Hydrogen peroxide(H_(2)O_(2))is an important chemical that can be sustainably produced through a twoelectron pathway in the electrocatalytic oxygen reduction reaction(ORR).However,the high cost and low reaction effici...Hydrogen peroxide(H_(2)O_(2))is an important chemical that can be sustainably produced through a twoelectron pathway in the electrocatalytic oxygen reduction reaction(ORR).However,the high cost and low reaction efficiency of catalysts currently limit the widespread application of this technology.Developing high-selectivity and scalable catalysts and accurately identifying the reaction active sites remain challenges.In this work,we have developed a promising nanodiamond(ND)catalyst to achieve high-selectivity H_(2)O_(2)production by oxygen reduction.Through surface carbon hybridization regulation to identify specific oxygen-containing functional groups combined with titration,model catalysis and DFT methods,it is found that the presence of carbonyl groups inducing the surrounding carbon atoms exhibit an optimal*OOH adsorption strength,thus promoting the two-electron pathway in ORR.Specifically,dynamic evolution processes of carbonyl groups and key adsorbed intermediate products including O_(2)(ads),superoxide anion*O_(2)^(-),and *OOH are monitored in situ spectroscopy.In the flowcell device,ND catalyst realizes the high H_(2)O_(2)Faradaic efficiency around 92% with a rate activity up to 105 mol gC=O^(-1)h^(-1),surpassing among reported non-metallic catalysts.The total H_(2)O_(2)yield reaches to 23.79 m M after a ten-hour test,which is 2.56 times higher than that of carbonyl-passivated ND,demonstrating its potential in scale-up application.Both titration and model catalytic processes proposed in this study further offer methods of designing efficient electrocatalysts for H_(2)O_(2)production.展开更多
The intriguing catalytic performance of non-metallic nitrogen-doped carbon materials in the oxygen reduction reaction(ORR) has garnered considerable interest in elucidating their active site structure.The existing stu...The intriguing catalytic performance of non-metallic nitrogen-doped carbon materials in the oxygen reduction reaction(ORR) has garnered considerable interest in elucidating their active site structure.The existing studies,however,present conflicting conclusions regarding the contributions of various N species to ORR activity.In this work,we designed and synthesized a series of molecules featuring well-defined structures and single N species,such as pyridinic N,graphitic N+(positively charged),and pyrrolic N,to serve as model catalysts.This approach aimed to eliminate the interference caused by the coexistence of multiple N species within carbon network,thereby providing a more precise understanding of their individual contributions to ORR activity.Our experimental results revealed that pyridinic N elevated onset potential,and graphitic N+enhanced current density in ORR.Both pyridinic N and graphitic N+can promote the transition of the ORR process from the 2e^(-) to the 4e^(-).Theoretical calculations further indicated that neutral graphitic N is more active than graphitic N+.Additionally,dynamic interconversion between graphitic N and graphitic N+(e.g.,via [4+1]e^(-),[2+1]e^(-),or [4-1]e^(-) pathways) during catalysis may adversely affect the intrinsic activity of graphitic N in practical applications.These findings provide insights into mechanism understanding in depth and design guidance for carbonbased catalysts for ORR.展开更多
Polymer thin film with uniform thickness and flat surface profile is the key point for polymer light emitting diodes(PLEDs) by inkjet printing. However, the coffee ring effect is usually observed due to the mismatch b...Polymer thin film with uniform thickness and flat surface profile is the key point for polymer light emitting diodes(PLEDs) by inkjet printing. However, the coffee ring effect is usually observed due to the mismatch between the evaporation of the solvent and the decrease of solution volume, which promotes the formation of radial flow from the interior of the drop to the edge. In this paper, coffee ring effects of inkjet printed poly(spirobifluorene) films were proposed to be restrained by decreasing capillary force by adding co-solvent with high boiling point and high viscosity to the main solvent. The low evaporation rate of the co-solvent can reduce the driving force of the radial flow; meanwhile the high viscosity of the co-solvent can increase the resistance of the radial flow. Thus, polymer films with improve uniformity can be obtained due to the suppression of the radial flow. The device performance was greatly improved under the condition of proper film thickness and film uniformity and the maximum luminous efficiency of devices with inkjet printed poly(spirobifluorene) can reach 80% of the spin-coated devices.展开更多
The carbon-based metal-free materials as catalysts(named as carbocatalysts) have been attracting tremendous attentions in electric-,solar-and thermal-driven reactions nowadays.Compared to electrocatalysis and photocat...The carbon-based metal-free materials as catalysts(named as carbocatalysts) have been attracting tremendous attentions in electric-,solar-and thermal-driven reactions nowadays.Compared to electrocatalysis and photocatalysis,the thermal-driven catalysis(thermocatalysis) including liquid phase and gas phase reactions involves wider scope and is relatively easy to realize practical large-scale applications.Over the past several years,some striking achievements on the design of new carbon-based metal-free materials with well-defined structures and heteroatom groups as well as the revelation of new reaction mechanisms and active sites in thermocatalysis have been obtained.However,comparative discussions regarding these recent achievements have been rarely highlighted.In this review,we systematically summarize and discuss six kinds of carbocatalysts and their applications in thermocatalysis.These materials include typical oxygen-attached carbon,surface modified carbon(graft with certain organic compounds),mono-doped carbon,co-doped carbon,carbon nitride and materials with carbon as dopant.Some new reaction processes as well as the related reaction mechanisms,active sites and intermediates are reviewed critically.Moreover,an outlook on the in-depth investigation of the metalfree carbocatalysis in the future is provided.展开更多
A metal-free catalytic system combining oxidized carbon nanotubes (oCNTs) and ionic liquids (ILs) is presented for the oxidation of aromatic thiophene compounds with H2O2 as an oxidant. The oCNTs exhibit impressively ...A metal-free catalytic system combining oxidized carbon nanotubes (oCNTs) and ionic liquids (ILs) is presented for the oxidation of aromatic thiophene compounds with H2O2 as an oxidant. The oCNTs exhibit impressively high activity and stability in the system, which show an even better performance than those of some reported metal catalysts. The ILs are proved to have indispensable influence on the enhanced catalytic performance of the oCNTs. Detailed characterization by TG-MS and XPS demonstrates that the carbonyl groups are the active sites for the oxidation process, which is further supported by the deactivation and the model catalysts experiments. The quantitative analysis of different oxygen groups in oCNTs could be achieved by an isothermal temperature programmed TG-MS method. The concentration of carbonyl groups is 1.46 mmol per 1 g oCNTs and the tuiriover frequency of oCNTs could also be obtained (10.7 h^-1 in the presence of OmimPF6). H2O2 decomposition experiments combined with the EPR results reveal that the presence of OmimPF6 can avoid the intermediate HO· to form O2 and then improve the catalytic performance of oCNTs for the oxidation of dibenzothiophene.展开更多
Fe-N-doped carbon materials(Fe-N-C)are promising candidates for oxygen reduction reaction(ORR)relative to Pt-based catalysts in proton exchange membrane fuel cells(PEMFCs).However,the intrinsic contributions of Fe-N_(...Fe-N-doped carbon materials(Fe-N-C)are promising candidates for oxygen reduction reaction(ORR)relative to Pt-based catalysts in proton exchange membrane fuel cells(PEMFCs).However,the intrinsic contributions of Fe-N_(4)moiety with different chemical/spin states(e.g.D1,D2,D3)to ORR are unclear since various states coexist inevitably.In the present work,Fe-N-C core-shell nanocatalyst with single lowspin Fe(Ⅱ)-N_(4)species(D1)is synthesized and identified with ex-situ ultralow temperature Mossbauer spectroscopy(T=1.6 K)that could essentially differentiate various Fe-N_(4)states and invisible Fe-O species.By quantifying with CO-pulse chemisorption,site density and turnover frequency of Fe-N-C catalysts reach 2.4×10^(-9)site g^(-1)and 23 e site~(-1)s^(-1)during the ORR,respectively.Half-wave potential(0.915V_(RHE))of the Fe-N-C catalyst is more positive(approximately 54 mV)than that of Pt/C.Moreover,we observe that the performance of PEMFCs on Fe-N-C almost achieves the 2025 target of the US Department of Energy by demonstrating a current density of 1.037 A cm^(-2)combined with the peak power density of 0,685 W cm^(-2),suggesting the critical role of Fe(Ⅱ)-N_(4)site(D1).After 500 h of running,PEMFCs still deliver a power density of 1.26 W cm^(-2)at 1.0 bar H_(2)-O_(2),An unexpected rate-determining step is figured out by isotopic labelling experiment and theoretical calculation.This work not only offers valuable insights regarding the intrinsic contribution of Fe-N_(4)with a single spin state to alkaline/acidic ORR,but also provides great opportunities for developing high-performance stable PEMFCs.展开更多
Metal-free carbon,as the most representative heterogeneous metal-free catalysts,have received considerable interests in electro-and thermo-catalytic reac-tions due to their impressive performance and sustainability.Ov...Metal-free carbon,as the most representative heterogeneous metal-free catalysts,have received considerable interests in electro-and thermo-catalytic reac-tions due to their impressive performance and sustainability.Over the past decade,well-designed carbon catalysts with tunable structures and heteroatom groups coupled with various characterization techniques have proposed numerous reaction mechanisms.However,active sites,key intermediate species,precise structure-activity relationships and dynamic evolution processes of carbon catalysts are still rife with controversies due to the monotony and limitation of used experimental methods.In this Review,we sum-marize the extensive efforts on model catalysts since the 2000s,particularly in the past decade,to overcome the influences of material and structure limitations in metal-free carbon catalysis.Using both nanomolecule model and bulk model,the real contribution of each alien species,defect and edge configuration to a series of fundamentally important reactions,such as thermocatalytic reactions,electrocatalytic reactions,were systematically studied.Combined with in situ techniques,isotope labeling and size control,the detailed reaction mechanisms,the precise 2D structure-activity relationships and the rate-determining steps were revealed at a molecular level.Furthermore,the outlook of model carbon catalysis has also been proposed in this work.展开更多
The use of renewable energy for hydrogen production through water electrolysis is a critical pathway for green hydrogen generation.Compared to pure water electrolysis,direct electrolysis of seawater offers several adv...The use of renewable energy for hydrogen production through water electrolysis is a critical pathway for green hydrogen generation.Compared to pure water electrolysis,direct electrolysis of seawater offers several advantages,such as raw material availability and application diversity.However,the complex composition of seawater presents significant technical challenges,particularly the competitive chloride oxidation reaction(ClOR)at the anode,which leads to equipment corrosion[1].展开更多
Oxygen evolution reaction(OER)is of significance in anodic reaction in the field of electrochemical energy conversion and storage,such as water splitting,metal-air battery,etc.[1,2].Being a thermodynamically downhill ...Oxygen evolution reaction(OER)is of significance in anodic reaction in the field of electrochemical energy conversion and storage,such as water splitting,metal-air battery,etc.[1,2].Being a thermodynamically downhill reaction comprising multiple-step proton coupled electron transfer within a narrow potential range(equations(1)-(5)),the reaction pathways involved in OER highly depend on the pH value of electrolyte[3,4].展开更多
The extensive utilization of proton exchange membrane fuel cells(PEMFCs)strongly depends on stable oxygen reduction reaction(ORR)catalysts operating under harsh conditions,i.e.,0.6–1.5 V,an acidic environment with pH...The extensive utilization of proton exchange membrane fuel cells(PEMFCs)strongly depends on stable oxygen reduction reaction(ORR)catalysts operating under harsh conditions,i.e.,0.6–1.5 V,an acidic environment with pH<1,and 60–80℃.Generally,structurally ordered L1_(0)-PtM(M being Fe,Co,Ni,etc.)intermetallic nanocrystals(i-NCs),stemming from a lower formation energy and higher cohesive energy,possess an enhanced durability,relative to the counterparts with a low ordering degree.展开更多
基金supported by the Natural Science Foundation of Xiamen City,China(3502Z20227256)National Natural Science Foundation of China(22202205,22209170)+3 种基金XMIREM Autonomously Deployment Project,China(2023CX14,2023GG01)Major Science and Technology Program of Xiamen City,China(3502Z20231054)National Natural Science Foundation of Fujian Province,China(2022J01502,2024J01185)STS Program of the Chinese Academy of Sciences,China(2023T3071)。
文摘Hydrogen peroxide(H_(2)O_(2))is an important chemical that can be sustainably produced through a twoelectron pathway in the electrocatalytic oxygen reduction reaction(ORR).However,the high cost and low reaction efficiency of catalysts currently limit the widespread application of this technology.Developing high-selectivity and scalable catalysts and accurately identifying the reaction active sites remain challenges.In this work,we have developed a promising nanodiamond(ND)catalyst to achieve high-selectivity H_(2)O_(2)production by oxygen reduction.Through surface carbon hybridization regulation to identify specific oxygen-containing functional groups combined with titration,model catalysis and DFT methods,it is found that the presence of carbonyl groups inducing the surrounding carbon atoms exhibit an optimal*OOH adsorption strength,thus promoting the two-electron pathway in ORR.Specifically,dynamic evolution processes of carbonyl groups and key adsorbed intermediate products including O_(2)(ads),superoxide anion*O_(2)^(-),and *OOH are monitored in situ spectroscopy.In the flowcell device,ND catalyst realizes the high H_(2)O_(2)Faradaic efficiency around 92% with a rate activity up to 105 mol gC=O^(-1)h^(-1),surpassing among reported non-metallic catalysts.The total H_(2)O_(2)yield reaches to 23.79 m M after a ten-hour test,which is 2.56 times higher than that of carbonyl-passivated ND,demonstrating its potential in scale-up application.Both titration and model catalytic processes proposed in this study further offer methods of designing efficient electrocatalysts for H_(2)O_(2)production.
基金financial support from the Natural Science Foundation of Xiamen City, China (3502Z20227256)National Natural Science Foundation of China (22202205, 22209170)+4 种基金XMIREM Autonomously Deployment Project, China (2023CX14, 2023GG01)Self-deployment Project Research Program of Haixi Institutes, Chinese Academy of Sciences (CXZX-2022-GH03, CXZX-2024-JQ02)Major Science and Technology Program of Xiamen City, China (3502Z20231054)National Natural Science Foundation of Fujian Province, China (2022J01502, 2024J01185)STS Program of the Chinese Academy of Sciences, China (2023T3071)。
文摘The intriguing catalytic performance of non-metallic nitrogen-doped carbon materials in the oxygen reduction reaction(ORR) has garnered considerable interest in elucidating their active site structure.The existing studies,however,present conflicting conclusions regarding the contributions of various N species to ORR activity.In this work,we designed and synthesized a series of molecules featuring well-defined structures and single N species,such as pyridinic N,graphitic N+(positively charged),and pyrrolic N,to serve as model catalysts.This approach aimed to eliminate the interference caused by the coexistence of multiple N species within carbon network,thereby providing a more precise understanding of their individual contributions to ORR activity.Our experimental results revealed that pyridinic N elevated onset potential,and graphitic N+enhanced current density in ORR.Both pyridinic N and graphitic N+can promote the transition of the ORR process from the 2e^(-) to the 4e^(-).Theoretical calculations further indicated that neutral graphitic N is more active than graphitic N+.Additionally,dynamic interconversion between graphitic N and graphitic N+(e.g.,via [4+1]e^(-),[2+1]e^(-),or [4-1]e^(-) pathways) during catalysis may adversely affect the intrinsic activity of graphitic N in practical applications.These findings provide insights into mechanism understanding in depth and design guidance for carbonbased catalysts for ORR.
基金financially supported by the National Natural Science Foundation of China (Nos. 21574130, 51473161, 51873212)the Ministry of Science and Technology of China (No. 2015CB655001)National Key R&D Program of "Strategic Advanced Electronic Materials" (Nos. 2016YFB0401301, 2016YFB04011001)
文摘Polymer thin film with uniform thickness and flat surface profile is the key point for polymer light emitting diodes(PLEDs) by inkjet printing. However, the coffee ring effect is usually observed due to the mismatch between the evaporation of the solvent and the decrease of solution volume, which promotes the formation of radial flow from the interior of the drop to the edge. In this paper, coffee ring effects of inkjet printed poly(spirobifluorene) films were proposed to be restrained by decreasing capillary force by adding co-solvent with high boiling point and high viscosity to the main solvent. The low evaporation rate of the co-solvent can reduce the driving force of the radial flow; meanwhile the high viscosity of the co-solvent can increase the resistance of the radial flow. Thus, polymer films with improve uniformity can be obtained due to the suppression of the radial flow. The device performance was greatly improved under the condition of proper film thickness and film uniformity and the maximum luminous efficiency of devices with inkjet printed poly(spirobifluorene) can reach 80% of the spin-coated devices.
基金supported by the Award Program for Fujian Minjiang Scholar Professorship,the National Natural Science Foundation of China(21571035)Chemical Engineering&Technology of Zhejiang Province First-Class Discipline(Taizhou University),Zhejiang Provincial Natural Science Foundation of China(LQ20B060001)Taizhou science and technology planning project(1902gy20)。
文摘The carbon-based metal-free materials as catalysts(named as carbocatalysts) have been attracting tremendous attentions in electric-,solar-and thermal-driven reactions nowadays.Compared to electrocatalysis and photocatalysis,the thermal-driven catalysis(thermocatalysis) including liquid phase and gas phase reactions involves wider scope and is relatively easy to realize practical large-scale applications.Over the past several years,some striking achievements on the design of new carbon-based metal-free materials with well-defined structures and heteroatom groups as well as the revelation of new reaction mechanisms and active sites in thermocatalysis have been obtained.However,comparative discussions regarding these recent achievements have been rarely highlighted.In this review,we systematically summarize and discuss six kinds of carbocatalysts and their applications in thermocatalysis.These materials include typical oxygen-attached carbon,surface modified carbon(graft with certain organic compounds),mono-doped carbon,co-doped carbon,carbon nitride and materials with carbon as dopant.Some new reaction processes as well as the related reaction mechanisms,active sites and intermediates are reviewed critically.Moreover,an outlook on the in-depth investigation of the metalfree carbocatalysis in the future is provided.
基金provided by the National Natural Science Foundation of China(No.21503241,21133010,21261160487,51221264,21411130120,21473223,91545119,91545110)the“Strategic Priority Research Program” of the Chinese Academy of Sciences(CAS)(No.XDA09030103)+1 种基金CAS/State Administration for Foreign Experts Affairs(SAFEA)International Partnership Program for Creative Research Teams and the Doctoral Starting up Foundation of Liaoning Province,China(No.20121068)the financial support from Max Planck Society and China Scholarship Council
文摘A metal-free catalytic system combining oxidized carbon nanotubes (oCNTs) and ionic liquids (ILs) is presented for the oxidation of aromatic thiophene compounds with H2O2 as an oxidant. The oCNTs exhibit impressively high activity and stability in the system, which show an even better performance than those of some reported metal catalysts. The ILs are proved to have indispensable influence on the enhanced catalytic performance of the oCNTs. Detailed characterization by TG-MS and XPS demonstrates that the carbonyl groups are the active sites for the oxidation process, which is further supported by the deactivation and the model catalysts experiments. The quantitative analysis of different oxygen groups in oCNTs could be achieved by an isothermal temperature programmed TG-MS method. The concentration of carbonyl groups is 1.46 mmol per 1 g oCNTs and the tuiriover frequency of oCNTs could also be obtained (10.7 h^-1 in the presence of OmimPF6). H2O2 decomposition experiments combined with the EPR results reveal that the presence of OmimPF6 can avoid the intermediate HO· to form O2 and then improve the catalytic performance of oCNTs for the oxidation of dibenzothiophene.
基金financial support from the“Hundred Talents Program”of the Chinese Academy of Sciencesthe“Young Talents Training Program”of the Shanghai Branch of the Chinese Academy of Sciences+3 种基金the financial support from the Xiamen City Natural Science Foundation of China(3502Z20227085,3502Z20227256)the National Science Youth Foundation of China(22202205)the Fujian Provincial Natural Science Foundation of China(2022J01502)Open Source Foundation of State Key Laboratory of Structural Chemistry。
文摘Fe-N-doped carbon materials(Fe-N-C)are promising candidates for oxygen reduction reaction(ORR)relative to Pt-based catalysts in proton exchange membrane fuel cells(PEMFCs).However,the intrinsic contributions of Fe-N_(4)moiety with different chemical/spin states(e.g.D1,D2,D3)to ORR are unclear since various states coexist inevitably.In the present work,Fe-N-C core-shell nanocatalyst with single lowspin Fe(Ⅱ)-N_(4)species(D1)is synthesized and identified with ex-situ ultralow temperature Mossbauer spectroscopy(T=1.6 K)that could essentially differentiate various Fe-N_(4)states and invisible Fe-O species.By quantifying with CO-pulse chemisorption,site density and turnover frequency of Fe-N-C catalysts reach 2.4×10^(-9)site g^(-1)and 23 e site~(-1)s^(-1)during the ORR,respectively.Half-wave potential(0.915V_(RHE))of the Fe-N-C catalyst is more positive(approximately 54 mV)than that of Pt/C.Moreover,we observe that the performance of PEMFCs on Fe-N-C almost achieves the 2025 target of the US Department of Energy by demonstrating a current density of 1.037 A cm^(-2)combined with the peak power density of 0,685 W cm^(-2),suggesting the critical role of Fe(Ⅱ)-N_(4)site(D1).After 500 h of running,PEMFCs still deliver a power density of 1.26 W cm^(-2)at 1.0 bar H_(2)-O_(2),An unexpected rate-determining step is figured out by isotopic labelling experiment and theoretical calculation.This work not only offers valuable insights regarding the intrinsic contribution of Fe-N_(4)with a single spin state to alkaline/acidic ORR,but also provides great opportunities for developing high-performance stable PEMFCs.
基金We are grateful for financial support from the“Hundred Talents Program”of the Chinese Academy of Sciences and the“Young Talents Training Program”of the Shanghai Branch of the Chinese Academy of Sciences.We acknowledge the financial support from the National Science Youth Foundation of China(22202205)Xiamen City Natural Science Foundation of China(3502Z20227256)Fujian Provincial Natural Science Foundation of China(2022J01502).
文摘Metal-free carbon,as the most representative heterogeneous metal-free catalysts,have received considerable interests in electro-and thermo-catalytic reac-tions due to their impressive performance and sustainability.Over the past decade,well-designed carbon catalysts with tunable structures and heteroatom groups coupled with various characterization techniques have proposed numerous reaction mechanisms.However,active sites,key intermediate species,precise structure-activity relationships and dynamic evolution processes of carbon catalysts are still rife with controversies due to the monotony and limitation of used experimental methods.In this Review,we sum-marize the extensive efforts on model catalysts since the 2000s,particularly in the past decade,to overcome the influences of material and structure limitations in metal-free carbon catalysis.Using both nanomolecule model and bulk model,the real contribution of each alien species,defect and edge configuration to a series of fundamentally important reactions,such as thermocatalytic reactions,electrocatalytic reactions,were systematically studied.Combined with in situ techniques,isotope labeling and size control,the detailed reaction mechanisms,the precise 2D structure-activity relationships and the rate-determining steps were revealed at a molecular level.Furthermore,the outlook of model carbon catalysis has also been proposed in this work.
基金supported by the National Natural Science Foundation of China(Grant Nos.22202205 and 22209170)XMIREM Autonomously Deployment Project,China(Nos.2023CX14,2023GG01)+4 种基金Self-deployment Project Research Program of Haixi Institutes,Chinese Academy of Sciences(Nos.CXZX-2022-GH03,CXZX-2024-JQ02)Major Science and Technology Program of Xiamen,China(No.3502Z20231054)Natural Science Foundation of Fujian Province,China(Grant Nos.2022J01502 and 2024J01185)STS Program of the Chinese Academy of Sciences,China(No.2023T3071)Natural Science Foundation of Xiamen,China(No.3502Z20227256).
文摘The use of renewable energy for hydrogen production through water electrolysis is a critical pathway for green hydrogen generation.Compared to pure water electrolysis,direct electrolysis of seawater offers several advantages,such as raw material availability and application diversity.However,the complex composition of seawater presents significant technical challenges,particularly the competitive chloride oxidation reaction(ClOR)at the anode,which leads to equipment corrosion[1].
基金support from the Xiamen City Natural Science Foundation of China(3502Z20227256)National Natural Science Foundation of China(22202205)Natural Science Foundation of Fujian Province(2022J01502).
文摘Oxygen evolution reaction(OER)is of significance in anodic reaction in the field of electrochemical energy conversion and storage,such as water splitting,metal-air battery,etc.[1,2].Being a thermodynamically downhill reaction comprising multiple-step proton coupled electron transfer within a narrow potential range(equations(1)-(5)),the reaction pathways involved in OER highly depend on the pH value of electrolyte[3,4].
基金supported by the Natural Science Foundation of Xiamen,China(Grant No.3502Z20227256)the XMIREM Autonomously Deployment Project,China(Grant Nos.2023CX14 and 2023GG01)+3 种基金the Major Science and Technology Program of Xiamen,China(Grant No.3502Z20231054)the Natural Science Foundation of Fujian Province,China(Grant No.2022J01502)the National Natural Science Foundation of China(Grant Nos.22202205 and 22209170)the STS Program of the Chinese Academy of Sciences,China(Grant No.2023T3071).
文摘The extensive utilization of proton exchange membrane fuel cells(PEMFCs)strongly depends on stable oxygen reduction reaction(ORR)catalysts operating under harsh conditions,i.e.,0.6–1.5 V,an acidic environment with pH<1,and 60–80℃.Generally,structurally ordered L1_(0)-PtM(M being Fe,Co,Ni,etc.)intermetallic nanocrystals(i-NCs),stemming from a lower formation energy and higher cohesive energy,possess an enhanced durability,relative to the counterparts with a low ordering degree.
