the insufficient performance of platinum(Pt)-based electrocatalysts for oxygen reduction reaction(ORR)hinders the overall efficiency of PEMFCs.Engineering the surface strain of catalysts is considered an effective way to tune their electronic structures and therefore optimize catalytic behavior.In this paper,insights into strain engineering for improving Pt-based catalysts toward ORR are elaborated in detail.First,recent advances in understanding the strain effects on ORR catalysts are comprehensively discussed.Then,strain engineering methodologies for adjusting Ptbased catalysts are comprehensively discussed.Finally,further information on the various challenges and potential prospects for strain modulation of Pt-based catalysts is provided.展开更多
The morphology and size of Pt-based bimetallic alloys are known to determine their electrocatalytic performance in reactions relevant to fuel cells.Here,we report a general approach for preparing Pt-M(M=Fe,Co and Ni)b...The morphology and size of Pt-based bimetallic alloys are known to determine their electrocatalytic performance in reactions relevant to fuel cells.Here,we report a general approach for preparing Pt-M(M=Fe,Co and Ni)bimetallic nano-branched structure(NBs)by a simple high temperature solution-phase synthesis.As-prepared Pt-M NBs show a polycrystalline structure and are rich in steps and kinks on the surface,which promote them favorable bifunctional catalytic properties in acidic electrolytes,specifically in terms of the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR).Specially,Pt-Co NBs/C catalyst shows 6.1 and 5.3 times higher in specific activity(SA)and mass activity(MA)for ORR than state-of-the-art commercial Pt/C catalysts,respectively.Moreover,it exhibits a loss of 4.0%in SA and 14.4%in MA after 10,000 cycles of accelerated durability tests(ADTs)compared with the initial activities.In addition,we also confirmed the superior MOR activity of Pt-Co NBs/C catalyst in acidic electrolytes.For Pt-M NBs with other alloying metals,the ORR and MOR activities are both higher than commercial catalysts and are in the sequence of Pt-Co/C>Pt-Fe/C>Pt-Ni/C>commercial Pt/C(or PtRu/C).The improved activities and durability can benefit from the morphological and compositional effects.This synthesis approach may be applied to develop bifunctional catalysts with enhanced ORR and MOR properties for future fuel cells designs.展开更多
Proton exchange membrane fuel cells are playing an increasing role in postpandemic economic recovery and climate action plans.However,their performance,cost,and durability are significantly related to Pt-based electro...Proton exchange membrane fuel cells are playing an increasing role in postpandemic economic recovery and climate action plans.However,their performance,cost,and durability are significantly related to Pt-based electrocatalysts,hampering their large-scale commercial application.Hence,considerable efforts have been devoted to improving the activity and durability of Pt-based electrocatalysts by controlled synthesis in recent years as an effective method for decreasing Pt use,and consequently,the cost.Therefore,this review article focuses on the synthesis processes of carbon-supported Pt-based electrocatalysts,which significantly affect the nanoparticle size,shape,and dispersion on supports and thus the activity and durability of the prepared electrocatalysts.The reviewed processes include(i)the functionalization of a commercial carbon support for enhanced catalyst-support interaction and additional catalytic effects,(ii)the methods for loading Pt-based electrocatalysts onto a carbon support that impact the manufacturing costs of electrocatalysts,(iii)the preparation of spheri-cal and nonspherical Pt-based electrocatalysts(polyhedrons,nanocages,nanoframes,one-and two-dimensional nanostruc-tures),and(iv)the postsynthesis treatments of supported electrocatalysts.The influences of the supports,key experimental parameters,and postsynthesis treatments on Pt-based electrocatalysts are scrutinized in detail.Future research directions are outlined,including(i)the full exploitation of the potential functionalization of commercial carbon supports,(ii)scaled-up one-pot synthesis of carbon-supported Pt-based electrocatalysts,and(iii)simplification of postsynthesis treatments.One-pot synthesis in aqueous instead of organic reaction systems and the minimal use of organic ligands are preferred to simplify the synthesis and postsynthesis treatment processes and to promote the mass production of commercial carbon-supported Pt-based electrocatalysts.展开更多
Pt-based electrocatalysts hold great promise for key electrocatalytic reactions in hydrogen-related energy conversion devices.Generally,the catalytic performance is significantly influenced by metal-support interactio...Pt-based electrocatalysts hold great promise for key electrocatalytic reactions in hydrogen-related energy conversion devices.Generally,the catalytic performance is significantly influenced by metal-support interactions(MSI)in the catalysts,making the tuning of MSI in Pt-based catalysts a highly intriguing research focus.In this review,the catalytic mechanism of Pt-based electrocatalysts is firstly introduced.Subsequently,the effects of MSI on supported Pt electrocatalysts are summarized into four types:geometric effects,electronic effects,synergistic effects,and structural reconfiguration.Finally,the prospect of optimizing the performance of Pt-based electrocatalysts by engineering MSI is exhibited,with the aim of inspiring innovation and advancement of supported Pt catalysts,thereby facilitating the development and utilization of hydrogen energy.展开更多
Proton exchange membrane fuel cells(PEMFCs)represent a promising technology to overcome the current energy and environmental issues,where high-performance cathodic catalysts are badly needed due to the sluggish kineti...Proton exchange membrane fuel cells(PEMFCs)represent a promising technology to overcome the current energy and environmental issues,where high-performance cathodic catalysts are badly needed due to the sluggish kinetics of oxygen reduction reaction(ORR).By far Pt stands for the best ORR catalyst,however,considering the scarcity and high cost,it is imperative to further improve its catalytic activity and atomic efficiency to reduce the loading amount.In view of the key issues,this review concentrates on recent advances on developing high-performance Pt-based nanocatalysts for ORR.The catalytic ORR mechanism was first described,followed by presenting the major principles to regulate ORR activity involving ligand effect and geometric effect.Guided by the principles,typical design strategies of Pt-based nanocatalysts were detailedly summarized,with emphasis on increasing intrinsic activity of single active site and electrochemical active surface area.We finally concluded by providing the remaining challenges and future directions in this field.展开更多
Carbon-supported Pt-based materials are highly promising electrocatalysts.The carbon support plays an important role in the Pt-based catalysts by remarkably influencing the growth,particle size,morphology,dispersion,e...Carbon-supported Pt-based materials are highly promising electrocatalysts.The carbon support plays an important role in the Pt-based catalysts by remarkably influencing the growth,particle size,morphology,dispersion,electronic structure,physiochemical property and function of Pt.This review summarizes recent progress made in the development of carbon-supported Pt-based catalysts,with special emphasis being given to how activity and stability enhancements are related to Pt–C interactions in various carbon supports,including porous carbon,heteroatom doped carbon,carbon-based binary support,and their corresponding electrocatalytic applications.Finally,the current challenges and future prospects in the development of carbon-supported Pt-based catalysts are discussed.展开更多
Pt catalysts are commonly used for chemical reaction processes due to its high catalytic activity and selectivity.Notably,the size of metal particles often has a significant impact on the performance of the metal-load...Pt catalysts are commonly used for chemical reaction processes due to its high catalytic activity and selectivity.Notably,the size of metal particles often has a significant impact on the performance of the metal-loaded catalysts.Therefore,developing highly efficiently synthesis method for the size control of Pt catalysts has great development prospects and research value.In this study,high-throughput size tuning of Pt-based catalysts was achieved by carbonizing the carriers.The experimental and characterization results showed that the size of the loaded Pt nanoparticles varied with different concentrations of glucose solution during carriers carbonization process.The reduction of 4-nitrophenol as a template reaction indicated that the reaction rate constant of the catalyst is approximately linear with the size of Pt particles.Importantly,a laboratory-built high-throughput synthesis system was applied for the catalyst synthesis,which enhances the automation of the laboratory exploratory experiments and makes it possible to synthesize catalysts with controllable size in batches.展开更多
The exploitation of durable and highly active Pt-based electrocatalysts for the oxygen reduction reaction(ORR)is essential for the commercialization of proton exchange membrane fuel cells(PEMFCs).Herein,we designed Pt...The exploitation of durable and highly active Pt-based electrocatalysts for the oxygen reduction reaction(ORR)is essential for the commercialization of proton exchange membrane fuel cells(PEMFCs).Herein,we designed Pt@Pt_(3)Ti core-shell nanoparticles with atomic-controllable shells through precise thermal diffusing Ti into Pt nanoparticles for effective and durable ORR.Combining theoretical and experiment analysis,we found that the lattice strain of Pt_(3)Ti shells can be tailored by precisely controlling the thick-ness of Pt_(3)Ti shell in atomic-scale on account of the lattice constant difference between Pt and Pt_(3)Ti to optimize adsorption properties of Pt_(3)Ti for ORR intermediates,thus enhancing its performance.The Pt@Pt_(3)Ti catalyst with one-atomic Pt_(3)Ti shell(Pt@1L-Pt_(3)Ti/TiO_(2)-C)demonstrates excellent performance with mass activity of 592 mA mgpt-1 and durability nearly 19.5-fold that of commercial Pt/C with negligible decay(2%)after 30,000 potential cycles(0.6-1.0 V vs.RHE).Notably,at higher potential cycles(1.0 V-1.5 V vs.RHE),Pt@1L-Pt_(3)Ti/TiO_(2)-C also showed far superior durability than Pt/C(9.6%decayed while 54.8% for commercial Pt/C).This excellent stability is derived from the intrinsic stability of Pt_(3)Ti alloy and the confinement effect of TiO_(2)-C.The catalyst's enhancement was further confirmed in PEMFC configuration.展开更多
Efficient electrocatalysts for oxygen reduction reaction(ORR)show significant importance for advancing the performance and affordability of proton exchange membrane fuel cells and other energy conversion devices.Herei...Efficient electrocatalysts for oxygen reduction reaction(ORR)show significant importance for advancing the performance and affordability of proton exchange membrane fuel cells and other energy conversion devices.Herein,PtCo_(3)nanoalloys dispersed on a carbon black support,were prepared using ultrafast Joule heating method.By tuning the heating modes,such as high-temperature shock and heating for 2 s,two kinds of PtCo_(3)nanoalloys with varying crystallinities were obtained,referred to as PtCo_(3)-HTS(average size of 5.4 nm)and PtCo_(3)-HT-2 s(average size of 6.4 nm),respectively.Impressively,PtCo_(3)-HTS exhibited superior electrocatalytic ORR activity and stability(E_(1/2)=0.897 V vs.RHE and 36mV negative shift after 50,000 cycles),outperforming PtCo_(3)-HT-2 s(E_(1/2)=0.872 V and 16.2mV negative shift),as well as the commercial Pt/C(20 wt%)catalyst(E_(1/2)=0.847 V and 21.0mV negative shift).The enhanced ORR performance of PtCo_(3)-HTS may be attributed to its low crystallinity,which results in an active local electronic structure and chemical state,as confirmed by X-ray diffraction(XRD)and X-ray absorption fine structure(XAFS)analyses.The ultrafast Joule heating method showed great potential for crystallinity engineering,offering a promising pathway to revolutionize the manufacturing of cost-effective and environmentally friendly catalysts for clean energy applications.展开更多
As an emergent energy carrier,ammonia benefits from a well-established industrial infrastructure for its transportation and production,positioning it as a promising candidate toward a carbon-free energy landscape.With...As an emergent energy carrier,ammonia benefits from a well-established industrial infrastructure for its transportation and production,positioning it as a promising candidate toward a carbon-free energy landscape.Within this context,the electrocatalytic ammonia oxidation reaction(AOR)is pivotal.Platinum(Pt),recognized as the most efficient AOR catalyst,has undergone extensive development over the years,yielding notable advancements across various domains,ranging from elucidating the reaction mechanism to exploring innovative materials.This review begins by elucidating the mechanism of ammonia oxidation,summarizing the evolution of the mechanism and the diverse intermediates identified through various detection methods.Subsequently,it outlines the research progress surrounding different Pt-based catalysts,followed by a discussion on standard protocols for electrochemical ammonia oxidation testing,which facilitates meaningful comparisons across studies and catalyzes the development of more efficient and potent catalysts.Moreover,the review addresses current challenges in ammonia oxidation and outlines potential future directions,providing a comprehensive outlook on the field.展开更多
Two major challenges,high cost and short lifespan,have been hindering the commercialization process of lowtemperature fuel cells.Professor Wei's group has been focusing on decreasing cathode Pt loadings without lo...Two major challenges,high cost and short lifespan,have been hindering the commercialization process of lowtemperature fuel cells.Professor Wei's group has been focusing on decreasing cathode Pt loadings without losses of activity and durability,and their research advances in this area over the past three decades are briefly reviewed herein.Regarding the Pt-based catalysts and the low Pt usage,they have firstly tried to clarify the degradation mechanism of Pt/C catalysts,and then demonstrated that the activity and stability could be improved by three strategies:regulating the nanostructures of the active sites,enhancing the effects of support materials,and optimizing structures of the three-phase boundary.For Pt-free catalysts,especialiy carbon-based ones,several strategies that they proposed to enhance the activity of nitrogen-/heteroatom-doped carbon catalysts are firstly presented.Then,an indepth understanding of the degradation mechanism for carbon-based catalysts is discussed,and followed by the corresponding stability enhancement strategies.Also,the carbon-based electrode at the micrometer-scale,faces the challenges such as low active-site density,thick catalytic layer,and the effect of hydrogen peroxide,which require rational structure design for the integral cathodic electrode.This review finally gives a brief conclusion and outlook about the low cost and long lifespan of cathodic oxygen reduction catalysts.展开更多
Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of nove...Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and Au.The electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and HER.Impressively,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 V.Moreover,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was assembled.Accordingly,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS equipment.The interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.展开更多
Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on Ce...Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation method.The physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron spectroscopy.The results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported Pt.The catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was tested.Compared with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min.展开更多
The development of electrocatalysts for the oxygen reduction reaction(ORR) that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetal...The development of electrocatalysts for the oxygen reduction reaction(ORR) that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetallics composed of platinum and transition metals are considered to be promising candidates for this purpose.However,they typically face challenges such as unfavorable intrinsic activity and a propensity for particle aggregation,diminishing their ORR performance.Against this backdrop,we present our findings on a N-doped carbon confined Pt_(3)Co intermetallic doped with p-block metal tin(Pt_(3)Co_(x)Sn_(1-x)/NC).The introduction of Sn induces lattice strain due to its larger atomic size,which leads to the distortion of the Pt_(3)Co lattice structure,while the coupling of carbon polyhedra inhibits the particle aggregation.The optimized Pt_(3)Co_(0.8)Sn_(0.2)/NC catalyst demonstrates an impressive half-wave potential of 0.86 V versus RHE,surpassing both Pt_(3)Co/NC and Pt_(3)Sn/NC catalysts.Moreover,the Pt_(3)Co_(0.8)Sn_(0.2)/NC exhibits a mass-specific activity as high as 1.4 A mg_(Pt)^(-1),ranking it in the top level among the intermetallicsbased ORR electrocatalysts.When further employed as a cathode material in a self-assembled zinc-air battery,it shows stable operation for over 80 h.These results underscore the significant impact of lattice strain engineering through the strategic doping of p-block metal in the carbon-confined Pt_(3)Co intermetallic,thereby enhancing the catalytic efficiency for the ORR.展开更多
基金supported by CITIC Dameng Mining Industries Limited-Guangxi University Joint Research Institute of Manganese Resources Utilization and Advanced Materials Technology,Guangxi University-CITIC Dameng Mining Industries Limited Joint Base of Postgraduate Cultivation,and State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structuresthe National Natural Science Foundation of China(Nos.11364003 and 52102470)+1 种基金Guangxi Innovation Driven Development Project Grant(Nos.AA17204100 and AA18118052)the Natural Science Foundation of Guangxi Province(No.2018GXNSFAA138186)。
文摘With the increasing consumption of fossil fuels,proton exchange membrane fuel cells(PEMFCs)have attracted considerable attention as green and sustainable energy conversion devices.The slow kinetics of the cathodic oxygen reduction reaction(ORR)has a major impact on the performance of PEMFCs,and although platinum(Pt)can accelerate the reaction rate of the ORR,the scarcity and high cost of Pt resources still limit the development of PEMFCs.Therefore,the development of low-cost high-performance ORR catalysts is essential for the commercial application and development of PEMFCs.This paper reviews the research progress of researchers on Pt-based ORR catalysts in recent years,including Pt/C catalysts,Pt-based alloy catalysts,Pt-based intermetallic compounds,and Pt-based single-atom catalysts(SACs),with a focus on Pt-based alloy catalysts with different nanostructures.We described in detail the difficulties and solutions in the research process of various ORR catalysts and explained the principle of their activity enhancement with density functional theory(DFT).In addition,an outlook on the development of Pt-based catalysts is given,and reducing the amount of Pt used and improving the performance of catalysts are the directions to work on in the coming period.
基金supported by the National Natural Science Foundation of China(21571038,22035004)the Education Department of Guizhou Province(2021312)+2 种基金the Foundation of Guizhou Province(2019-5666)the National Key R&D Program of China(2017YFA0700101)the State Key Laboratory of Physical Chemistry of Solid Surfaces(Xiamen University,202009)。
文摘Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for formic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm^(-2),considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C occurs via a CO_(2)-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)suppresses CO^(*)formation while optimizing dehydrogenation steps and synergistic effect and modified Pt effectively enhance H_(2)O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources.
基金supported by the National Key R&D Program of China(2020YFA0406104,2020YFA0406101)the National MCF Energy R&D Program of China(2018YFE0306105)+5 种基金the Innovative Research Group Project of the National Natural Science Foundation of China(51821002)the National Natural Science Foundation of China(51725204,21771132,51972216,52041202)the Natural Science Foundation of Jiangsu Province(BK20190041)the Key-Area Research and Development Program of Guang Dong Province(2019B010933001)the Collaborative Innovation Center of Suzhou Nano Science&Technologythe 111 Project。
文摘The regulation of interface electron-transfer and catalytic kinetics is very important to design the efficient electrocatalyst for alkaline hydrogen oxidation reaction(HOR).Here,we show the Pt-Ni alloy nanoparticles(PtNi_(2))have an enhanced HOR activity compared with single component Pt catalyst.While,the interface electron-transfer kinetics of PtNi_(2)catalyst exhibits a very wide electron-transfer speed distribution.When combined with carbon dots(CDs),the interface charge transfer of PtNi_(2)-CDs composite is optimized,and then the PtNi_(2)-5 mg CDs exhibits about 2.67 times and 4.04 times higher mass and specific activity in 0.1 M KOH than that of 20%commercial Pt/C.In this system,CDs also contribute to trapping H^(+)and H_(2)O generated during HOR,tuning hydrogen binding energy(HBE),and regulating interface electron transfer.This work provides a deep understanding of the interface catalytic kinetics of Pt-based alloys towards highly efficient HOR catalysts design.
基金funding support from the Agency for Science,Technology and Research(A*STAR,No.SERC A1983c0032)AME Individual Research Grant(IRG)the computing resources from National Supercomputing Centre Singapore。
文摘The melting mechanisms of Pt-based multimetallic nanoparticles(NPs)are important to help determine their optimal melting processes.To understand the melting and coalescence behaviors of heterogeneous NPs(Pd-Pt NPs)with various sizes and compositions,molecular dynamics(MD)simulation was employed.The MD results for larger Pd-Pt NPs with an effective diameter of4.6-7.8 nm show that PtPd alloy can form at Pd/Pt interface before Pd NP melted completely,while for Pt-core/Pdshell NP and Pd-core/Pt-shell NP,PtPd alloy formed only after Pd portion melted completely.For smaller Pd-Pt NPs with an effective diameter of 2.5-4.0 nm,PdPt alloy is not formed until both Pd and Pt NPs melted completely.Besides,the coalescence process of Pd-Pt NPs depends on the melting temperature of Pt NP when Pt composition is higher than 20 at%.Furthermore,the melting mechanisms of Pd/Pt/Ir trimetallic NPs are investigated.A two-step melting process occurs in Pd-Pt-Ir NPs and Ir-core/Ptshell/Pd-shell NP,and the melting sequence of Pd-core/Ptshell/Ir-shell NP and Pt-core/Pd-shell/Ir-shell NP is different from Pd/Pt bimetallic NPs.
基金supported by the National Natural Science Foundation of China(92061125,21978294)Beijing Natural Science Foundation(Z200012)+3 种基金Jiangxi Natural Science Foundation(20212ACB213009)DNL Cooperation Fund,CAS(DNL201921)Self-deployed Projects of Ganjiang Innovation Academy,Chinese Academy of Sciences(E055B003)Hebei Natural Science Foundation(B2020103043)。
文摘Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR catalysts by density functional theory calculations,ranging from single-atom,nanocluster to bulk Pt catalysts.The results showed that the ORR overpotential of these Pt-based catalysts increased when its size enlarged to the nanoparticle scale or reduced to the single-atom scale,and the Pt_(38)cluster had the lowest ORR overpotential(0.46 V)compared with that of Pt_(111)(0.57 V)and single atom Pt(0.7 V).Moreover,we established a volcano curve relationship between the ORR overpotential and binding energy of O*(ΔE_(O*),confirming the intermediate species anchored on Pt38cluster with suitable binding energy located at top of volcano curve.The interaction between intermediate species and Pt-based catalysts were also investigated by the charge distribution and projected density of state and which further confirmed the results of volcano curve.
基金support of this research by the National Natural Science Foundation of China(Nos.22179034 and 22279030)the Natural Science Foundation of Heilongjiang Province(No.ZD2023B002).
文摘To achieve the goals of the peak carbon dioxide emissions and carbon neutral,the development and utilization of sustainable clean energy are extremely important.Hydrogen fuel cells are an important system for converting hydrogen energy into electrical energy.However,the slow hydrogen oxidation reaction(HOR)kinetics under alkaline conditions has limited its development.Therefore,elucidating the catalytic mechanism of HOR in acidic and alkaline media is of great significance for the construction of highly active and stable catalysts.In terms of practicality,Pt is still the primary choice for commercialization of fuel cells.On the above basis,we first introduced the hydrogen binding energy theory and bifunctional theory used to describe the HOR activity,as well as the pH dependence.After that,the rational design strategies of Pt-based HOR catalysts were systematically classified and summarized from the perspective of activity descriptors.In addition,we further emphasized the importance of theoretical simulations and in situ characterization in revealing the HOR mechanism,which is crucial for the rational design of catalysts.Moreover,the practical application of Pt-based HOR catalysts in fuel cells was also presented.In closing,the current challenges and future development directions of HOR catalysts were discussed.This review will provide a deep understanding for exploring the mechanism of highly efficient HOR catalysts and the development of fuel cells.
基金supported by the Natural Science Foundation of Shaanxi Province,China(Nos.2023-JC-YB-122,2024JCYBQN-0072)the High-level Innovation and Entrepreneurship Talent Project from Qinchuangyuan of Shaanxi Province,China(No.QCYRCXM-2022-226)+3 种基金the Fundamental Research Funds for the Central Universities,China(No.D5000210987)the Joint Fund Project-Enterprise-Shaanxi Coal Joint Fund Project,China(No.2021JLM-38)the National Natural Science Foundation of China(Grant No.22379123,No.22250710676)the Fujian Province Minjiang Scholar Program,China.
文摘Proton exchange membrane fuel cells(PEMFCs)are playing irreplaceable roles in the construction of the future sustainable energy system.However,the insufficient performance of platinum(Pt)-based electrocatalysts for oxygen reduction reaction(ORR)hinders the overall efficiency of PEMFCs.Engineering the surface strain of catalysts is considered an effective way to tune their electronic structures and therefore optimize catalytic behavior.In this paper,insights into strain engineering for improving Pt-based catalysts toward ORR are elaborated in detail.First,recent advances in understanding the strain effects on ORR catalysts are comprehensively discussed.Then,strain engineering methodologies for adjusting Ptbased catalysts are comprehensively discussed.Finally,further information on the various challenges and potential prospects for strain modulation of Pt-based catalysts is provided.
基金This work was supported by the National Natural Science Foundation of China(Nos.51571072 and 51871078)Heilongjiang Science Foundation(No.E2018028)the China Scholarship Council,and the NSF MRSEC Program(DMR-14-19807).
文摘The morphology and size of Pt-based bimetallic alloys are known to determine their electrocatalytic performance in reactions relevant to fuel cells.Here,we report a general approach for preparing Pt-M(M=Fe,Co and Ni)bimetallic nano-branched structure(NBs)by a simple high temperature solution-phase synthesis.As-prepared Pt-M NBs show a polycrystalline structure and are rich in steps and kinks on the surface,which promote them favorable bifunctional catalytic properties in acidic electrolytes,specifically in terms of the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR).Specially,Pt-Co NBs/C catalyst shows 6.1 and 5.3 times higher in specific activity(SA)and mass activity(MA)for ORR than state-of-the-art commercial Pt/C catalysts,respectively.Moreover,it exhibits a loss of 4.0%in SA and 14.4%in MA after 10,000 cycles of accelerated durability tests(ADTs)compared with the initial activities.In addition,we also confirmed the superior MOR activity of Pt-Co NBs/C catalyst in acidic electrolytes.For Pt-M NBs with other alloying metals,the ORR and MOR activities are both higher than commercial catalysts and are in the sequence of Pt-Co/C>Pt-Fe/C>Pt-Ni/C>commercial Pt/C(or PtRu/C).The improved activities and durability can benefit from the morphological and compositional effects.This synthesis approach may be applied to develop bifunctional catalysts with enhanced ORR and MOR properties for future fuel cells designs.
基金the Natural Sciences and Engineering Research Council of Canada(NSERC)via CRD Grant No.CRDPJ 522410-17a Discovery Grant from the Canadian Urban Transit Research&Innovation Consortium(CUTRIC)via Project No.160028Ballard Power Systems Inc.via Project No.SRA#077701.
文摘Proton exchange membrane fuel cells are playing an increasing role in postpandemic economic recovery and climate action plans.However,their performance,cost,and durability are significantly related to Pt-based electrocatalysts,hampering their large-scale commercial application.Hence,considerable efforts have been devoted to improving the activity and durability of Pt-based electrocatalysts by controlled synthesis in recent years as an effective method for decreasing Pt use,and consequently,the cost.Therefore,this review article focuses on the synthesis processes of carbon-supported Pt-based electrocatalysts,which significantly affect the nanoparticle size,shape,and dispersion on supports and thus the activity and durability of the prepared electrocatalysts.The reviewed processes include(i)the functionalization of a commercial carbon support for enhanced catalyst-support interaction and additional catalytic effects,(ii)the methods for loading Pt-based electrocatalysts onto a carbon support that impact the manufacturing costs of electrocatalysts,(iii)the preparation of spheri-cal and nonspherical Pt-based electrocatalysts(polyhedrons,nanocages,nanoframes,one-and two-dimensional nanostruc-tures),and(iv)the postsynthesis treatments of supported electrocatalysts.The influences of the supports,key experimental parameters,and postsynthesis treatments on Pt-based electrocatalysts are scrutinized in detail.Future research directions are outlined,including(i)the full exploitation of the potential functionalization of commercial carbon supports,(ii)scaled-up one-pot synthesis of carbon-supported Pt-based electrocatalysts,and(iii)simplification of postsynthesis treatments.One-pot synthesis in aqueous instead of organic reaction systems and the minimal use of organic ligands are preferred to simplify the synthesis and postsynthesis treatment processes and to promote the mass production of commercial carbon-supported Pt-based electrocatalysts.
基金supported by the National Natural Science Foundation of China (22122202,22072051,21972051)the Guangdong Basic and Applied Basic Research Foundation (2021A1515012343)。
文摘Pt-based electrocatalysts hold great promise for key electrocatalytic reactions in hydrogen-related energy conversion devices.Generally,the catalytic performance is significantly influenced by metal-support interactions(MSI)in the catalysts,making the tuning of MSI in Pt-based catalysts a highly intriguing research focus.In this review,the catalytic mechanism of Pt-based electrocatalysts is firstly introduced.Subsequently,the effects of MSI on supported Pt electrocatalysts are summarized into four types:geometric effects,electronic effects,synergistic effects,and structural reconfiguration.Finally,the prospect of optimizing the performance of Pt-based electrocatalysts by engineering MSI is exhibited,with the aim of inspiring innovation and advancement of supported Pt catalysts,thereby facilitating the development and utilization of hydrogen energy.
基金National Key Research and Development Program of China(No.2021YFA1502000)NSFC(No.U2032149 and 22102052)+1 种基金Science and Technology Innovation Program of Hunan Province(No.2021RC3065 and 2021RC2053)Hunan Provincial Natural Science Foundation of China(No.2020JJ2001).
文摘Proton exchange membrane fuel cells(PEMFCs)represent a promising technology to overcome the current energy and environmental issues,where high-performance cathodic catalysts are badly needed due to the sluggish kinetics of oxygen reduction reaction(ORR).By far Pt stands for the best ORR catalyst,however,considering the scarcity and high cost,it is imperative to further improve its catalytic activity and atomic efficiency to reduce the loading amount.In view of the key issues,this review concentrates on recent advances on developing high-performance Pt-based nanocatalysts for ORR.The catalytic ORR mechanism was first described,followed by presenting the major principles to regulate ORR activity involving ligand effect and geometric effect.Guided by the principles,typical design strategies of Pt-based nanocatalysts were detailedly summarized,with emphasis on increasing intrinsic activity of single active site and electrochemical active surface area.We finally concluded by providing the remaining challenges and future directions in this field.
基金National Key Research and Development Program of China(Grant Nos.2022YFB3805600 and 2022YFB3805604)National Natural Science Foundation of China(Grant No.52201286)+5 种基金Sino-German Center COVID19 Related Bilateral Collaborative Project(C-0046),FRFCU(2021qntd13)National 111 Project(B20002)Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2019A1515110436,2021A1515111131,2022A1515011905,and 2022A1515010137)Guangzhou Science and Technology Project(Grant No.202102020463)Guangdong Province International Scientific and Technological Cooperation Projects(Grant No.2020A0505100036)Shenzhen Science and Technology Program(Grant Nos.GJHZ20210705143204014,JCYJ20210324142010029,and KCXFZ20211020170006010).
文摘Carbon-supported Pt-based materials are highly promising electrocatalysts.The carbon support plays an important role in the Pt-based catalysts by remarkably influencing the growth,particle size,morphology,dispersion,electronic structure,physiochemical property and function of Pt.This review summarizes recent progress made in the development of carbon-supported Pt-based catalysts,with special emphasis being given to how activity and stability enhancements are related to Pt–C interactions in various carbon supports,including porous carbon,heteroatom doped carbon,carbon-based binary support,and their corresponding electrocatalytic applications.Finally,the current challenges and future prospects in the development of carbon-supported Pt-based catalysts are discussed.
基金This work was supported by the National Key Research and Development Program of China(grant No.2022YFB3807500)National Natural Science Foundation of China(grant No.22078005)。
文摘Pt catalysts are commonly used for chemical reaction processes due to its high catalytic activity and selectivity.Notably,the size of metal particles often has a significant impact on the performance of the metal-loaded catalysts.Therefore,developing highly efficiently synthesis method for the size control of Pt catalysts has great development prospects and research value.In this study,high-throughput size tuning of Pt-based catalysts was achieved by carbonizing the carriers.The experimental and characterization results showed that the size of the loaded Pt nanoparticles varied with different concentrations of glucose solution during carriers carbonization process.The reduction of 4-nitrophenol as a template reaction indicated that the reaction rate constant of the catalyst is approximately linear with the size of Pt particles.Importantly,a laboratory-built high-throughput synthesis system was applied for the catalyst synthesis,which enhances the automation of the laboratory exploratory experiments and makes it possible to synthesize catalysts with controllable size in batches.
基金supported by the National Natural Science Foundation of China(No.21875039)the Project on the Integration of Industry-Education-Research of Fujian Province(No.2021H6020)the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology).
文摘The exploitation of durable and highly active Pt-based electrocatalysts for the oxygen reduction reaction(ORR)is essential for the commercialization of proton exchange membrane fuel cells(PEMFCs).Herein,we designed Pt@Pt_(3)Ti core-shell nanoparticles with atomic-controllable shells through precise thermal diffusing Ti into Pt nanoparticles for effective and durable ORR.Combining theoretical and experiment analysis,we found that the lattice strain of Pt_(3)Ti shells can be tailored by precisely controlling the thick-ness of Pt_(3)Ti shell in atomic-scale on account of the lattice constant difference between Pt and Pt_(3)Ti to optimize adsorption properties of Pt_(3)Ti for ORR intermediates,thus enhancing its performance.The Pt@Pt_(3)Ti catalyst with one-atomic Pt_(3)Ti shell(Pt@1L-Pt_(3)Ti/TiO_(2)-C)demonstrates excellent performance with mass activity of 592 mA mgpt-1 and durability nearly 19.5-fold that of commercial Pt/C with negligible decay(2%)after 30,000 potential cycles(0.6-1.0 V vs.RHE).Notably,at higher potential cycles(1.0 V-1.5 V vs.RHE),Pt@1L-Pt_(3)Ti/TiO_(2)-C also showed far superior durability than Pt/C(9.6%decayed while 54.8% for commercial Pt/C).This excellent stability is derived from the intrinsic stability of Pt_(3)Ti alloy and the confinement effect of TiO_(2)-C.The catalyst's enhancement was further confirmed in PEMFC configuration.
基金supported by the National Natural Science Foundation of China(No.12205165).
文摘Efficient electrocatalysts for oxygen reduction reaction(ORR)show significant importance for advancing the performance and affordability of proton exchange membrane fuel cells and other energy conversion devices.Herein,PtCo_(3)nanoalloys dispersed on a carbon black support,were prepared using ultrafast Joule heating method.By tuning the heating modes,such as high-temperature shock and heating for 2 s,two kinds of PtCo_(3)nanoalloys with varying crystallinities were obtained,referred to as PtCo_(3)-HTS(average size of 5.4 nm)and PtCo_(3)-HT-2 s(average size of 6.4 nm),respectively.Impressively,PtCo_(3)-HTS exhibited superior electrocatalytic ORR activity and stability(E_(1/2)=0.897 V vs.RHE and 36mV negative shift after 50,000 cycles),outperforming PtCo_(3)-HT-2 s(E_(1/2)=0.872 V and 16.2mV negative shift),as well as the commercial Pt/C(20 wt%)catalyst(E_(1/2)=0.847 V and 21.0mV negative shift).The enhanced ORR performance of PtCo_(3)-HTS may be attributed to its low crystallinity,which results in an active local electronic structure and chemical state,as confirmed by X-ray diffraction(XRD)and X-ray absorption fine structure(XAFS)analyses.The ultrafast Joule heating method showed great potential for crystallinity engineering,offering a promising pathway to revolutionize the manufacturing of cost-effective and environmentally friendly catalysts for clean energy applications.
基金the National Key Research and Development Program of China(No.2022YFB4102000)the National Natural Science Foundation of China(Nos.22102018 and 52171201)+5 种基金the Huzhou Science and Technology Bureau(No.2022GZ45)the China Postdoctoral Science Foundation-Funded Project(No.2022M710601)the Huzhou Science and Technology Bureau(No.2023GZ02)the Natural Science Foundation of Sichuan Province(No.24NSFSC5779)the National Natural Science Foundation of China(Nos.22322201 and 22278067)the Natural Science Foundation of Sichuan Province(No.2023NSFSC0094)。
文摘As an emergent energy carrier,ammonia benefits from a well-established industrial infrastructure for its transportation and production,positioning it as a promising candidate toward a carbon-free energy landscape.Within this context,the electrocatalytic ammonia oxidation reaction(AOR)is pivotal.Platinum(Pt),recognized as the most efficient AOR catalyst,has undergone extensive development over the years,yielding notable advancements across various domains,ranging from elucidating the reaction mechanism to exploring innovative materials.This review begins by elucidating the mechanism of ammonia oxidation,summarizing the evolution of the mechanism and the diverse intermediates identified through various detection methods.Subsequently,it outlines the research progress surrounding different Pt-based catalysts,followed by a discussion on standard protocols for electrochemical ammonia oxidation testing,which facilitates meaningful comparisons across studies and catalyzes the development of more efficient and potent catalysts.Moreover,the review addresses current challenges in ammonia oxidation and outlines potential future directions,providing a comprehensive outlook on the field.
基金supported by the National Key Research and Development Program of China(No.2020YFB1506002,2019YFB1504503,2016YFB0101202)National 973 Program of China(No.2012CB215501)National Natural Science Foundation of China(No.52021004,22022502(2021),21822803(2019),21576031(2016),51272297(2013),20936008(2010),20676156(2007),20376088(2004),20176066(2002),29976047(2000)).
文摘Two major challenges,high cost and short lifespan,have been hindering the commercialization process of lowtemperature fuel cells.Professor Wei's group has been focusing on decreasing cathode Pt loadings without losses of activity and durability,and their research advances in this area over the past three decades are briefly reviewed herein.Regarding the Pt-based catalysts and the low Pt usage,they have firstly tried to clarify the degradation mechanism of Pt/C catalysts,and then demonstrated that the activity and stability could be improved by three strategies:regulating the nanostructures of the active sites,enhancing the effects of support materials,and optimizing structures of the three-phase boundary.For Pt-free catalysts,especialiy carbon-based ones,several strategies that they proposed to enhance the activity of nitrogen-/heteroatom-doped carbon catalysts are firstly presented.Then,an indepth understanding of the degradation mechanism for carbon-based catalysts is discussed,and followed by the corresponding stability enhancement strategies.Also,the carbon-based electrode at the micrometer-scale,faces the challenges such as low active-site density,thick catalytic layer,and the effect of hydrogen peroxide,which require rational structure design for the integral cathodic electrode.This review finally gives a brief conclusion and outlook about the low cost and long lifespan of cathodic oxygen reduction catalysts.
基金supported by the Key projects of intergovernmental international cooperation in the Key R&D programs of the Ministry of Science and Technology of China(No.2021YFE0115800)the National Science Funding Committee of China(No.U20A20250)。
文摘Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient strategy.Herein,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and Au.The electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and HER.Impressively,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 V.Moreover,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was assembled.Accordingly,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS equipment.The interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.
基金supported by the Key Research and Design Program of Qinhuangdao(202101A005)the Science and Technology Project of Hebei Education Department(QN2023094)+2 种基金the Cultivation Project for Basic Research and Innovation of Yanshan University(2021LGQN028)the Project for Research and Development of Metal Catalysts for Photo-thermal Decomposition of Waste Plastics to Prepare Value-added Chemicals(x2023322)the Subsidy for Hebei Key Laboratory of Applied Chemistry after Operation Performance(22567616H).
文摘Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation method.The physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron spectroscopy.The results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported Pt.The catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was tested.Compared with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min.
基金Natural Science Foundation of Jiangsu Province (BK20210735)National Natural Science Foundation of China (52201269, 52302296)+4 种基金Collaborative Innovation Center of Suzhou Nano Science and Technologythe 111 Projectthe Suzhou Key Laboratory of Functional Nano and Soft MaterialsJiangsu Key Laboratory for Carbon-Based Functional Materials & Devicesthe funding from the Gusu leading talent plan for scientific and technological innovation and entrepreneurship (ZXL2022487)。
文摘The development of electrocatalysts for the oxygen reduction reaction(ORR) that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetallics composed of platinum and transition metals are considered to be promising candidates for this purpose.However,they typically face challenges such as unfavorable intrinsic activity and a propensity for particle aggregation,diminishing their ORR performance.Against this backdrop,we present our findings on a N-doped carbon confined Pt_(3)Co intermetallic doped with p-block metal tin(Pt_(3)Co_(x)Sn_(1-x)/NC).The introduction of Sn induces lattice strain due to its larger atomic size,which leads to the distortion of the Pt_(3)Co lattice structure,while the coupling of carbon polyhedra inhibits the particle aggregation.The optimized Pt_(3)Co_(0.8)Sn_(0.2)/NC catalyst demonstrates an impressive half-wave potential of 0.86 V versus RHE,surpassing both Pt_(3)Co/NC and Pt_(3)Sn/NC catalysts.Moreover,the Pt_(3)Co_(0.8)Sn_(0.2)/NC exhibits a mass-specific activity as high as 1.4 A mg_(Pt)^(-1),ranking it in the top level among the intermetallicsbased ORR electrocatalysts.When further employed as a cathode material in a self-assembled zinc-air battery,it shows stable operation for over 80 h.These results underscore the significant impact of lattice strain engineering through the strategic doping of p-block metal in the carbon-confined Pt_(3)Co intermetallic,thereby enhancing the catalytic efficiency for the ORR.
