The electrocatalytic nitrogen reduction reaction(NRR)is challenging but crucial for the sustainable development of both industry and agriculture.To enhance NRR performance,it is critically important to construct advan...The electrocatalytic nitrogen reduction reaction(NRR)is challenging but crucial for the sustainable development of both industry and agriculture.To enhance NRR performance,it is critically important to construct advanced electrocatalysts that offer satisfactory performance containing high activity and selectivity.However,the strong affinity of nitrogen-containing species on the Ru surface resulted in suboptimal NRR activity.Herein,we propose a dual-site catalyst,RuNi,to optimize the binding strength,which leads to superior electrocatalytic performance,achieving a high NH_(3)yield rate of 5.07μg h^(-1)cm^(-2)at-0.2 V vs.RHE and a Faradaic efficiency(FE)of 26.2%at-0.1 V vs.RHE in 0.1 mol/L Na_(2)SO_(4).Owing to the synergistic interaction between Ru and Ni,a remarkable performance is realized over the RuNi catalyst.In-situ characterization evidenced that hydrogen radicals(H^(*))on the Ni site of the RuNi catalyst participate in the dissociation of N_(2)adsorbed on the Ru site,and theoretical investigations indicated that RuNi reduces the adsorption strength of intermediates.This offers an effective approach to the synthesis of dual-site catalysts for electrocatalytic ammonia synthesis.展开更多
The plasma-coupled electrocatalytic cascade technology with NO_x~-as intermediate product is a potential method to realize green ammonia synthesis.The matching of the formation rate and consumption rate of NO_(2)^(-)a...The plasma-coupled electrocatalytic cascade technology with NO_x~-as intermediate product is a potential method to realize green ammonia synthesis.The matching of the formation rate and consumption rate of NO_(2)^(-)as the main absorption product is an important prerequisite for the system to achieve stable operation.Therefore,this paper firstly emphasizes the importance of operating parameters on the cascade system based on the single factor experiment.Secondly,the empirical equation between electrocatalytic operating conditions and NO_(2)^(-)consumption rate was established by response surface analysis.Based on this equation,the electrocatalytic operating parameters were optimized to achieve the dynamic equilibrium between NO_(2)^(-)formation rate and consumption rate.Finally,the techno-economic assessment model was established to calculate the levelized cost of ammonia based on the cascade system,and the single-variable sensitivity analysis was performed to provide the clear guidance for cost reduction.展开更多
基金supported by the National Natural Science Foundation of China(Nos.U22A20418,22075196)the Research Project Supported by Shanxi Scholarship Council of China(No.2022–050)。
文摘The electrocatalytic nitrogen reduction reaction(NRR)is challenging but crucial for the sustainable development of both industry and agriculture.To enhance NRR performance,it is critically important to construct advanced electrocatalysts that offer satisfactory performance containing high activity and selectivity.However,the strong affinity of nitrogen-containing species on the Ru surface resulted in suboptimal NRR activity.Herein,we propose a dual-site catalyst,RuNi,to optimize the binding strength,which leads to superior electrocatalytic performance,achieving a high NH_(3)yield rate of 5.07μg h^(-1)cm^(-2)at-0.2 V vs.RHE and a Faradaic efficiency(FE)of 26.2%at-0.1 V vs.RHE in 0.1 mol/L Na_(2)SO_(4).Owing to the synergistic interaction between Ru and Ni,a remarkable performance is realized over the RuNi catalyst.In-situ characterization evidenced that hydrogen radicals(H^(*))on the Ni site of the RuNi catalyst participate in the dissociation of N_(2)adsorbed on the Ru site,and theoretical investigations indicated that RuNi reduces the adsorption strength of intermediates.This offers an effective approach to the synthesis of dual-site catalysts for electrocatalytic ammonia synthesis.
基金financially supported by National Key Research and Development Program of China(2020YFA0710000)National Natural Science Foundation of China(U22A20391,22308274)+2 种基金Postdoctoral Fellowship Program of CPSF(GZB20240600,2023TQ0265,2024M752589)Innovation Capability Support Program of Shaanxi(NO.2023-CX-TD-26)the Programme of Introducing Talents of Discipline to Universities(B23025)。
文摘The plasma-coupled electrocatalytic cascade technology with NO_x~-as intermediate product is a potential method to realize green ammonia synthesis.The matching of the formation rate and consumption rate of NO_(2)^(-)as the main absorption product is an important prerequisite for the system to achieve stable operation.Therefore,this paper firstly emphasizes the importance of operating parameters on the cascade system based on the single factor experiment.Secondly,the empirical equation between electrocatalytic operating conditions and NO_(2)^(-)consumption rate was established by response surface analysis.Based on this equation,the electrocatalytic operating parameters were optimized to achieve the dynamic equilibrium between NO_(2)^(-)formation rate and consumption rate.Finally,the techno-economic assessment model was established to calculate the levelized cost of ammonia based on the cascade system,and the single-variable sensitivity analysis was performed to provide the clear guidance for cost reduction.
