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
Addressing inadequate OH^(*)adsorption in Ru Co alloy catalysts is crucial for boosting intermediate coverage and redirecting the water-splitting pathway.Herein,the adaptive P sites were strategically incorporated to ...Addressing inadequate OH^(*)adsorption in Ru Co alloy catalysts is crucial for boosting intermediate coverage and redirecting the water-splitting pathway.Herein,the adaptive P sites were strategically incorporated to overcome the aforementioned challenge.The P sites,as potent OH^(*)adsorption centers,synergize with Co sites to promote water dissociation and enrich surrounding Ru sites with H*intermediates,thus triggering the Volmer-Tafel route for hydrogen evolution reaction(HER).Besides,during the oxygen evolution reaction(OER),the surface of P-Ru Co was reconstructed into Ru-doped Co OOH with anchored PO_(4)^(3-).These PO_(4)^(3-)not only circumvent the intrinsic OH^(*)adsorption limitations of Ru-Co OOH in the adsorbate evolution mechanism(AEM)by rerouting to a more expeditious lattice oxygen oxidation mechanism(LOM)but also improve the coverage of key oxygen-containing intermediates,significantly accelerating OER kinetics.Consequently,the P-Ru Co demonstrates exceptional bifunctional performance,with overpotentials of 29 m V for HER and 222 m V for OER at 10 m A cm^(-2).Remarkably,the mass activities of PRu Co for HER(5.48 A mg^(-1))and OER(2.13 A mg^(-1))are 6.2 and 11.2 times higher than those of its commercial counterparts(Ru/C for HER and RuO_(2)for OER),respectively.When integrated into an anionexchange-membrane electrolyzer,this catalyst achieves ampere-level current densities of 1.32 A cm^(-2)for water electrolysis and 1.23 A cm^(-2)for seawater electrolysis at 2.1 V,with a 500-h durability.展开更多
By adjusting various Ru/M （M=Co, Ni） molar ratios, a series of highly dispersed bimetallic RuM alloy nanoparticles （NPs） anchored on MIL-110（Al） have been successfully prepared via a conventional impregnation-re...By adjusting various Ru/M （M=Co, Ni） molar ratios, a series of highly dispersed bimetallic RuM alloy nanoparticles （NPs） anchored on MIL-110（Al） have been successfully prepared via a conventional impregnation-reduction method. And they are first used as heterogeneous catalysts for the dehydrogenation reaction of AB at room temperature. The results reveal that the as-prepared RulCo1@MIL-110 and RulNi1@MIL-110 exhibit the highest catalytic activities in different RuCo and RuNi molar ratios, respectively. It is worthy of note that the turnover frequency （TOF） values of Ru1Co1@MIL-110 and Ru1Ni1@MIL-110 catalysts reached 488.1 and 417.1 mol H2 min-1 （mol Ru）-1 and the activation energies （Ea） are 31.7 and 36.0 k J/tool, respectively. The superior catalytic performance is attributed to the bimetallic synergistic action between Ru and M, uniform distribution of metal NPs as well as bi-functional effect between RuM alloy NPs and MIL-110. Moreover, these catalysts exhibit favorable stability after 5 consecutive cycles for the hydrolysis of AB.展开更多
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(Nos.52301279 and 51901115)the Shandong Provincial Natural Science Foundation,China(ZR2023MB122 and ZR2019PEM001)+1 种基金the Outstanding Youth Innovation Team of Universities in Shandong Province(2024KJH067)the Innovation fund project for graduate student of China University of Petroleum(East China)supported by the Fundamental Research Funds for the Central Universities(No.23CX04010A)。
文摘Addressing inadequate OH^(*)adsorption in Ru Co alloy catalysts is crucial for boosting intermediate coverage and redirecting the water-splitting pathway.Herein,the adaptive P sites were strategically incorporated to overcome the aforementioned challenge.The P sites,as potent OH^(*)adsorption centers,synergize with Co sites to promote water dissociation and enrich surrounding Ru sites with H*intermediates,thus triggering the Volmer-Tafel route for hydrogen evolution reaction(HER).Besides,during the oxygen evolution reaction(OER),the surface of P-Ru Co was reconstructed into Ru-doped Co OOH with anchored PO_(4)^(3-).These PO_(4)^(3-)not only circumvent the intrinsic OH^(*)adsorption limitations of Ru-Co OOH in the adsorbate evolution mechanism(AEM)by rerouting to a more expeditious lattice oxygen oxidation mechanism(LOM)but also improve the coverage of key oxygen-containing intermediates,significantly accelerating OER kinetics.Consequently,the P-Ru Co demonstrates exceptional bifunctional performance,with overpotentials of 29 m V for HER and 222 m V for OER at 10 m A cm^(-2).Remarkably,the mass activities of PRu Co for HER(5.48 A mg^(-1))and OER(2.13 A mg^(-1))are 6.2 and 11.2 times higher than those of its commercial counterparts(Ru/C for HER and RuO_(2)for OER),respectively.When integrated into an anionexchange-membrane electrolyzer,this catalyst achieves ampere-level current densities of 1.32 A cm^(-2)for water electrolysis and 1.23 A cm^(-2)for seawater electrolysis at 2.1 V,with a 500-h durability.
基金supported by the Natural Science Fund for Creative Research Groups of Hubei Province(No.2014CFA015)Hubei Province Education Office Key Laboratory(No.2016-KL-007)of Chinasupported by the Hubei College Students’Innovation Training Program of China(No.201410512024and No.201510512030)
文摘By adjusting various Ru/M （M=Co, Ni） molar ratios, a series of highly dispersed bimetallic RuM alloy nanoparticles （NPs） anchored on MIL-110（Al） have been successfully prepared via a conventional impregnation-reduction method. And they are first used as heterogeneous catalysts for the dehydrogenation reaction of AB at room temperature. The results reveal that the as-prepared RulCo1@MIL-110 and RulNi1@MIL-110 exhibit the highest catalytic activities in different RuCo and RuNi molar ratios, respectively. It is worthy of note that the turnover frequency （TOF） values of Ru1Co1@MIL-110 and Ru1Ni1@MIL-110 catalysts reached 488.1 and 417.1 mol H2 min-1 （mol Ru）-1 and the activation energies （Ea） are 31.7 and 36.0 k J/tool, respectively. The superior catalytic performance is attributed to the bimetallic synergistic action between Ru and M, uniform distribution of metal NPs as well as bi-functional effect between RuM alloy NPs and MIL-110. Moreover, these catalysts exhibit favorable stability after 5 consecutive cycles for the hydrolysis of AB.
