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
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
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 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
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
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 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
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
Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction(HER).Here,we reported PtNi nanoparti...Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction(HER).Here,we reported PtNi nanoparticles with a refined size of 2.71 nm and regular strains loaded on carbon black,synthesized using the high-temperature liquid shock(HTLS)method.This approach offers significant advantages over conventional synthesis methods,including high scalability,rapid reaction rates,and precise control over the size and shape of nanocrystals.Importantly,the synthesized PtNi electrocatalysts demonstrate outstanding catalytic activity and long-term stability for HER,achieving low overpotentials of 19 and 203 mV at current densities of 10 and 1000 mA/cm^(2),respectively.The superior performance can be attributed to the combination of a refined particle size,lattice strains,and synergistic effects between Pt and Ni.This rapid liquid-state synthesis demonstrated here holds great potential for scalable and industrial manufacturing of micro-/nano-catalysts.展开更多
This study proposes a green electrochemical strategy for addressing the high-energy-barrier oxygen evolution reaction(OER)in traditional overall water splitting.Leveraging the thermodynamic advantages of N–H bond act...This study proposes a green electrochemical strategy for addressing the high-energy-barrier oxygen evolution reaction(OER)in traditional overall water splitting.Leveraging the thermodynamic advantages of N–H bond activation/cleavage and N–N coupling processes,the 3,5-diamino-1,2,4-triazole(DAT)oxidative coupling reaction(DATOR)has been introduced to replace the high-energy-barrier oxygen evolution reaction(OER).This substitution enables low-energy-consumption hydrogen production while simultaneously yielding high-value azo energetic materials.Furthermore,to enhance electron and atom economy,the anodic DATOR process allows the hydrogen radicals(H^(*))generated from amine dehydrogenation to chemically combine via the Tafel process,producing hydrogen gas.By constructing coupling system with Pts,n@NiS_(2)@CC cathode and Cu O/CF anode,the operating voltage of the system was significantly reduced(0.96 V@10 m A cm^(-2)),which was 680 mV more energy efficient than conventional water electrolysis(1.64 V).In situ spectroscopy and theoretical calculations indicate that the anode DATOR generates DAAT through the N–H bond cleavage and N–N coupling path mediated by hydroxyl radicals(OH*),while releasing hydrogen gas.The coupling system has been operating stably for more than 300 h at an industrial-grade current density.This research provides new ideas for dual-electrode hydrogen production and green electrosynthesis of functional materials,with significant energy and economic benefits.展开更多
Regulating the critical process of proton migration from water dissociation for boosting alkaline hydrogen evolution reaction(HER)remains a challenge.Herein,we propose an electrostatic attraction strategy to achieve t...Regulating the critical process of proton migration from water dissociation for boosting alkaline hydrogen evolution reaction(HER)remains a challenge.Herein,we propose an electrostatic attraction strategy to achieve the migration of a highly efficient hydrogen species to Pt sites over Pt/Co@NC,which is obtained through a facile calcination and electrodeposition method.It exhibits an outstanding geometric activity(η_(10)=31 m V),which surpasses the commercial 20 wt%Pt/C(η_(10)=37 mV).Moreover,the mass activity of Pt/Co@NC is 5.6 A mg_(Pt)^(-1) at-50 mV vs.RHE,which is 2.23 times higher than that of 20 wt%Pt/C.Experimental and theoretical results indicate that the work function of the outer carbon layer,which is changed by the introduction of the inner cobalt core,plays a crucial role in reversing the direction of electron migration between the carbon layer and Pt.The negatively charged Pt^(δ-)can spontaneously attract positively charged protons via the electrostatic interaction effect,thereby achieving the directional migration of hydrogen species.This work presents a strategy for designing advanced alkaline HER electrocatalysts by the electrostatic effect.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
Propane dehydrogenation(PDH)is a key process for increasing the production of propylene,which is an important part of the chemical industry.Platinum-based catalysts have emerged as efficient catalysts for this reactio...Propane dehydrogenation(PDH)is a key process for increasing the production of propylene,which is an important part of the chemical industry.Platinum-based catalysts have emerged as efficient catalysts for this reaction due to their excellent activity and selectivity.However,challenges such as high platinum cost,catalyst deactivation,and side reactions remain significant barriers to their widespread use in industry.This review provides a comprehensive overview of recent advances in platinumbased catalysts for PDH,focusing on strategies to optimize their performance.We discuss the design and synthesis of Pt-based catalysts,emphasizing the role of promoters,such as Sn,Zn,Ga,and other promoters,in improving selectivity and stability.We also explore the effects of support materials and zeolite encapsulated catalysts on dispersion and activity for Pt-based catalysts.In addition,we highlight the use of machine learning to predict catalyst performance and guide the development of nextgeneration Pt-based catalyst materials.This review synthesizes insights from experimental studies and machine learning computational modeling and aims to provide a route for overcoming the limitations of Pt-based catalysts and advancing the PDH process.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
Over recent decades,fuel cell technologies have emerged as viable solutions to address the energy and environmental challenges stemming from fossil fuel dependence.Especially,ammonia has gained increasing attention as...Over recent decades,fuel cell technologies have emerged as viable solutions to address the energy and environmental challenges stemming from fossil fuel dependence.Especially,ammonia has gained increasing attention as an attractive alternative to hydrogen,offering comparable energy density while maintaining carbon-free characteristics,along with superior storage and transport properties that give direct ammonia fuel cells(DAFCs)distinct safety advantages over hydrogen-based systems.Central to this technology is the anodic ammonia oxidation reaction(AOR),where platinum(Pt)remains the most efficient catalyst after years of intensive research.This review offers a comprehensive overview of Ptbased AOR electrocatalysts with potential for application in low-temperature DAFCs.Following an introductory section highlighting key historical developments and catalytic breakthroughs,a fundamental understanding of low-temperature DAFC operation and AOR mechanisms is systematically presented.Subsequently,it outlines the advancements in Pt-based catalysts from simple monometallic systems to sophisticated multimetallic alloys and composites,highlighting material innovations and performance enhancements.Afterward,key challenges and future research directions for advancing AOR electrocatalysts are identified,with the aim of providing valuable guidance for developing practical,highperformance,and low-temperature DAFC systems.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 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 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the staff of beamline BL13SSW at Shanghai Synchrotron Radiation Facility for experiments supports. This study was financially supported by the National Natural Science Foundation of China (No. 12205165)Hebei Province Innovation Ability Improvement Plan Project (No. 225676111H).
文摘Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction(HER).Here,we reported PtNi nanoparticles with a refined size of 2.71 nm and regular strains loaded on carbon black,synthesized using the high-temperature liquid shock(HTLS)method.This approach offers significant advantages over conventional synthesis methods,including high scalability,rapid reaction rates,and precise control over the size and shape of nanocrystals.Importantly,the synthesized PtNi electrocatalysts demonstrate outstanding catalytic activity and long-term stability for HER,achieving low overpotentials of 19 and 203 mV at current densities of 10 and 1000 mA/cm^(2),respectively.The superior performance can be attributed to the combination of a refined particle size,lattice strains,and synergistic effects between Pt and Ni.This rapid liquid-state synthesis demonstrated here holds great potential for scalable and industrial manufacturing of micro-/nano-catalysts.
基金support from the National Natural Science Foundation of China(22473089,22573079)Shaanxi Key Research and Development Project(2024GX-YBXM-452)+3 种基金the Postdoctoral Research Project of Shaanxi(2023BSHYDZZ137)the Young Elite Scientists Sponsorship Program by Xi’an Association for Science and Technology(959202313084)the Scientific Research Program Funded by Education Department of Shaanxi Provincial Government(24JS050)the Zhijian Laboratory Program(2024-ZJSYS-KF02-03)。
文摘This study proposes a green electrochemical strategy for addressing the high-energy-barrier oxygen evolution reaction(OER)in traditional overall water splitting.Leveraging the thermodynamic advantages of N–H bond activation/cleavage and N–N coupling processes,the 3,5-diamino-1,2,4-triazole(DAT)oxidative coupling reaction(DATOR)has been introduced to replace the high-energy-barrier oxygen evolution reaction(OER).This substitution enables low-energy-consumption hydrogen production while simultaneously yielding high-value azo energetic materials.Furthermore,to enhance electron and atom economy,the anodic DATOR process allows the hydrogen radicals(H^(*))generated from amine dehydrogenation to chemically combine via the Tafel process,producing hydrogen gas.By constructing coupling system with Pts,n@NiS_(2)@CC cathode and Cu O/CF anode,the operating voltage of the system was significantly reduced(0.96 V@10 m A cm^(-2)),which was 680 mV more energy efficient than conventional water electrolysis(1.64 V).In situ spectroscopy and theoretical calculations indicate that the anode DATOR generates DAAT through the N–H bond cleavage and N–N coupling path mediated by hydroxyl radicals(OH*),while releasing hydrogen gas.The coupling system has been operating stably for more than 300 h at an industrial-grade current density.This research provides new ideas for dual-electrode hydrogen production and green electrosynthesis of functional materials,with significant energy and economic benefits.
基金financially supported by the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(23KJB610003)the Natural Science Foundation of Jiangsu Province(BK20240339)+2 种基金the Science and Technology Support Plan for Youth Innovation of Colleges and Universities of Shandong Province of China(No.2023KJ104)the National Natural Science Foundation of China(No.52202092)the Natural Science Foundation of Shandong Province(No.ZR2022QE076)。
文摘Regulating the critical process of proton migration from water dissociation for boosting alkaline hydrogen evolution reaction(HER)remains a challenge.Herein,we propose an electrostatic attraction strategy to achieve the migration of a highly efficient hydrogen species to Pt sites over Pt/Co@NC,which is obtained through a facile calcination and electrodeposition method.It exhibits an outstanding geometric activity(η_(10)=31 m V),which surpasses the commercial 20 wt%Pt/C(η_(10)=37 mV).Moreover,the mass activity of Pt/Co@NC is 5.6 A mg_(Pt)^(-1) at-50 mV vs.RHE,which is 2.23 times higher than that of 20 wt%Pt/C.Experimental and theoretical results indicate that the work function of the outer carbon layer,which is changed by the introduction of the inner cobalt core,plays a crucial role in reversing the direction of electron migration between the carbon layer and Pt.The negatively charged Pt^(δ-)can spontaneously attract positively charged protons via the electrostatic interaction effect,thereby achieving the directional migration of hydrogen species.This work presents a strategy for designing advanced alkaline HER electrocatalysts by the electrostatic effect.
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.
文摘Propane dehydrogenation(PDH)is a key process for increasing the production of propylene,which is an important part of the chemical industry.Platinum-based catalysts have emerged as efficient catalysts for this reaction due to their excellent activity and selectivity.However,challenges such as high platinum cost,catalyst deactivation,and side reactions remain significant barriers to their widespread use in industry.This review provides a comprehensive overview of recent advances in platinumbased catalysts for PDH,focusing on strategies to optimize their performance.We discuss the design and synthesis of Pt-based catalysts,emphasizing the role of promoters,such as Sn,Zn,Ga,and other promoters,in improving selectivity and stability.We also explore the effects of support materials and zeolite encapsulated catalysts on dispersion and activity for Pt-based catalysts.In addition,we highlight the use of machine learning to predict catalyst performance and guide the development of nextgeneration Pt-based catalyst materials.This review synthesizes insights from experimental studies and machine learning computational modeling and aims to provide a route for overcoming the limitations of Pt-based catalysts and advancing the PDH process.
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supported by the National Natural Science Foundation of China(No.52401284)the Natural Science Foundation of Jiangsu Province(No.BK20240957)+1 种基金the Key Research and Development Program of Nantong(No.GZ2024005)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX25_3677)。
文摘Over recent decades,fuel cell technologies have emerged as viable solutions to address the energy and environmental challenges stemming from fossil fuel dependence.Especially,ammonia has gained increasing attention as an attractive alternative to hydrogen,offering comparable energy density while maintaining carbon-free characteristics,along with superior storage and transport properties that give direct ammonia fuel cells(DAFCs)distinct safety advantages over hydrogen-based systems.Central to this technology is the anodic ammonia oxidation reaction(AOR),where platinum(Pt)remains the most efficient catalyst after years of intensive research.This review offers a comprehensive overview of Ptbased AOR electrocatalysts with potential for application in low-temperature DAFCs.Following an introductory section highlighting key historical developments and catalytic breakthroughs,a fundamental understanding of low-temperature DAFC operation and AOR mechanisms is systematically presented.Subsequently,it outlines the advancements in Pt-based catalysts from simple monometallic systems to sophisticated multimetallic alloys and composites,highlighting material innovations and performance enhancements.Afterward,key challenges and future research directions for advancing AOR electrocatalysts are identified,with the aim of providing valuable guidance for developing practical,highperformance,and low-temperature DAFC systems.
