Sulfur and nitrogen dual-doped graphdiyne(NSGD)has been found to be a promising catalyst for oxygen reduction reaction(ORR)through a combination of density functional theory(DFT)calculation and the application of oxyg...Sulfur and nitrogen dual-doped graphdiyne(NSGD)has been found to be a promising catalyst for oxygen reduction reaction(ORR)through a combination of density functional theory(DFT)calculation and the application of oxygen evolution reaction(OER)experiments.The DFT analysis suggests that adsorption characteristics are significantly altered by resulting nitrogen and sulfur doping,which in turn affect the ORR activity.In particular,the NSGD-800 catalyst exhibits an increased ORR half-wave potential of 0.754 V,with enhanced stability due to the synergy effect of N and S.Meanwhile,thanks to the unique acetylene-rich structure of graphdiyne to anchor metal oxides with strong d-πinteractions,the activity and stability of com-RuO2 for OER were significantly enhanced by mixing with NSGD-800.The zinc-air battery(ZAB)with NSGD shows a much higher peak power density(87.3 mW cm^(−2))and longer charge-discharge cycle stability compared with the ZAB with Pt/C,making it an excellent candidate air electrode for ZAB and other energy storage and conversion devices.展开更多
Glutamate-ammonia ligase(GLUL, also known as glutamine synthetase) is a crucial enzyme that catalyzes ammonium and glutamate into glutamine in the ATP-dependent condensation. Although GLUL plays a critical role in mul...Glutamate-ammonia ligase(GLUL, also known as glutamine synthetase) is a crucial enzyme that catalyzes ammonium and glutamate into glutamine in the ATP-dependent condensation. Although GLUL plays a critical role in multiple cancers, the expression and function of GLUL in gastric cancer remain unclear. In the present study, we have found that the expression level of GLUL was significantly lower in gastric cancer tissues compared with adjacent normal tissues, and correlated with N stage and TNM stage, and low GLUL expression predicted poor survival for gastric cancer patients. Knockdown of GLUL promoted the growth, migration, invasion and metastasis of gastric cancer cells in vitro and in vivo, and vice versa, which was independent of its enzyme activity. Mechanistically, GLUL competed with β-Catenin to bind to N-Cadherin, increased the stability of N-Cadherin and decreased the stability of β-Catenin by alerting their ubiquitination. Furthermore, there were lower N-Cadherin and higher β-Catenin expression levels in gastric cancer tissues compared with adjacent normal tissues. GLUL protein expression was correlated with that of N-Cadherin, and could be the independent prognostic factor in gastric cancer. Our findings reveal that GLUL stabilizes N-Cadherin by antagonizing β-Catenin to inhibit the progress of gastric cancer.展开更多
Developing non-noble metal-based electrocatalyst with high catalytic activity is essential for advancing hydrogen energy technologies.This study introduces a hydrothermal method for synthesizing order Ni(OH)_(2) nanos...Developing non-noble metal-based electrocatalyst with high catalytic activity is essential for advancing hydrogen energy technologies.This study introduces a hydrothermal method for synthesizing order Ni(OH)_(2) nanosheets,with H_(3)O_(40)PW_(12)(denoted as PW_(12))loaded onto reduced graphene oxide(rGO)coated on nickel foam(referred to as PW_(12)-Ni(OH)_(2)/rGO).This method contrasts with the electrodeposition of Ni(OH)_(2),where PW_(12) is added to the synthetic system to direct the assembly and morphology of the Ni(OH)_(2) through a hydrothermal reaction.In this work,the nickel foam acts dual roles as both the substrate and the source of nickel for the formation of Ni(OH)_(2).The PW_(12)-Ni(OH)_(2)/rGO nanosheets,when successfully prepared and loaded onto the nickel foam(NF),exhibited superior electrocatalytic activity for the hydrogen evolution reaction(HER)in an alkaline electrolyte,achieving a current density of 10 mA·cm^(-2) at an overpotential of 69 mV.Furthermore,we endeavored to expand the application of this material towards the oxygen evolution reaction(OER)by preparing PW_(12)-(Fe/Co)Ni(OH)_(2)/rGO through the addition of metal cations.This nanocomposite displayed outstanding electrocatalytic activity in alkaline electrolytes,with a current density of 10 mA·cm^(-2)at an overpotential of 211 mV,and demonstrated excellent stability over a 50 h period in a 1 M KOH solution.The results presented in this paper offer an effective strategy for the preparation of polyoxometalate-based inorganic materials with diverse functionalities,applicable to both HER and OER.展开更多
Polyoxometalate-based nanocomposites with electrocatalytic activity have been applied in hydrogen evolution reactions(HER).Seawater as the main water resource on the earth should be developed as the water electrolysis...Polyoxometalate-based nanocomposites with electrocatalytic activity have been applied in hydrogen evolution reactions(HER).Seawater as the main water resource on the earth should be developed as the water electrolysis to prepare high-purity hydrogen.In this paper,we used two synthesis strategies to prepare the nanocomposite Co_(4)-POM@Co-PGDY(Co_(4)-POM:the Kegging-type microcrystals of K_(10)[Co_(4)(PW_(9)O_(3)4)2]and Co-PGDY:cobalt-porphyrin linked graphdiyne)with excellent activity for HER.Co-PGDY as the porous material is applied not only as the protection of microcrystals towards the metal ion in seawater but also as the co-electrocatalyst of Co_(4)-POM.Co_(4)-POM@Co-PGDY exhibits excellent HER performance in seawater electrolytes with low overpotential and high stability at high density.Moreover,we have observed a key H_(3)O+intermediate emergence on the surface of nanocomposite during hydrogen evolution process in seawater by Raman synchrotron radiation-based Fourier transform infrared(SR-FTIR).The results in this paper provide an effective strategy for preparing polyoxometalate-based electrocatalysts with high-performance toward hydrogen evolution reaction.展开更多
Electrochemical energy storage(EES)is a key technology in global research that focuses on the efficient storage and utilization of electrical energy generated from intermittent sources.The development of EES systems w...Electrochemical energy storage(EES)is a key technology in global research that focuses on the efficient storage and utilization of electrical energy generated from intermittent sources.The development of EES systems with high energy and power densities is essential for meeting the future energy demands of electrochemical capacitors,such as capacitors,which can store electrical energy obtained from intermittent sources and enable rapid energy transfer and transformation.Electrical double-layer capacitors(EDLCs)within porous carbon materials(Fig.1(a))are commercially popular because of their excellent conductivity and relatively low cost.Despite their advantages,the complex structure of nanoporous carbon materials hinders the optimization of supercapacitor performance.Although previous research has suggested that adjusting the pore size of nanoporous carbon materials can enhance their capacitive performance,conflicting reports and the lack of a definitive correlation between capacitance and pore size remain issues[1].Understanding the relationship between the structure of carbon materials and their capacitance is crucial for designing devices with high energy densities.展开更多
Osteosarcoma(OS)is the most common primary malignant bone tumor in children and adolescents.Although activator of HSP90 ATPase activity 1(AHA1)is reported to be a potential oncogene,its role in osteosarcoma progressio...Osteosarcoma(OS)is the most common primary malignant bone tumor in children and adolescents.Although activator of HSP90 ATPase activity 1(AHA1)is reported to be a potential oncogene,its role in osteosarcoma progression remains largely unclear.Since metabolism reprogramming is involved in tumorigenesis and cancer metastasis,the relationship between AHA1 and cancer metabolism is unknown.In this study,we found that AHA1 is significantly overexpressed in osteosarcoma and related to the prognosis of osteosarcoma patients.AHA1 promotes the growth and metastasis of osteosarcoma both in vitro and in vivo.Mechanistically,AHA1 upregulates the metabolic activity to meet cellular bioenergetic needs in osteosarcoma.Notably,we identifed that isocitrate dehydrogenase 1(IDH1)is a novel client protein of Hsp90 AHA1.Furthermore,the IDH1 protein level was positively correlated with AHA1 in osteosarcoma.And IDH1 overexpression could partially reverse the effect of AHA1 knockdown on cell growth and migration of osteosarcoma.Moreover,high IDH1 level was also associated with poor prognosis of osteosarcoma patients.This study demonstrates that AHA1 positively regulates IDH1 and metabolic activity to promote osteosarcoma growth and metastasis,which provides novel prognostic biomarkers and promising therapeutic targets for osteosarcoma patients.展开更多
Platinum based alloys are hereinto the mostly used methanol oxidation catalysts.However,there are limited ways to improve the methanol oxidation reaction(MOR)performance of catalysts in terms of both activity and stab...Platinum based alloys are hereinto the mostly used methanol oxidation catalysts.However,there are limited ways to improve the methanol oxidation reaction(MOR)performance of catalysts in terms of both activity and stability.Herein we developed a simple heat-treatment method to synthesize PtCu_(3)/C intermetallic compound catalyst with lattice compression.The as-prepared PtCu_(3)/C-1000 exhibited high specific activity of 3.23 mA·cm^(-1) and mass activity of 1,200 mA·mgPt^(-1),which is much higher than the PtCu_(3)/C-untreated and commercial Pt/C catalysts,respectively.The XAS and DFT results shows the high activity of the catalyst towards MOR comes from the tightening of the Pt-M bond,which leads to the decrease of Fermi energy level and the make it difficulty in adsorbing carbon intermediates,thus releasing more active sites to promote the improvement of MOR performance.Moreover,the PtCu_(3)/C-1000 shows better stability which is due to the surface-rich Pt prevents Cu from dissolution.展开更多
Zinc-air batteries hold great promise as a next-generation efficient and environmentally friendly energy technology.However,the sluggish kinetics of the oxygen reduction reaction(ORR)process pose a significant challen...Zinc-air batteries hold great promise as a next-generation efficient and environmentally friendly energy technology.However,the sluggish kinetics of the oxygen reduction reaction(ORR)process pose a significant challenge to their development.To address this issue,atom dispersion catalysts are developed to maximize the utilization of metal active centers.Metal-organic frameworks(MOFs)are a series of molecular materials with high atomic-level dispersion metal utilization,but they often lack sufficient electrical conductivity.Their application in MOF electrocatalysis remains limited unless the MOF material is transferred to a carbon-based material through heat treatment.To overcome this limitation,we employed coordination engineering to incorporate hexaaminotriphenylene(HATP)molecules with strong conjugation into Co-MOF-74.The resulting Co-MOF-74-HATP catalyst represents high activity,achieving an ORR half-wave potential(E_(1/2))of 0.84 V and demonstrating good stability(ΔE_(1/2)=20 mV after 10,000 cycles).Additionally,the Co-MOF-74-HATP also performs a 320 mV overpotential(10 mA·cm^(-2))for the oxygen evolution reaction.Meanwhile,Co-MOF-74-HATP displays a peak power density of 96.6 mW·cm^(-2) in zinc-air batteries,surpassing the commercially available Pt/C+RuO_(2).This work presents a new pathway to design MOF-based ORR catalysts and provides a new direction for the preparation of key materials for zinc-air battery(ZAB).展开更多
The development of electrocatalysts for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is crucial for sustainable energy and environmental initiatives.This work establishes an atomically-dispersed R...The development of electrocatalysts for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is crucial for sustainable energy and environmental initiatives.This work establishes an atomically-dispersed Ru-based model to investigate the promoting mechanism by the Ru-Integration effect in RuCo bimetallic nanoparticles supported on nitrogen-doped carbon(RuCo@NC).Specially,the Ru content in RuCo@NC plays a vital role for both HER and OER.The optimized catalyst shows an outstanding performance,requiring only 217 and 97 mV overpotential to reach a current density of 10 mA·cm^(−2)for OER and HER respectively in alkaline conditions.Combined with advanced characterizations such as spherical aberration-corrected scanning transmission electron microscopy,X-ray absorption spectroscopy,in-situ Raman spectroscopy,and density functional theory calculations,it is found that Ru plays multiple crucial roles:(1)Ru restricts the growth of large Co NPs,while the small-sized Co NPs facilitate the formation of carbon nanotubes,which significantly enhances the mass/electron transfer;(2)Ru not only tunes the surface properties of Co but also acts as an active site for HER.As a result,when using RuCo@NC as an overall water splitting catalyst,it only needs a potential of 1.62 V to reach a current density of 100 mA·cm^(−2).This work offers valuable insights into designing Ru-based electrocatalysts for water splitting.展开更多
Green hydrogen production by proton exchange membrane water electrolysis(PEMWE)is considered a promising method for sustainable hydrogen production using renewable energy[1],[2].Currently,iridium-based oxides(IrOx)are...Green hydrogen production by proton exchange membrane water electrolysis(PEMWE)is considered a promising method for sustainable hydrogen production using renewable energy[1],[2].Currently,iridium-based oxides(IrOx)are widely used in PEMWE as anodic catalysts for the oxygen evolution reaction(OER)owing their high durability and activity(Fig.1(a)).展开更多
基金supported by the National Natural Science Foundation of China(22202037 and 22102105)the Fundamental Research Funds for the Central Universities(2412023QD019 and 2412024QD014)+1 种基金the support from grants under the Science and Technology Development Plan Project of Jilin Province,China(20240101192JC)seventh batch of the Jilin Province Youth Science and Technology Talent Lifting Project(QT202305)。
文摘Sulfur and nitrogen dual-doped graphdiyne(NSGD)has been found to be a promising catalyst for oxygen reduction reaction(ORR)through a combination of density functional theory(DFT)calculation and the application of oxygen evolution reaction(OER)experiments.The DFT analysis suggests that adsorption characteristics are significantly altered by resulting nitrogen and sulfur doping,which in turn affect the ORR activity.In particular,the NSGD-800 catalyst exhibits an increased ORR half-wave potential of 0.754 V,with enhanced stability due to the synergy effect of N and S.Meanwhile,thanks to the unique acetylene-rich structure of graphdiyne to anchor metal oxides with strong d-πinteractions,the activity and stability of com-RuO2 for OER were significantly enhanced by mixing with NSGD-800.The zinc-air battery(ZAB)with NSGD shows a much higher peak power density(87.3 mW cm^(−2))and longer charge-discharge cycle stability compared with the ZAB with Pt/C,making it an excellent candidate air electrode for ZAB and other energy storage and conversion devices.
基金supported by funds from the National Key Research and Development Program of China No.2017YFA0505104(Zhi Shi)the National Natural Science Foundation of China Nos.81772540 and 82272996(Zhi Shi)+1 种基金the Science and Technology Program of Guangdong No.2019A050510023(Zhi Shi,China)the Science and Technology Program of Guangzhou No.20220-6010081(Zhi Shi,China).
文摘Glutamate-ammonia ligase(GLUL, also known as glutamine synthetase) is a crucial enzyme that catalyzes ammonium and glutamate into glutamine in the ATP-dependent condensation. Although GLUL plays a critical role in multiple cancers, the expression and function of GLUL in gastric cancer remain unclear. In the present study, we have found that the expression level of GLUL was significantly lower in gastric cancer tissues compared with adjacent normal tissues, and correlated with N stage and TNM stage, and low GLUL expression predicted poor survival for gastric cancer patients. Knockdown of GLUL promoted the growth, migration, invasion and metastasis of gastric cancer cells in vitro and in vivo, and vice versa, which was independent of its enzyme activity. Mechanistically, GLUL competed with β-Catenin to bind to N-Cadherin, increased the stability of N-Cadherin and decreased the stability of β-Catenin by alerting their ubiquitination. Furthermore, there were lower N-Cadherin and higher β-Catenin expression levels in gastric cancer tissues compared with adjacent normal tissues. GLUL protein expression was correlated with that of N-Cadherin, and could be the independent prognostic factor in gastric cancer. Our findings reveal that GLUL stabilizes N-Cadherin by antagonizing β-Catenin to inhibit the progress of gastric cancer.
基金supported by the National Natural Science Foundation of China(Nos.21831001,21801014,22171024,and 22202037)the Fundamental Research Funds for the Central Universities(No.2412023QD019)supported by the Analysis&Testing Center of Beijing Institute of Technology.
文摘Developing non-noble metal-based electrocatalyst with high catalytic activity is essential for advancing hydrogen energy technologies.This study introduces a hydrothermal method for synthesizing order Ni(OH)_(2) nanosheets,with H_(3)O_(40)PW_(12)(denoted as PW_(12))loaded onto reduced graphene oxide(rGO)coated on nickel foam(referred to as PW_(12)-Ni(OH)_(2)/rGO).This method contrasts with the electrodeposition of Ni(OH)_(2),where PW_(12) is added to the synthetic system to direct the assembly and morphology of the Ni(OH)_(2) through a hydrothermal reaction.In this work,the nickel foam acts dual roles as both the substrate and the source of nickel for the formation of Ni(OH)_(2).The PW_(12)-Ni(OH)_(2)/rGO nanosheets,when successfully prepared and loaded onto the nickel foam(NF),exhibited superior electrocatalytic activity for the hydrogen evolution reaction(HER)in an alkaline electrolyte,achieving a current density of 10 mA·cm^(-2) at an overpotential of 69 mV.Furthermore,we endeavored to expand the application of this material towards the oxygen evolution reaction(OER)by preparing PW_(12)-(Fe/Co)Ni(OH)_(2)/rGO through the addition of metal cations.This nanocomposite displayed outstanding electrocatalytic activity in alkaline electrolytes,with a current density of 10 mA·cm^(-2)at an overpotential of 211 mV,and demonstrated excellent stability over a 50 h period in a 1 M KOH solution.The results presented in this paper offer an effective strategy for the preparation of polyoxometalate-based inorganic materials with diverse functionalities,applicable to both HER and OER.
基金supported by the National Natural Science Foundation of China(Nos.21831001,21801014,22171024,and 22202037)the Fundamental Research Funds for the Central Universities(No.2412023QD019).
文摘Polyoxometalate-based nanocomposites with electrocatalytic activity have been applied in hydrogen evolution reactions(HER).Seawater as the main water resource on the earth should be developed as the water electrolysis to prepare high-purity hydrogen.In this paper,we used two synthesis strategies to prepare the nanocomposite Co_(4)-POM@Co-PGDY(Co_(4)-POM:the Kegging-type microcrystals of K_(10)[Co_(4)(PW_(9)O_(3)4)2]and Co-PGDY:cobalt-porphyrin linked graphdiyne)with excellent activity for HER.Co-PGDY as the porous material is applied not only as the protection of microcrystals towards the metal ion in seawater but also as the co-electrocatalyst of Co_(4)-POM.Co_(4)-POM@Co-PGDY exhibits excellent HER performance in seawater electrolytes with low overpotential and high stability at high density.Moreover,we have observed a key H_(3)O+intermediate emergence on the surface of nanocomposite during hydrogen evolution process in seawater by Raman synchrotron radiation-based Fourier transform infrared(SR-FTIR).The results in this paper provide an effective strategy for preparing polyoxometalate-based electrocatalysts with high-performance toward hydrogen evolution reaction.
基金supported by the National Natural Science Foundation of China(grant numbers 22102105 and 22202037)the Fundamental Research Funds for the Central Universities(grant numbers 2412024QD014 and 2412023QD019)support from Northeast Normal University.Z.X.thanks support from grants under the seventh batch of the Jilin Province Youth Science and Technology Talent Lifting Project(grant number QT202305).
文摘Electrochemical energy storage(EES)is a key technology in global research that focuses on the efficient storage and utilization of electrical energy generated from intermittent sources.The development of EES systems with high energy and power densities is essential for meeting the future energy demands of electrochemical capacitors,such as capacitors,which can store electrical energy obtained from intermittent sources and enable rapid energy transfer and transformation.Electrical double-layer capacitors(EDLCs)within porous carbon materials(Fig.1(a))are commercially popular because of their excellent conductivity and relatively low cost.Despite their advantages,the complex structure of nanoporous carbon materials hinders the optimization of supercapacitor performance.Although previous research has suggested that adjusting the pore size of nanoporous carbon materials can enhance their capacitive performance,conflicting reports and the lack of a definitive correlation between capacitance and pore size remain issues[1].Understanding the relationship between the structure of carbon materials and their capacitance is crucial for designing devices with high energy densities.
基金This work was supported by funds from the National Key Research and Development Program of China(No.2017YFA0505104)National Natural Science Foundation of China(Nos.81772540,81472506.81772861)+7 种基金the Science and Technology Program of Guangdong(No.2019A050510023)Guangdong Province Special Fund for Science and Technology Development(No.2017A050501015)Natural Science Foundation of Guangdong(Nos.2016A030313227,2018A030313689)the Science and Technology Program of Guangzhou(Nos.201704030008,201707010007)the Fundamental Research Funds for the Central Universities(No.19ykzd10)Cultivation of Major Projects,Sun Yat-sen University(No.80000-18823701)Cultivation of International Scientifhc Research Cooperation Platform.Sun Yat-sen University(No.800018827202)“3×3”Project,the First Afliated Hospital of Sun Yat-sen Universty(No.Y70215).
文摘Osteosarcoma(OS)is the most common primary malignant bone tumor in children and adolescents.Although activator of HSP90 ATPase activity 1(AHA1)is reported to be a potential oncogene,its role in osteosarcoma progression remains largely unclear.Since metabolism reprogramming is involved in tumorigenesis and cancer metastasis,the relationship between AHA1 and cancer metabolism is unknown.In this study,we found that AHA1 is significantly overexpressed in osteosarcoma and related to the prognosis of osteosarcoma patients.AHA1 promotes the growth and metastasis of osteosarcoma both in vitro and in vivo.Mechanistically,AHA1 upregulates the metabolic activity to meet cellular bioenergetic needs in osteosarcoma.Notably,we identifed that isocitrate dehydrogenase 1(IDH1)is a novel client protein of Hsp90 AHA1.Furthermore,the IDH1 protein level was positively correlated with AHA1 in osteosarcoma.And IDH1 overexpression could partially reverse the effect of AHA1 knockdown on cell growth and migration of osteosarcoma.Moreover,high IDH1 level was also associated with poor prognosis of osteosarcoma patients.This study demonstrates that AHA1 positively regulates IDH1 and metabolic activity to promote osteosarcoma growth and metastasis,which provides novel prognostic biomarkers and promising therapeutic targets for osteosarcoma patients.
基金This work was supported by the National Natural Science Foundation of China(Nos.51872209 and 51972239)the Key programs for Science and Technology Innovation of Wenzhou(No.2018ZG005).
文摘Platinum based alloys are hereinto the mostly used methanol oxidation catalysts.However,there are limited ways to improve the methanol oxidation reaction(MOR)performance of catalysts in terms of both activity and stability.Herein we developed a simple heat-treatment method to synthesize PtCu_(3)/C intermetallic compound catalyst with lattice compression.The as-prepared PtCu_(3)/C-1000 exhibited high specific activity of 3.23 mA·cm^(-1) and mass activity of 1,200 mA·mgPt^(-1),which is much higher than the PtCu_(3)/C-untreated and commercial Pt/C catalysts,respectively.The XAS and DFT results shows the high activity of the catalyst towards MOR comes from the tightening of the Pt-M bond,which leads to the decrease of Fermi energy level and the make it difficulty in adsorbing carbon intermediates,thus releasing more active sites to promote the improvement of MOR performance.Moreover,the PtCu_(3)/C-1000 shows better stability which is due to the surface-rich Pt prevents Cu from dissolution.
基金This work was supported by National Natural Science Foundation of China(Nos.22202037,22472023 and 22102105)the Fundamental Research Funds for the Central Universities(Nos.2412024QD014 and 2412023QD019).
文摘Zinc-air batteries hold great promise as a next-generation efficient and environmentally friendly energy technology.However,the sluggish kinetics of the oxygen reduction reaction(ORR)process pose a significant challenge to their development.To address this issue,atom dispersion catalysts are developed to maximize the utilization of metal active centers.Metal-organic frameworks(MOFs)are a series of molecular materials with high atomic-level dispersion metal utilization,but they often lack sufficient electrical conductivity.Their application in MOF electrocatalysis remains limited unless the MOF material is transferred to a carbon-based material through heat treatment.To overcome this limitation,we employed coordination engineering to incorporate hexaaminotriphenylene(HATP)molecules with strong conjugation into Co-MOF-74.The resulting Co-MOF-74-HATP catalyst represents high activity,achieving an ORR half-wave potential(E_(1/2))of 0.84 V and demonstrating good stability(ΔE_(1/2)=20 mV after 10,000 cycles).Additionally,the Co-MOF-74-HATP also performs a 320 mV overpotential(10 mA·cm^(-2))for the oxygen evolution reaction.Meanwhile,Co-MOF-74-HATP displays a peak power density of 96.6 mW·cm^(-2) in zinc-air batteries,surpassing the commercially available Pt/C+RuO_(2).This work presents a new pathway to design MOF-based ORR catalysts and provides a new direction for the preparation of key materials for zinc-air battery(ZAB).
基金supported by National Natural Science Foundation of China(Nos.22472023,22202037 and 22102105)the Fundamental Research Funds for the Central Universities(Nos.2412024QD014 and 2412023QD019)This work was also supported by the Science and Technology Development Plan Project of Jilin Province,China(No.20240101192JC).
文摘The development of electrocatalysts for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is crucial for sustainable energy and environmental initiatives.This work establishes an atomically-dispersed Ru-based model to investigate the promoting mechanism by the Ru-Integration effect in RuCo bimetallic nanoparticles supported on nitrogen-doped carbon(RuCo@NC).Specially,the Ru content in RuCo@NC plays a vital role for both HER and OER.The optimized catalyst shows an outstanding performance,requiring only 217 and 97 mV overpotential to reach a current density of 10 mA·cm^(−2)for OER and HER respectively in alkaline conditions.Combined with advanced characterizations such as spherical aberration-corrected scanning transmission electron microscopy,X-ray absorption spectroscopy,in-situ Raman spectroscopy,and density functional theory calculations,it is found that Ru plays multiple crucial roles:(1)Ru restricts the growth of large Co NPs,while the small-sized Co NPs facilitate the formation of carbon nanotubes,which significantly enhances the mass/electron transfer;(2)Ru not only tunes the surface properties of Co but also acts as an active site for HER.As a result,when using RuCo@NC as an overall water splitting catalyst,it only needs a potential of 1.62 V to reach a current density of 100 mA·cm^(−2).This work offers valuable insights into designing Ru-based electrocatalysts for water splitting.
基金supported by the National Natural Science Foundation of China(22102105,22202037)the Fundamental Research Funds for the Central Universities(Nos.2412023QD019 and 2412024QD014)。
文摘Green hydrogen production by proton exchange membrane water electrolysis(PEMWE)is considered a promising method for sustainable hydrogen production using renewable energy[1],[2].Currently,iridium-based oxides(IrOx)are widely used in PEMWE as anodic catalysts for the oxygen evolution reaction(OER)owing their high durability and activity(Fig.1(a)).
